Journal of Cleaner Production 211 (2019) 1553e1566

Contents lists available at ScienceDirect

Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Review

Food waste valorization advocating Circular Bioeconomy - A critical

review of potentialities and perspectives of spent coffee grounds
biorefinery
Anastasia Zabaniotou*, Paraskevi Kamaterou
Biomass Group, Department of Chemical Engineering, Aristotle University of Thessaloniki, Greece

a r t i c l e i n f o a b s t r a c t

Article history: Waste biorefineries are instrumental for advocating Circular Bioeconomy. Food waste valorization is a
Received 13 July 2018 goal of sustainable development, gaining high interest in resolving environmental and resources chal-
Received in revised form lenges. Coffee use generates massive quantities of spent coffee grounds (SCG), a resource rich in fatty
5 November 2018
acids, amino acids, polyphenols, minerals, and polysaccharides. This review aims to shed light on the
Accepted 23 November 2018
Available online 24 November 2018
potentialities, prospects, and challenges of the transition from a mono-process to a cascade SCG bio-
refinery, in a circular economy thinking. It was found that mono-process approaches of SCG extraction
have been investigated by many researchers, while SGC biorefining approaches are still at an early stage
Keywords:
Spent coffee ground
of research. Studies on SCG biorefineries, their environmental and economic assessment are few in the
Food waste literature, therefore imitations in extrapolating information and comparing the results were faced. It was
Cascade biorefinery made evident that more studies are needed on the economic assessment of the mono-process SCG break
Sustainability down, at higher Technology Reediness Level (TRL) for realistic assessments. Efficient conversion of SCG in
Circular economy a cascade biorefinery depends on the spectrum of various end-products and cost-effective processing
Bioeconomy schemes. Lipids and/or polysaccharides extraction followed by the conversion of by-streams to energy
and biochar, in a closing loop concept, has good potentialities. The review allowed the exploration of
knowledge-based strategies to unlock the potential of SCG for bio-derived chemicals, carbon materials,
fuels and fertilizer production and probably impacting waste management regulations. Some guidelines
for the sustainable design of SCG biorefineries were provided.
© 2018 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1554
2. Methodology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1555
2.1. Sourcing, screening, analyzing the articles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1555
3. Materials and methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1556
3.1. SCG composition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1556
3.2. Mono-process approach: what can be extracted from SCG? . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1556
3.2.1. Oil recovery . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1557
3.2.2. Polysaccharides recovery . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1558
3.2.3. Phenolic compounds recovery . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1558
3.2.4. Tannins recovery . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1558
3.2.5. Caffeine recovery . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1559
3.3. SCG valorization for bioenergy and carbon materials production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1559
3.3.1. Biodiesel production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1559
3.3.2. Biooil production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1559

* Corresponding author. Dept of Chemical Engineering, Aristotle University of

Thessaloniki, U.Box 455, GR24154, Greece.
E-mail address: azampani@auth.gr (A. Zabaniotou).

https://doi.org/10.1016/j.jclepro.2018.11.230
0959-6526/© 2018 Elsevier Ltd. All rights reserved.
1554 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566

Abbreviations PEF Pulsed-electric field extraction

PEI Potential environmental impact
ABTS 2,20 -azino-bis (3-ethylbenzothiazoline-6-sulphonic Ph Phenol
acid) PHAs Polyhydroxyalkanoates
ACs Activated carbons PLE Pressurized liquid extraction
AO7 Acid orange 7 PMHS Polymethylhydrosiloxane
BSG Brewer's spent grains SCG-GAC Spent coffee grounds into calcium-alginate beads
CGA Chlorogenic Acid SCGs Spent coffee grounds
CM Coffee melanoidins SDGsSFE Sustainable Development Goals Supercritical fluid
CS Coffee silverskin extraction
db Dry base SL Solid-liquid
DSCG Dried spent coffee grounds TBAs Tannin-based absorbents
EAE Enzyme-assisted extraction TE Trolox equivalents
FFA Free fatty acid TS Total solid
FWHHV Food Waste Higher heating value UAE Ultrasound-assisted extraction
GAE Gallic acid equivalents UNDPUSDA United Nation Development Program United States
HTL Hydrothermal liquefaction Department of Agriculture
MAE Microwave assisted extraction VOCsEMYFC Volatiles Organic Compounds effective mass yield
MB Methylene blue Feature Complexity index

3.3.3. Biochar production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1560

3.3.4. Activated carbon production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1560
3.3.5. Nanocarbons production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1560
3.3.6. Liquid polyols production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1560
3.3.7. Energy production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1560
3.3.8. Cogeneration of heat and power (CHP) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1560
3.4. Biorefinery approach . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1561
4. Discussion on SCG biorefinery approach . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1561
4.1. Prospects of SCG biorefinery . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
4.2. Economic viability and sustainability challenges . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
4.3. Business development and market perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
4.4. Policy and regulations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
4.5. Indexes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1563
4.6. Circular economy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1563
4.7. Design guidelines . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1563
5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1564
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1564

1. Introduction must be achieved by developing and deploying not only technol-

ogies and practices, but also changing behaviors and patterns of
Beyond climate change, the main challenges the world is facing production and consumption (https://www.wri.org/), as depicted
today, are the substantial increase in energy demand, food and in the 17 Sustainable Development Goals (SDGs) of United Nation
material unsustainable consumption and production, and anthro- development program (UNDP). New interconnected areas, such as
pogenic wastes generation. According to World Resources Institu- climate change, innovation, sustainable consumption, are included
tion (https://www.wri.org/), the planet is projected to hold 9.6 among other in the SDGs (United Nations Development Program,
billion people by 2050, consuming the equivalent of 1.6 planet's 2018).
resources, with a consequent high amount of wastes generated. A new approach to sustainability has been proposed in Europe.
Consequences of the unsustainable consumption and production This encompasses the Circular Economy model, as a pathway to
patterns are resource depletion, climate change, air and water engage with challenges of sustainable production and consump-
pollution, loss of biodiversity and of fertile soil, amongst other tion. A priority in the EU is to stimulate the transition towards a
environmental, social, and economic challenges (FAO, 2013). Circular Economy that fosters the promotion of sustainable and
The production of the enormous quantities of food waste (FW) is resource-efficient policies for long-term socio-economic and
becoming a global concern (Dahiya et al., 2016), because the world environmental benefits, by adopting strategies of “closing the loop”
need to adequately feed the 9.6 billion people by 2050, in a way that in industrial production systems (Maina et al., 2017). One of the
advances economic development and reduces pressure on the most relevant goals in the application of this approach is to convert
environment (https://www.wri.org/). Long-term strategies are low-value side streams/residues/wastes into more valuable
needed aligning short and medium-term goals. The long-term goal products.
for many countries and especially for Europe, is ensuring a transi- Limitations of this approach related to the social aspects of
tion from carbon-intensive to low-carbon societies. This transition circularity, result to the call for more ethical and socially inclusive
 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566
approaches to the Circular Economy (Lazell et al., 2018).
Food waste (FW) valorization is a goal of sustainable develop-
ment and it gains high interest since many bio-based products can
be derived from them, besides energy and fuels (Rama Mohan,
2016). Coffee is one of the most popular and appreciated bever-
ages worldwide, and plays an important role in the global economy,
as it is the second most traded commodity after oil (Murthy and
Naidu, 2012). Coffee industries are a key sector in the global
economy, due to income reporting and job creation. Based on
United States Department of Agriculture (USDA) report (USDA,
2017), global coffee industry reached an estimated production of
9.34 million tons in 2016/17, which generated massive quantities of
bio-wastes that are incinerated, dumped in a landfill, or composted.
Coffee companies produce annually more than 2 billion tons of by-
products, such as coffee spent grounds (SCG) and coffee silverskin
(CS), most of which are thrown away for landfilling (Jimenez-
Zamora et al., 2015).
The generation of energy and various commodities in an inte-
grated approach addressing sustainability, is a challenge and a
perspective for Europe (Dahiya et al., 2016). New generations of
biorefinery can combine innovative bio-waste resources from
different origins. Integrated and cascade biorefineries are corner-
stones of the Circular Bioeconomy. SCG can be used as feedstock to
produce various bio-based products and bioenergy in a biorefinery
concept (Mata et al., 2018), by closing loops (Karmee Sanjib Kumar,
2018). Targeting economic viability and sustainability is very
important for a Circular Bioeconomy (Va ^nia et al., 2018).
This paper aims to review the potentialities and perspectives of
SCG biorefinery, as a solution to current bio-waste disposal prob-
lems, in a Circular Bioeconomy. The objective is to review the
mono-process pathways for the valorization of SCG, reported in the
international literature, and to ding in the multi-process-multi-
product cascade biorefinery concept that is a cornerstone in the
transition to Circular Bioeconomy. It finally aims to provide general
guidelines on how to build a sustainable SCG biorefinery, by sum-
marizing various researcher's suggestions, who have worked on the
topic of sustainable biorefineries.
2. Methodology
In this paper, a systematic literature review was performed
following the method proposed by Thürer et al. (2018), for sourcing,
screening, and analyzing the published articles. The target was to
retrieve and select those articles which investigate and define the
current state-of-the-art on valorization of spent coffee grounds
(SCG), via sustainable pathways in the concept of biorefinery. Main
effort was devoted to find studies on biorefineries’ economic
viability and sustainability. Since the strategy of Circular Economy
is recent and mainly articulated in Europe, very few studies
appeared in the international literature, mainly published during
2018.
2.1. Sourcing, screening, analyzing the articles
Scopus and open access are the bibliographic databases selected
for retrieving the articles, because they provide extensive literature
tools (books, articles). For quality assurance of the research, only
peer-reviewed articles were selected. The criteria used for the ar-
ticles' selection were the title, abstract, keywords, and document
type (restricted to ‘articles’ and ‘reviews’), and the year of publi-
cation for a period of almost 10 years (from 2009 to 2018). The
inquiry took place in July 2018 using the terms ‘Spent AND Coffee
AND Grounds AND Conversion’; ‘Spent AND Coffee AND Grounds
AND Extraction’; ‘Spent AND Coffee AND Grounds AND Valoriza-
tion’; ‘Spent AND Coffee AND Grounds AND Pyrolysis’; ‘Spent AND
1555
Coffee AND Grounds AND Biorefinery’; ‘Spent AND Coffee AND
Grounds AND Environmental’; ‘Spent AND Coffee AND Grounds
AND economic’. Other articles, concerning biorefining and Circular
Economy, as also three books were included.
The literature inquiry brought to light 637 articles (109 for the
search term ‘Spent AND Coffee AND Grounds AND Conversion’, 252
for the search term ‘Spent AND Coffee AND Grounds AND Extrac-
tion’, 119 for ‘Spent AND Coffee AND Grounds AND Valorization’, 98
from ‘Spent AND Coffee AND Grounds AND Pyrolysis’, 33 for ‘Spent
AND Coffee AND Grounds AND Biorefinery’, 6 for ‘Spent AND Coffee
AND Grounds AND Environmental’, while only 3 dealing with
economics. Seventeen review studies were retrieved, which pub-
lished just recently.
The original sample contained 263 duplicates articles, which
were removed. From the 374 remaining articles, 41 were subtracted
as unrelated and 13 were cut-off due to their year of publication,
which was out of the time spectrum set in this study. All 320 papers
were examined. By focusing on extracting, grouping of papers
concerning sustainable SCG valorization that give information,
knowledge, and data, to reply to the research questions set, finally
83 papers were used as the most appropriate and interesting for the
review. Another 7 internet sources and 2 books on SGC valorization,
and one book on food wastes, sustainability and Circular Economy
topics were also included. A total of 93 sources were selected for
this review (Table 1).
The screening of the 320 papers was made by prioritizing papers
discussing sustainability, techno economic assessment, biorefinery
approach, mono-process approach of the SCG and related review
papers published within the decade 2009e2018.
The research questions for the screening of the 320 papers were:
 Which is SCG's composition?
 Which useful components could be extracted from SCG and
how?
 What about thermochemical conversion routes for SCG
valorization?
 Can SCG produce biochar via pyrolysis?
 Can biorefining be applied for SCG valorization?
 How sustainable is to valorize SCG by biorefinery?
 What is the economic viability of a SCG biorefinery?
 What is the environmental sustainability of the SCG
biorefinery?
 Are there any guidelines for a multi process-multi product
approach of SCG valorization?
 Which are the prospects arising from this paper?
Fig. 1 depicts the number of the related papers published per
year. Fig. 2 depicts the paper related to the extracted product per
year of publication. It is obvious that papers on mono-process
approach are the first appeared in the international literature and
continue to be published in a large number. Papers on biorefinery
approach are recent and mainly of the year 2018. Papers on
Table 1
Screening procedure of peer review articles.
Screening Step Number of articles in Sample
1. First sample 637
2. Sample after duplicates removal 374
3. Sample after less relevant articles removal 333
4. Remaining sample after cut-off point 320
5. Final sample 83
6. Books 3
7. Internet sources 7
Final Sample 93
1556 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566

sustainability and technoeconomic assessment are few. Concerning

review papers, these are showing an increasing trend the last 3
years.

3. Materials and methods

The first research question for the screening of the 320 papers is
related to SCG's composition. The SCG composition defines the
choices for the valorization.

3.1. SCG composition

The biochemical composition of SCG as reported in literature, is

Fig. 1. Published articles concerning SCG, per year of publication.
presented in Table 2. SCG contain 9-16 wt% db lipids, 5e15 wt% db
proteins and are considered as an important source of poly-
saccharides (carbohydrate whose molecules consist of several
sugar molecules bonded together). Literature review revealed that
almost half of the material (45.3 wt% db) is sugars polymerized into
cellulose and hemicellulose structures (Mussato et al., 2011) and
that most polysaccharides (around 70 wt% db of total poly-
saccharides from roasted coffee) remains in SCG (Arya and Rao,
2007). Mussato et al. (2012) have hydrolyzed SCG and efficiently
fermented it to ethanol by yeast. SCGs coffee fibers exhibit anti-
oxidant properties suggesting their use as potential dietary sup-
plement (Campos-Vega et al., 2015). Ballesteros et al. (2015)
investigated the antimicrobial and antioxidant capacities of poly-
saccharides extracted from SCG.
The ultimate/proximate analysis of reported SCG is presented in
Table 3. The carbon content of SCG ranges between 45 and 53 wt%
whereas the values for hydrogen and nitrogen content are 6e7 wt%
and 2e4 wt%. The amounts of ash (1e2 wt% db) containing in SCG is
low compared to other biomass sources (Zabaniotou et al., 2017).
SCG is characterized by high total volatiles content (Tsai et al.,
2012).

3.2. Mono-process approach: what can be extracted from SCG?

SCG represent a resource rich in valuable components which

Fig. 2. Published articles on single-extraction process products, per year of publication. could be valorized giving a range of commodities. Large amounts of
organic compounds are contained in SCG, such as fatty acids, amino

Table 2
SCG biochemical composition (wt%db).

Lipids (wt%db) Carbohydrates (wt%db) Proteins (wt%db) References

n.d. 14.1 14.4 Somnuk et al. (2017)

9e16 45e47 13e17 Burniol-Figols et al. (2016)
13 ± 0.04 65.9 ± 6.5 4.9 ± 0.6 Passos and Coimbra. (2013)
13.7 ± 0.1 54.1 ± 2.2 13.8 ± 0.1 Wang et al. (2016)
45.3 13.6 Campos-Vega et al. (2015)b

Table 3
Proximate and ultimate analysis of SCG.

Ultimate Analysis (ww% db)

C H N S O References
53.0 6.8 2.1 0.1 38.1 Somnuk et al. (2017)
52.5 ± 0.4 7.0 ± 0.03 3.46 ± 0.01 0.10 ± 0.00 34.8 ± 0.1 Tsai et al. (2012)

Proximate Analysis (ww%db)

Moisture Volatile Ash Fixed Carbon

e e 1.6 e Somnuk et al. (2017)

11.5 ± 0.4 79.5 ± 0.01 0.7 ± 0.2 8.2 Tsai et al. (2012)
 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566 1557

acids, polyphenols, minerals, and polysaccharides (Campos-Vega
et al., 2015). Coffee is considered an important source of poly-
saccharides (Ballesteros et al., 2017), proteins (Mussato et al., 2011)
and lipids (Campos-Vega et al., 2015). SCG is rich in sugars (45 ww%,
dry weight of the material) which can be polymerized into cellulose
and hemicellulose structures. Mannans is the major polysaccharide
of SCG which contains 47 wt% db mannose, 30 wt% db galactose,
19 wt% db glucose, and 4 wt% db arabinose (Mussatto et al., 2011).
Remarkable amount of proteins (13e17 wt% db) are contained in
SCG Mussato et al. (2011). Other N-containing substances like
caffeine, trigonelline, free amines and amino acids are contained in
SCG (Delgado et al., 2008).
Caffeine is a non-protein nitrogenous compound which can be
recovered from SCG. Panusa et al. (2013) estimated a low content of
caffeine (0.96e0.97 mg/g dry sample) in SCG extracts. According to
Cruz et al. (2012) the range of caffeine content found higher for the
espresso coffee (1.9e7.9 mg/g db). However, caffeine, tannins and
chlorogenic acid are of eco-toxicological concern and can limit their
value-adding applications.
There is an especial interest in SCG lipids extraction. Total lipids
content of espresso coffee residues ranges from 9.3 to 16.2 wt% db
(Cruz et al., 2012) depending on the coffee variety (Jenkins et al.,
2014), a promising feedstock to produce biodiesel (Al-Hamamre
et al., 2012). Hexane is the most popular solvent for oil extraction,
but Supercritical Fluid Extraction is a modern environmentally
friendly technology which is increasingly being used for SCG oil
extraction (Campos-Vega et al., 2015).
SCG contain phenolic compounds which are known as human
health related compounds, with demonstrated antioxidant, anti-
bacterial, antiviral, anti-inflammatory and anti-carcinogenic activ-
ities (de Souza et al., 2004). Polyphenols and chlorogenic acid (CGA)
have been extracted from SCG via a conventional solid-liquid
method (Campos-Vega et al., 2015).
The techniques for extraction of compounds are classified into
two categories: the conventional and the non-conventional (Azmir
et al., 2013). The conventional techniques are:
 Soxhlet extraction
 Maceration
 Hydrodistillation
The non-conventional extraction techniques are (Azmir et al.,
2013):
 Ultrasound-assisted extraction (UAE)
 Pulsed-electric field extraction (PEF)
 Enzyme-assisted extraction (EAE)
 Microwave assisted extraction (MAE)
 Pressurized liquid extraction (PLE)
 Supercritical fluid extraction (SFE)
Table 4 presents the valuable components that can be extracted
from SCG, as demonstrated in the literature. By searching the
literature, opportunities were found concerning the recovery of
oils, polysaccharides, phenolic compounds, tannins that can be
used in various commodities, by using mono-extraction processes,
as depicted in Fig. 3.
3.2.1. Oil recovery
The oil content of SCG ranges from 10 to 15 wt%, depending on
the coffee varieties (Jenkins et al., 2014). Somnuk et al. (2017)
studied the effect of four different solvents (hexane, ethanol, hy-
drous ethanol and methanol) on coffee oil yield, by using a circu-
lation process. The optimal conditions (30.4 min extraction time
and 22.5 g/g ratio of DSCG-to-hexane) resulted in approximately
11.8 wt% oil yield. Phimsen et al. (2016) utilized a Soxhlet extractor
and n-hexane as a solvent in order to extract the oil from dried
SCGs. The extracted oil, yielded from 10 to 13 wt% db SCG, and then

Table 4
Single-extraction SGC processes for high added value compounds reported in the literature.

Reference Process SCGs single-extraction process

Process Parameters Oil Product

Polysacharides Phenolics Tannins Caffeine

Extraction characteristics SCG/Solvent Extraction Temperature (w/w% (w/w% d.b.) (w/w% d.b.) (mg/g (mg/g
ratio (g/g) time (min) ( C) d.b.) d.b.) d.b.)

Somnuk et al. Oil extraction (Solvent Extr) 22.5 30.4 30 14.7 e e e e

(2017) Hexane
Ethanol anhydr. 22.8 33.5 30 13.1 e e e e
Ethanol hydrous 20.3 25.5 30 11.8 e e e e
Methanol 23.8 19.6 30 7.5 e e e e
Phimsen et al. Polysacharides (Soxhlet extr.) Hexane 400 g/3l 480 13 e e e e
(2016) extraction
Mussato et al. Sulfuric acid 0.5 M 45 121 e 45.3 e e e
(2011)
Ballesteros (Autohydrolysis) 1 g/15 ml 10 160 e 29.29 234.1407 mg e e
et al. (2017) Water GAE/g
Passos et al. (Microwave superheated 1gSCG/10 ml 2 200 e 55 e e e
(2013) water extraction)
Water
Xu et al. (2015) Phenolics extraction (Subcritical water 14.1 g/l 38e55 160e180 e e 86.2 mg GAE/ e e
extraction) g
Water
Shang et al. Phenolics and (Pressurized liquid 195 e e 19-26 e 3
(2017) Caffeine extraction extraction) mgGAE/gdb e9 mg/
Water g db
Ethanol 195 e e e e e
Low et al. Tannins' Extraction Sodium hydroxide 5 wt% 8.2 30 100 e e e 21.02 e
(2015)
Brazinha et al. Caffeine extraction Membrane technology e e e e 3e9
(2015)
1558 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566
Fig. 3. High added value products derived from a mono-extraction process.
it was hydrotreated in a shaking batch reactor, by using NiMo/g-
Al2O3 and Pd/C as catalysts. It has proved the bio-hydrotreated fuel
production and potentiality to be used as a renewable energy.
3.2.2. Polysaccharides recovery
Polysaccharides play multiple role in life process and present an
immense potential in healthcare, food, and cosmetic industries, due
to their content of bioactivities that have therapeutic effects and
relatively low toxicity (Shi L. 2016). Due to their enormous struc-
tural heterogeneity, the approaches for isolation and purification of
polysaccharides are distinct from that of the other macromolecules
such as proteins etc. (Shi L. 2016). Therefore, various methods
widely used in isolation and purification of polysaccharides. The
extraction of polysaccharides from SCG has been studied, mainly
using chemicals as extraction agents. Sodium hydroxide
(Ballesteros et al., 2015) and potassium hydroxide have been
employed in SCG alkali treatments, while sulfuric acid has been
used to recover carbohydrates from SCG dilute acid hydrolysis
(Mussatto et al., 2011).
Mayanga-Torres et al. (2017) proposed the recovery of sugars
compounds from coffee industry residues using subcritical water
hydrolysis as the valorization technique. Evaluation of optimal
conditions which simultaneously maximize holocellulose hydro-
lysis and minimize both sugar degradation and dilution is
proposed.
The extraction of polysaccharides by autohydrolysis of SCG was
investigated by Ballesteros et al. (2017). The extracted poly-
saccharides (29.29 wt%) characterized by high antioxidant activity.
The conditions for the extraction were 15 ml water/g SCG, for
10 min, at 160  C. The polysaccharides obtained were thermostable
in a large range of temperature and had typical carbohydrate
pattern. Their use for industrial applications, mainly in the food
area was proposed.
The feasibility of microwave superheated water extraction of
polysaccharides from SCG was studied by Passos et al. (2013). They
found that a maximum of 0.57 g/batch polysaccharides for 1 g SCG:
10 mL water can be recovered. Further extraction of poly-
saccharides was achieved with a second extraction (re-extraction)
of the remaining un-extracted insoluble material, under the same
conditions.
3.2.3. Phenolic compounds recovery
Polyphenols are micronutrients. The health benefits of poly-
phenols and their protective effects in food systems as antioxidant
compounds, are well known and have been extensively
investigated (Shavandi et al., 2018). Recovery of relevant natural
antioxidants for use as nutritional supplements, foods, or cosmetic
additives can be achieved by SCG extraction with environmentally
friendly procedures (Panusa et al., 2013).
The bibliographic search shown that various extraction methods
were used. Subcritical water extraction of SCG resulted in signifi-
cant antioxidative phenolics production (Xu et al., 2015) at tem-
perature range of 160e180  C, time range of 38e55 min and solid-
to-liquid ratio of 14.1 g/l. 86.2 mg GAE/g of total phenolic com-
pounds were recovered. Shang et al. (2017) optimized the SCG
extraction conditions for total phenolics by using pressurized liquid
extraction (PLE) method with water and ethanol. Optimal condi-
tions obtained at 195  C extraction temperature. The total phenolics
content ranged from 19 to 26 mgGAE/gDW.
Al-Dhabi et al. (2017) developed and validated the SCG
ultrasound-assisted solid-liquid extraction of phenolic compounds.
Ultrasonic power, temperature, time, and solid-liquid (SL) ratio
were studied as parameters. The optimum process conditions
were: 244 W of ultrasonic power, 40  C of temperature, 34 min of
time and 1:17 g/mL of SL ratio and the extraction obtained yields
reached 33.84 GAE/g of total phenolic content.
Coffee cherry pulp is a by-product derived from the process of
coffee production. Coffee cherry pulp contains considerable
amounts of phenolic compounds and caffeine. An attempt to pro-
duce “Cascara”, a refreshing beverage, has been made by Heeger
et al. (2017). Six dried coffee pulp samples and Cascara produced
out of one of those samples, were investigated in Switzerland.
Aqueous extraction of coffee pulps revealed a content of total
polyphenols between 4.9 and 9.2 mg gallic acid equivalents (GAE)/g
db. The antioxidant capacity was between 51 and 92 lmol Trolox
equivalents (TE)/g DM, as measured with ABTS radical. Bourbon
variety from Congo and Maragogype variety showed highest
caffeine contents, 6.5 and 6.8 mg/g DM, respectively. In all samples,
chlorogenic acid, protocatechuic acid, gallic acid and rutin, were
present. The beverage Cascara contained 226 mg/l of caffeine and
283 mg GAE/l of total polyphenols and an antioxidant capacity of
8.9 mmol TE/l.
Jimenez-Zamora et al. (2015) showed the prebiotic, antimicro-
bial and antioxidant capacity of SCGs and CS, as well as those
melanoidins (a coffee component generated during the roasting
process), obtained from the former. The prebiotic activity was
important in both CSG and CS, although the presence of coffee
melanoidins (CM) interfered with such beneficial properties. On
the contrary, CM exerted an intense antimicrobial activity that
could be used to avoid the growth of pathogenic bacteria in food
products. CSG, CS and CM were highly antioxidant. The addition of
sugar during coffee roasting, namely torrefaction, increased the
antioxidant and antimicrobial activity due to a larger generation of
CM, although prebiotic activity was not affected.
3.2.4. Tannins recovery
Tannins extensively assessed as natural alternatives to in-feed
antibiotics (Huang et al., 2017). Low et al. (2015) investigated the
influence of extraction parameters in SCG tannins’ recovery. They
found that sodium hydroxide concentration, extraction tempera-
ture and liquid to solid ratio considerably effected the SCG tannin
extraction yield and its reactivity. Extraction time had only mar-
ginal effect in the tannin extraction process. The optimal extraction
conditions were found: 5 wt% sodium hydroxide concentration,
100  C extraction temperature, 30 min extraction time, and 8.2
liquid to solid ratio. These conditions resulted in a high tannin
extraction yield (21.02 wt%) and high reactivity.
Tannins have traditionally been regarded as “anti-nutritional
factor” for poultry. Recent researches have mentioned that when
applied in appropriate manner, improved intestinal microbial
 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566
Fig. 4. SCG thermochemical conversion processes and their products.
ecosystem, enhanced gut health and hence increased productive
performance (Huang et al., 2017). However, tannins if used as ad-
ditives in poultry feed to control diseases and to improve animal
performance, must ensure a consistent quality (Redondo et al.,
2014).
Tannins are also low-cost natural biopolymers and excellent
candidates to produce bio-sorbents. Low-cost and eco-friendly
products, such as adhesive, plastic, polyform can be produced by
using the SCG extracted tannins. Tannin-added films can be used as
green, nontoxic packaging materials for food and pharmaceutical
products (Missio et al., 2018). Tannin-based absorbents (TBAs) have
a natural affinity to absorb heavy metals dyes, and pharmaceutical
compounds from contaminated waters (Bacelo et al., 2016).
3.2.5. Caffeine recovery
Brazinha et al. (2015) optimized the process of producing a
natural extract from SCG by using membrane technology, with no
organic solvents or adsorbents involved. The extracted product was
enriched in caffeine with specific health benefits.
Shang et al. (2017) optimized the SCG extraction conditions to
caffeine using pressurized liquid extraction (PLE) method with
water and ethanol. At the optimal conditions (195  C extraction
temperature) caffeine's yield reached 9 mg/g db.
3.3. SCG valorization for bioenergy and carbon materials
production
Energy recovery from biomass is a way to reduce waste, produce
fuels, protect the environment and mitigate greenhouse gas (GHG)
emissions (Limousy et al., 2017). Energy recovery should be com-
bined with material recovery for enhanced resources efficiency, in
the concept of a Circular Economy.
Energy recovery from SCG was documented in the international
literature. Biochemical (transesterification) and thermochemical
(pyrolysis, gasification, hydrothermal liquefaction, combustion),
enzymatic conversion technologies were used for this, as it is depicted
in Fig. 4. Biodiesel, biooil, CHP, heat, biochar, activated carbons, carbon
nanotutes, are the main products of the application of a mono-
thermochemical process fueled with SCG (Limousy et al., 2017).
3.3.1. Biodiesel production
SCG contain significant amounts of lipids (~16%w/w), which
could potentially be utilized as feedstock in biodiesel production.
Many researchers used transferification of the exctracted oil (Loyao
et al., 2018). Solvent extraction technologies, with a wide range of
1559
solvents for lipid extraction from SCG, were used to determine the
effect of solvent selection and process temperature on the extrac-
tion efficiency and composition of the obtained oil, by
Efthymiopoulos et al. (2018). Al-Hamamre et al. (2012) studied oil
extraction from dried spent coffee grounds (DSCGs) for biodiesel
production. They obtained 60 g DSCG. Kondamudi et al. (2008)
extracted the SCG oil (10e15 %wt) using solvents such as hexane,
ether, and dichloromethane under reflux conditions. They trans-
esterified the oil to produce biodiesel and achieved 100% conver-
sion. The produced biodiesel was found to be stable for more than 1
month under ambient conditions.
The valorization route of lipid recovery followed by trans-
esterification for biodiesel production was also studied by Go and
Yeom (2017). Lipid extraction was estimated at 92.7%, using
13.7 ml-hexane/g-WCG, within 30 min extraction time, and 25  C.
NaOH was used as an alkaline catalyst. Optimum conditions for
transesterification were achieved with the addition of 0.5% catalyst,
1.5 mL methanol/g-lipid, at 45  C, and 9 h of reaction time. Biodiesel
production was mainly influenced by reaction time and tempera-
ture. Caetano et al. (2014) examined the potential of biodiesel
production from SCG. They used various solvents and proposed a
two-step process of acid esterification followed by alkaline trans-
esterification for lipids with high free fatty acids, as the best route
to biodiesel. However, the properties of the derived biodiesel
(iodine number, acid value, and ester content) did not comply with
the NP EN 14214:2009 standards (Caetano et al., 2014). For meeting
standard requirements, they proceeded with two remediation
procedures: a) blending of SCGs lipids with other higher-quality
vegetable oils before transesterification, b) mixing the produced
biodiesel with higher-quality biodiesel.
€hlerta et al. (2016) studied the catalytic conversion of tri-
Do
glycerides derived from SCGs to produce diesel, by using a cheap
reductant agent, the polymethylhydrosiloxane (PMHS) under mild
reaction conditions. Significant amounts of PMHS-waste generated
as by-products of the process (~1.7% of the PMHS is required for the
oil reduction). They were depolymerized in a subsequent step,
resulting in PMHS-waste conversion to methyltrifluorosilane and
difluoromethylsilane, which can be useful for new silicones pro-
duction as building blocks. The acid catalytic solvo-thermal in situ
transesterification of SCG was demonstrated by Park et al. (2018).
They suggested them for boosting the economic feasibility of bio-
diesel production from wet SCGs.
Kookos (2018), by performing an economic and environmental
analysis of biodiesel production from SCG, concluded that the
process economics can be attractive only in the case of a centralized
large-scale production plant. Biodiesel production from SCG is not
economically sound for small scale units.
3.3.2. Biooil production
Fast pyrolysis can convert the SCG into biooil and biochar. The
fast pyrolysis of SCG targeting biooil production was studied by
Kelkar et al. (2015). The experiments took place in a compact,
transportable, screw conveyor reactor. Biooil yields showed a
maximum yield of 61.8 ww% at 500  C, while the highest biochar
yield was observed at the lowest pyrolysis temperature (429  C).
SCG-biooil contained fatty acids, fatty acid esters, medium-chain
paraffins, olefins and caffeine.
Fast pyrolysis of SCG was also studied by Bok et al. (2012). They
produced biooil with a maximum yield of 55 ww% at 550  C py-
rolysis temperature, pyrolysed in a fluidized bed reactor. Li et al.
(2014) investigated SCG bioenergy production potential using py-
rolysis, at two different heating rates (10 and 60  C/min). Biogas
contained mainly CO2, CO, CH4 and the gaseous volatile. An effi-
ciency of 77e85% was achieved in relation to the feedstock mois-
ture content.
1560 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566
SCG pyrolysis was performed by Cho et al. (2016) targeting both,
waste disposal and biooil recovery. In their study, SCG were pre-
treated with FeCl3, and carbon dioxide to enhance syngas genera-
tion and reduce condensable hydrocarbons, such as tar. Syngas
enhancement was achieved via the CO2-induced thermal cracking
of VOCs, due to the reaction between CO2 and VOCs. Tar reduction
was achieved by using Fe as catalyst in a CO generation from Fe-SCG
pyrolysis. This has also resulted in CO2 dramatical increase (up to
8000%), compared to SCG pyrolysis with N2.
Hydrothermal liquefaction (HTL) of SCG, in hot-compressed
water was applied to produce crude bio-oil in a 100 cm3
stainless-steel autoclave reactor, with N2 atmosphere, (Yang et al.,
2016). The effects of operating parameters (retention times -
5 min, 10 min, 15 min, 20 min and 25 min, reaction temperatures 
200  C, 225  C, 250  C, 275  C and 300  C, water/feedstock mass
ratios  5:1, 10:1, 15:1 and 20:1, process gas initial
pressure 2.0 MPa and 0.5 MPa), were investigated targeting biooil
yield with designed properties. A yield of 47.3 ww% of the crude
biooil was achieved at 275  C liquefaction temperature, 10 min
retention time, water/feedstock mass ratio of 20:1 and initial
pressure of 2.0 MPa. The higher heating value (HHV) of crude biooil
was estimated at 31.0 MJ/kg.
Yang et al. (2017) investigated the co-liquefaction in subcritical
water of SCG mixed with paper filter, corn stalk and white pine
bark, aiming to bio-crude oil production. The optimum reaction
temperature was estimated at 250  C, and the mixing biomass ratio
was 1:1. The best feedstock combination was SCG and CS and
addition of 5% NaOH, as a catalyst. Biooil quality and high yield
suggest SCG as a valuable biooil feedstock.
3.3.3. Biochar production
Slow pyrolysis of SCG can produce biochar. Pyrolytic char from
SCG is a much better fertilizer compared to direct SCG use in the
fields, as it was proved by various studies. SCG and SCG-char were
applied as biochar, by Kim et al. (2014). In the case of SCG appli-
cation, the soil phytotoxicity increased, because a massive amount
of dissolved carbon amount was released from SCG in the soil. In
contrast, SCG-char application did not exhibit this phenomenon
because any easily released organic matter was removed previously
in the pyrolysis process.
Tsai et al. (2012) evaluated SCG as a potential feedstock for the
production of biochar via pyrolysis. The conditions used were:
Tpyrolysis ¼ 400e700  C, heating rate ¼ 10  C/min. It was reported
that the produced biochars showed high carbon content (>80 ww
%), fixed carbon (>60 ww%) and calorific value (>30.1 MJ/kg). The
produced char can be also used also as solid fuel in the industrial
sector due to high calorific value.
Researchers (Cho et al., 2017) investigated co-pyrolysis of paper
mill sludge mixed with SCG, focusing on biochar production. CO2
was used as reaction medium aiming to syngas generation
enhancement and biochar's physico-chemical properties modifi-
cation. The synergistic effects of CO2 and Fe/Ca caused a decrease in
pyrolytic oil. The presence of Fe/Ca in PMS favored CO generation
Fe-ions were converted into magnetite (Fe3O4) and porous biochar
was created. Cho et al. (2017) concluded that co-pyrolysis of paper
mill sludge and SCG, using CO2 as reaction medium could feasibly
generate CO and biochar, suitable for environmental applications.
3.3.4. Activated carbon production
Jung et al. (2016) prepared activated carbons from SCG into
calcium-alginate beads (SCG-GAC). The activated carbon powder
originated from SCG was used for the removal of acid orange 7
(AO7) and methylene blue (MB), from aqueous media. PH played a
highly important role in dye adsorption, whereas the influence of
ionic effects was essentially neutral. The pore diffusion model
describing the adsorption kinetics, revealed that the rate-limiting
step during the adsorption process was pore diffusion. The
maximum SCG-GAC adsorption capacity for AO7 at pH ¼ 3.0 was
estimated at 665.9, for MB 986.8 mg/g absorption obtained, at 30  C
and pH ¼ 11.0.
Different impregnation ratios of KOH were utilized by Laksaci
et al. (2017) for the synthesis of new activated carbons (ACs),
from SCG. Many functional groups were identified on the ACs sur-
face. BET measurement revealed a maximal specific surface area of
1778 m2 g1, for an impregnation ratio of 36 mmol of KOH/g. ACs
removal efficiency of phenol (Ph) and methylene blue (MB) mole-
cules was tested.
3.3.5. Nanocarbons production
Zein et al. (2017) studied the SCG microwave radiation to pro-
duce nanocarbons. They found that the optimum condition for
maximizing nanocarbons yield (60 ww%) obtained at 200  C,
650 W microwave power and 45 min residence time. They
concluded that this method could potentially produce spherical
shaped nanocarbons, which could be utilized for future scientific
innovations.
3.3.6. Liquid polyols production
Soares et al. (2014) investigated the possibility of SCG conver-
sion into liquid polyols, using acid liquefaction at moderate tem-
perature and autogenous pressure. They concluded that the
produced polyols have characteristics similar to those of
petroleum-based polyols, which are used in the polyurethane foam
industry.
3.3.7. Energy production
The possibility of using SCG for energy via combustion, was
proposed by Ciesielczuk et al. (2015). They used briquettes made of
mixed beech shavings and SCG, for increasing the calorific value.
SCG tested as a new bulking agent for biodrying of dewatered
sludge (DS). It was proved that SCG is an excellent bulking agent
that accelerates DS biodrying and produces a solid fuel with a high
calorific value (Hao et al., 2018).
3.3.8. Cogeneration of heat and power (CHP)
Food manufacturers have been piling into the bioenergy sector
turning waste and production by-products into energy, producing
enough heat and power for their own needs, with surplus energy
feeding back to the grid. Combined heat and power (CHP) can be
produced by SCG gasification. Cutting-edge, innovative and
economical gasification techniques with high efficiencies are a
prerequisite for the application of gasification. Feedstock types, the
impact of different operating parameters, tar formation and
cracking, and modelling approaches for biomass gasification of
biomass have widely studied.
Steam gasification of SCG was investigated by Pacioni et al.
(2016) in the temperature range of 650e850  C, with a steam par-
tial pressure range of 0.05e0.3 bar. A magnetic suspension ther-
mobalance was used for the gasification tests which were
performed isothermally. Gas chromatograph equipped with TCD/
FID detectors was used for gaseous products analysis. Product
characterization revealed that the products contained higher car-
bon and lower volatile matter compared to the original SCG and
had high calorific value. Temperature and steam partial pressure
influenced syngas production. H2þCO yields were higher for a
conversion range of 50e80%. The H2/CO ratio showed an increasing
trend with temperature.
To improve the feasibility and sustainability of SCG gasification,
technological advancement and the minimization of socio-
environmental effects are needed (Ingrao et al., 2018a).
 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566 1561

Table 5
SCG biorefinery approaches reported in literature.

No Reference Processes Parameters Products

1 Burniol-Figols et al. a. Phenols extraction Solvent: Ethanol Chlorogenic acid

(2016) Temperature: 70  C
L/Sa: 25 ml solvent/g TS liquid-solid
ratio
b. Acid hydrolysis 1 w/w% H2SO4
Temperature: 140  C
Time: 45 min
L/Sa: 10 g liquid/g TS
c. Ethanol Fermentation Strain: Saccharomyces cerevisiae Bioethanol
2 Obruca et al. (2015) a. Oil extraction Solvent: n-hexane Oil
b. Polyphenols extraction Solvent: Ethanol Polyphenols
c. Bacterial Fermentation Bacteria: Burkholderia cepacia PHAs
3 Caetano et al. (2017) a. 1st SCG Extraction Solvent: water/ethanol/supercritical CO High value extracts: antioxidants, caffeine, tannins, polyphenols,
etc.
b. 2nd SCG Extraction Triglycerides
c. Transesterification Biodiesel, Glycerin, Hydrogen
d. Drying & Pelleting Pellets
e. Pyrolysis and Torrefaction Biochar, biooil
f. Hydrolysis & Ethanol
Fermentation
4 Vardon et al. (2013) a. Oil extraction Oil
b. Transesterification Biodiesel
c. Slow pyrolysis Biochar, biooil
a
L/S ratio ¼ Liquid to Solid ratio.

3.4. Biorefinery approach

The European Commission has set a long-term goal to develop a

competitive, resource efficient and low carbon economy by 2050
(EC, 2011). Bioeconomy is expected to play an important role in the
low carbon economy. The European strategy for building a sus-
tainable bio-based economy with emphasis on the sustainable use
of natural resources, competitiveness, socioeconomic and envi-
ronmental issues, is on the spot (Scarlat et al., 2015).
Strategies relying on complete biomass disintegration through
combustion, gasification, or fermentation only, do not lead to
optimal utilization of biomass feedstock. Cascading approaches are
required to maximize biomass valorization (Ingrao et al., 2018a,
2018b; Zabaniotou et al., 2017, 2018).
In the waste-biorefinery concept, multifunctional processes are
integrated in an optimized sequence to utilize waste, with an
objective of maximizing the productivity of marketable in-
termediates and products (chemicals, materials, and bioenergy/
biofuels), to enhance of the process economics.
By searching carefully the international literature, 6 studies and
2 review papers were found, dedicated to explore the various SCG
Fig. 5. SCG biorefineries reported in literature.
biorefineries at laboratory scale, which signifies a low Technology
Readiness Level (TRL). All 8 papers were published during the last
two years (2016e2018). The two review papers published on 2018, concluded that for obtaining a wider product portfolio, several
summarise various SCG biorefineries. (Kourmentza et al., 2018; separation processes are required and a combination of biological
Mata et al., 2018). While the authors of the first review support and chemical processes is necessary. They also concluded that the
the SCG biorefinery approach, the authors of the second review most of them have limited scope and the final products have low
conclude that most of the studied biorefineries have limited scope economic value.
and low economic value (Mata et al., 2018).
The reported SCG biorefineries (2013e2018) integrate various
number of processes and products as shown in Table 5, Fig. 5. When 4. Discussion on SCG biorefinery approach
compared with the mono process/extraction proposals, it is clear
that the biorefinery allows a more complete utilization of SCG, by The valorization of SCG by a mono-process pathway has
obtaining high value products, using technologies and process attracted a lot of attention recently from both the academia and
already available at commercial scale. For applications in a Circular industry. However, very few studies dealt with the economic
Bioeconomy, the biorefinery approach is a corne stone (Karmee viability assessment of a mono-process approach of SCG
Sanjib Kumar, 2018). valorization.
Mata et al. (2018) in their review paper described several pro- Food wastes create huge environmental, economic, and social
posals for a SCG bio-refinery, and compared each other. They problems, being also sources of added-value materials. Coffee in-
dustries are a key sector in the global economy due to income
1562 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566
reporting and job creation. Coffee companies produce annually
more than 2 billion tons of by-products such as coffee spent
grounds (SCG) and coffee silverskin (CS). Proper design of a bio-
refinery system, aiming to a wide range of products generation
could serve as a unique sustainable solution to SCG wastes man-
agement and valorization in a Circular Economy.
Techno-economic analysis and optimization models are crucial
to design process scale, understand how major cost categories
affect the process and assess their sustainability. It is evident that
new business models introducing high-value bioproducts to bio-
refineries are essential for achieving economic viability of in-
dustries within Bioeconomy. Economically feasible production of
conventional bioenergy such as biofuels, biopower and bioheat, is a
challenge. Biorefineries must compete with the inexpensive fossil
fuel energies.
4.1. Prospects of SCG biorefinery
Besides, contributing to more sustainable and circular econo-
mies, the biorefinery has high commercial value when compared to
the ones obtained by currently used waste treatment methods. The
major advantage of biorefineries is their suitability for maximizing
valorization of structural and energetic potentials lying in biomass
(Budzianowski Wojciech, 2017).
The prospects of SCG biorefinery, as explored at laboratory level
and reported in the international literature, are very encouraging.
SCG can feed a biorefenery and via advanced chemical and
biotechnological methods, can produce a large number of value-
added products (polyhydroxyalkanoates, biosorbent, activated
carbon, polyol, polyurethane foam, carotenoid, phenolic antioxi-
dants, green composite) and bioenergy (biodiesel, bio-oil, biogas),
due to their rich composition in lipid, carbohydrates, carbonaceous,
and nitrogen containing compounds among others. However,
exploration at a high Technology Readiness Level (TRL), is still
lacking behind.
4.2. Economic viability and sustainability challenges
The economic viability is a decisive parameter for the bio-
refinery deployment. This was made obvious in a study performed
by Kookos I.K. (2018), who recommended that research on SCG
valorization should be oriented towards the efficient recovery of
the bioactive compounds for a more economically attractive con-
version. The economic performance of the biodiesel production via
a mono-process pathway is only viable at large production capac-
ities, realized at centralized facilities, despite that the environ-
mental assessment of the process showed that biodiesel production
has good environmental indicators.
Results from a recent study on the techno-economic analysis of
food waste biorefineries at European level, showed that the most
profitable options are those related to economies of scale. However,
the risk of increasing externalities due to logistics is possible
(Cristo bal et al., 2018).
There is a shortage in studies of a cascade SCG biorefinery.
Garcia et al. (2017) reported that hydrogen production via SCG
gasification biorefinery is viable, but without referring to the pro-
duction of high-value bioproducts. Mussatto et al. (2013) have
suggested the integrated biorefinery of the Brazilian case of spent
grains (BSG) for the production of xylitol, lactic acid, activated
carbon and phenolic acids integrated with heat production, as
viable pathway, because the economic viability and environmental
performance that achieved have shown positive indicators. The
obtained economic margin was evaluated at 62.25%, the potential
environmental impact was 0.012 PEI/kg products, and the carbon
footprint of the processing stage represented 0.96 kg CO2-e/kg of
BSG.
Apart from the economic viability, the environmental sustain-
ability of the SCG biorefinery is a request (Ingrao et al., 2018a,
2018b). The challenge is to produce value added products by inte-
grating different strategies that lead to an interconnected envi-
ronmental biorefinery for maintaining the ecological footprint.
However, sustainable biorefinery systems are still a challenge, since
weak designs lead to not viable solutions, with almost similar
environmental burdens with the petrochemical systems. They face
socio-economic issues related to land use, labor, food security and
others, sdditionaly (Moncada et al., 2016).
In the economic analysis, results must be evaluated taking into
account the high uncertainty that this kind of study entails, which
include the cost estimation and process parameters estimation for
low TRL technologies (Cristo bal et al., 2018).
4.3. Business development and market perspectives
It was made obvious that there is a need for design procedures of
economically feasible sustainable biorefineries that could meet
technical and market requirements and improve cascading biomass
utilization, (Budzianowski Wojciech, 2017). Methodologies for
biorefineriy conceptual design and optimization are needed. Ap-
proaches need to consider raw materials, technologies, processing
routes, products, and technical, economic, and environmental as-
pects. Processes must be optimized for the specific feedstock used
(due to variations on feedstock composition, cost and logistics of
process efficiencies and economics), coupled with energy gener-
ated from its residue (Mata et al. (2018).
The screening of sustainable SCG biorefinery pathways for the
production of bio-based products and energy is a complex chal-
lenge. Critical tools for predicting the commercialization feasibility
of biorefining pathway include laboratory and pilot-scale experi-
mental results, processes modelling, technoeconomic and market
analysis. More R&D is needed at higher Technology Reediness level
(TRL). Economic and environmental assessment for the practical
implementation of a SCG biorefinery at industrial scale is also
needed (Zabaniotou et al., 2017). High-value, low-volume bio-
products coupled to bioenergies, with a potential to improve eco-
nomic viability of biorefineries and biomass resource utilization,
are urgently required (Budzianowski Wojciech M., 2017).
It is difficult to assess which biorefinery will have a market
perspective because detailed economic analysis should be con-
ducted for each. It is suggested that integrated and holistic ap-
proaches for bio-waste utilization, as industrial feedstocks, will
boost the transition towards the bioeconomy era, the establishment
of which would expand and diversify the market outlets of bio-
based products (Maina et al., 2017). SCG biorefineries, as many
food waste-based biorefineries should be tailored to the local and
regional context, and to be profitable and sustainable in the long
term.
The scale should be analyzed in every biorefinery, during the
preliminary design stages. Different factors define the minimal
scale for biorefinery's feasibility. The number and quantity of high
added value products usually is associated with low scales
(Kachrimanidou et al., 2015).
4.4. Policy and regulations
Policy analysis is a new dimension to the sustainability assess-
ment of food waste reduction and valorization. Regulatory frame-
work and policy actions undertaken by local and global actors are
the drivers of change in food-waste reduction and valorization.
Today, very different national policies apply to bio-waste man-
agement, ranging from small action in some Member States, to
 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566
ambitious policies, in others. This can lead to increased environ-
mental impacts and can delay the full utilization of advanced bio-
waste management methods, while action on national level and
community is needed. The lack of a standard universal definition of
food waste has impact on the efficient use of by-products for
technological and commercial exploitation (Morone et al., 2017).
Mathematical mapping methods to assess food consumption
impacts and protocols, based on laboratory investigation and
demonstration, will formulate pathways for the sustainable valo-
rization of CSG and food waste in general (Morone et al., 2017;
Galanakis, 2017).
4.5. Indexes
A number of indexes related to economy and environmental
impacts have estimated by Salazar (2013). Indexes as a new basic
concept need to be applied for understanding the biorefinery effi-
ciency (Moncada et al., 2016).
The effective mass yield (EMY) and the Feature Complexity in-
dex (FC) are indexes that have been used in other waste-
biorefineries (Zabaniotou et al., 2018). The effective mass yield
(EMY) is defined as the percentage of the mass of the desired
products relative to the mass of used as feedstock. The Feature
Complexity (FC) of the biorefinery has to do with the number of
different features: it is increasing by the number of features, by the
state of technology of a single feature; it is decreasing with the
maturity of the technology (high TRL). This means that a high
Technology Readiness Level (TRL) of a feature has lower technical
and economic risks and a lower complexity. This led to the calcu-
lation procedure of the Biorefinery Complexity Index that the
complexity is directly linked to the number of features and the
Technology Readiness Level (TRL) of each single feature involved by
the IEA Bioenergy Task 42 ‘Bio refining’ (Jungmeier, 2009).
The Feature Complexities (FC) are rating from 1 to 9 according to
the TRL of the process (1e9); TRL1:basic (FC9), TRL2:applied
research (FC8), TRL3: critical function or proof of concept estab-
lished (FC7), TRL4: lab testing/validation of prototype (FC6), TRL5:
prototype system verified (FC5), TRL6: integrated pilot system
demonstrate(FC4), TRL7:system incorporated in commercial design
(FC3), TRL8: system incorporated in commercial design (FC2), TRL9:
system proven and ready for full commercial deployment (FC1)
(Jungmeier, 2009).
4.6. Circular economy
Food waste prevention is an integral part of the new Circular
Economy Package, with benefits such as boost of the global
competitiveness, sustainable growth and, generationof new jobs.
One of the issues of the Circular Economy model is the collection of
SCG and the scale of the endeavor.
The circularity of a coffee micro-economy naturally brings up
questions related to scalability. The collection of coffee grounds
requires storage space, proximity among participating buyers,
proximity to additional production facilities in which spent
grounds will be used, and numerous other logistical concerns.
Due to their high organic matter, SCG sometimes are used as a
fertilizer. However, SCG are highly toxic to the plants due to the
presence of caffeine, tannins, and polyphenols. In addition, due to
the presence of organic matter in SCG, a huge quantity of oxygen is
required for their degradation in landfills. Simultaneously,
methane, which is a greenhouse gas and even more harmful than
carbon dioxide, is also released in the landfills, contributing to
global warming. Therefore, usual disposal methods need to be
replaced by more sustainable towards increased resources recovery
and higher energy efficiency. Valorization of this waste towards
1563
material and energy recovery rather than disposal, is gaining
interest.
Although, the biorefinery concept is considered as one of the
research cornerstones in the last years and as the best option to
transform the different waste systems by a multi-process, multi-
product pathways, (Moncada et al., 2016), there is a shortage of
analysis of the potential benefits on associated business
development.
Only one paper found in the book of Morone et al. (2017), to
assess the logistics, economical and social feasibility to isolate SCG
from the catering industry and use them as raw material for a novel
process to produce alternative high added value products in a near-
perfect circular economy cycle, making use of reverse logistics and
generating near-zero waste (Topi and Bilinska, 2017). The study was
based on a series of theoretical scenarios corresponding to the
different possible logistic and process options that stakeholders
could identify. This theoretical approach concluded that the process
is technically feasible with available technology within current
infrastructure and modest investments and the economic case is
very attractive to investors.
Some international companies of coffee beverage have started
to devote efforts on sustainable valorization of SCG, advocating
Circular Economy model, by organizing collection systems and
exploring technological pathways for valorization (Bernstein,
2012).
Alternative scenarios for using the SCG to produce alternative
high added value products should be considered and developed, by
using the participatory mapping approach and economic, envi-
ronmental and social benefits compared with compost production
scenarios (Morone et al., 2017).
4.7. Design guidelines
Reflections and guidelines for sustainable biorefinery concepts
are mainly proposed by Moncada et al. (2016). These include the
following quotes that could be also suggested for a SCG biorefinery
design.
 Integration increases the efficiency.
 Integrated technologies should have priority over separated
technologies.
 Integration of cogeneration CHP using biorefinery solid residues
is suggested.
 Energy integrations levels are important to reach maximum
energy efficiency levels.
 Include as many as possible products in the biorefinery.
 Cascade approaches are sustainable pathways in the circular
economy.
 Innovative engineering solutions should be preferred.
 The CHP gasification technology has a better performance than
the technology based on direct combustion.
 The use of modern tools and strategies of analysis and evalua-
tion for environmental, technical, and economic impacts is very
important.
 The implementation of optimization strategies and models
could be interesting when coupling with further design.
 Supply chain and logistics are essential part of a green
biorefinery.
 Use of indexes is important.
In addition to the above, conducting sensitivity analyses for
comparison of different systems, enables global evaluation and
rating of those systems on the same scale of normalized values. LCA
can be used as a valid tool to support designers, decision-makers
towards promotion of more sustainable options of SCG
1564 A. Zabaniotou, P. Kamaterou / Journal of Cleaner Production 211 (2019) 1553e1566
valorization for energy, fuel, biochar and high added value/low
volume products (Ingrao et al., 2018b), although weighing is based
often upon social or political considerations (De Benedetto and
Klemes, 2009). Therefore, weighing step could be recognized as
mandatory by the subject International Standards (Ingrao et al.,
2018b; 2018a).
5. Conclusions
This study was conducted to review the field of SCG valorization,
its prospects, potentialities and challenges. The review attained the
proposed goal, as it brought important issues of the SCG mono- and
biorefinery valorization options, as reported in the international
literature. Limitations were found in extrapolating information and
results from the papers reviewed, since each paper explored
different end-products and processes, so evaluations and compar-
isons were difficult to be made.
The review allowed the authors to deepen the knowledge in the
SCG biorefinery, that represents the platform to start the devel-
opment at higher TRL, for further integration and optimization of
SCG recycling systems. It allowed the development of knowledge-
based strategies to unlock the potential of SCG, produce bio-
derived chemicals, fuels and carbon materials, and probably effect
waste management regulations.
The review focus was centered upon SCG, which is an important
food waste of global society, containing substances that make it a
valuable bio-resource. Today, food wastes are a major concern and
require for their management advanced techniques with economic
benefits and environmental safety. It was made evident, that the
development of sustainable and efficient refining of SCG depends
on the spectrum of various end-products, market outlets and cost-
effective processing schemes. It was documented that poly-
saccharides, phenolic compounds, tannins, biodiesel, bioethanol
can be produced from the SCG, by using mono-extraction pro-
cesses, while a cascade biorefinery can produce fuels, energy, car-
bon materials and biochar, in a closing loop approach, in addition.
SCG cascade or integrated biorefinery seems to be a more
economically viable and resource efficient option, compared to
strategies relying on complete biomass disintegration, that do not
lead to optimal utilization of biomass feedstock. Cascading ap-
proaches are favorable because they maximize biomass recycling
with material and energy recovery. Besides, contributing to more
sustainable and circular economies, SCG cascade biorefinery seems
to have a commercial value.
A shortage of economic and environmental assessments was
observed in the international literature, so it was difficult to draw
concise economic and environmental conclusions for the SCG bio-
refinery options, with the exception of a study performed by Bra-
zilian researchers (Mussatto et al., 2013), on integrated biorefinery
of the Brazilian case of spent grains (BSG) for the production of
xylitol, lactic acid, activated carbon and phenolic acids, integrated
with heat production. This study provided good economic and
environmental indicators, with an economic margin of 62.25%,
potential environmental impact of 0.012 PEI/kg products, and the
carbon footprint of the processing stage represented 0.96 kg CO2-e/
kg of BSG.
Considering findings from this review, it seems that efforts are
required to sustainability assessment, policy analysis and national
regulatory framework harmonization to the EU, that are the drivers
of change in food-waste reduction and valorization. Different na-
tional policies apply to bio-waste management, can delay the uti-
lization of advanced bio-waste valorization methods. There is an
urgent need for creation of technical standards and indicators to
guide and regulate the assessment of the sustainability of SCGs-
based biorefineries. LCA proposed as a valid tool to support
designers, and decision-makers towards promoting and developing
sustainable solutions.
Only one paper found to assess theoretically SCG collection and
valorization in a circular economy (Topi and Bilinska, 2017),
concluding that collection and valorization of SCG is technically
feasible with available technology, within current infrastructure,
and modest investments. In this case, the economic case is very
attractive to investors.
Based upon the analysis of the papers, the authors found that
there is an urgent need for R&D, effective regulations, methodo-
logical approaches to design and estimation of the SCG collection
systems, investment and manufacturing costs, indicators develop-
ment for assessments prior to the development of new business
models within a Circular Bieconomy. Through the review some
guidelines were highlighted, useful for the design of biorefineries.
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