Chemical Engineering Journal 451 (2023) 138485

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Chemical Engineering Journal

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

Model quantification of the effect of coproducts and refinery

co-hydrotreating on the economics and greenhouse gas emissions of a
conceptual biomass catalytic fast pyrolysis process
Abhijit Dutta a, *, Hao Cai b, Michael S. Talmadge a, Calvin Mukarakate a, Kristiina Iisa a,
Huamin Wang c, Daniel M. Santosa c, Longwen Ou b, Damon S. Hartley d, A. Nolan Wilson a,
Joshua A. Schaidle a, Michael B. Griffin a
a
National Renewable Energy Laboratory (NREL), 15013 Denver West Parkway, Golden, CO 80401, United States
b
Argonne National Laboratory (ANL), 9700 S Cass Ave, Lemont, IL 60439, United States
c
Pacific Northwest National Laboratory (PNNL), 902 Battelle Blvd, Richland, WA 99354, United States
d
Idaho National Laboratory (INL), 1955 N Fremont Ave, Idaho Falls, ID 83415, United States

A R T I C L E I N F O A B S T R A C T

Keywords: In this work we present model results for a scaled-up conceptual process informed by bench scale biomass
Techno-economic analysis catalytic fast pyrolysis (CFP) and hydrotreating experimental data. This process uses a Pt/TiO2 catalyst during
Lifecycle analysis CFP, which produces a partially deoxygenated organic biocrude intermediate that is then hydroprocessed to a
Biomass catalytic fast pyrolysis
hydrocarbon fuel blendstock; the catalyst also enables high yields of acetone and methyl-ethyl-ketone (MEK)
Refinery coprocessing
Biorefinery coproducts
coproducts. Two options for hydroprocessing were modeled: (A) co-hydrotreating at a petroleum refinery using
hydrogen sourced from steam reforming of natural gas and (B) standalone hydrotreating at a biorefinery using
hydrogen sourced from CFP off gases. The results revealed that Case A was economically advantageous with a
modeled minimum fuel selling price (MFSP) of $2.83/GGE or gallon gasoline equivalent (in 2016 US dollars),
while the additional cost of standalone hydrotreating facilities in Case B increased the MFSP to $3.13/GGE.
Conversely, greenhouse gas (GHG) emissions were lower for Case B (3.9 g CO2e/MJ) compared to Case A (21.5 g
CO2e/MJ) due to the use of biogenic (Case B) and fossil-derived (Case A) hydrogen. In a third option (Case C), the
requirements for separation and purification of acetone and MEK were removed from the refinery co-processing
scenario (Case A) to evaluate the impacts of this process simplification. Elimination of these coproducts increased
the MFSP to $3.21/GGE and GHG emissions to 35 g CO2e/MJ. These comparisons based on our detailed con­
ceptual models provide economic and sustainability guidance regarding processing choices for future bio­
refineries. While refinery coprocessing using existing equipment and the production of relatively valuable
coproducts can benefit the economics, the hydrogen-source and biogenic coproducts can have significant impacts
on the sustainability of the process, and feasibility to use CFP off-gases or other renewable sources for hydrogen
production can help lower GHG emissions.

1. Introduction infrastructure-compatible hydrocarbon fuels is impeded by oxygen

The transportation sector is the largest source of CO2 and greenhouse
gas (GHG) emissions in the U.S., contributing about 35 % of CO2 and 28
% GHG emissions in 2019 [1]. Liquid fuels from biomass are an
important tool for increasing the sustainability of transportation fuels.
Oxygenated polymeric materials (cellulose, hemicellulose, and lignin)
are the primary constituents of biomass. Conversion of biomass to
present in the biomass (~40 wt% in woody material). Deoxygenation
and hydrogenation chemistries are necessary to produce hydrocarbon
liquid fuels from biomass. Fast pyrolysis (FP) of biomass is a thermal
conversion process capable of producing significant proportions of an
oxygenated liquid intermediate known as pyrolysis oil. However, the
pyrolysis oil from FP retains a similar high proportion of oxygen as in the
source biomass. The oxygen renders the pyrolysis oil unstable, with

* Corresponding author.
E-mail address: abhijit.dutta@nrel.gov (A. Dutta).

https://doi.org/10.1016/j.cej.2022.138485

Available online 9 August 2022

1385-8947/© 2022 Elsevier B.V. All rights reserved.
A. Dutta et al.
Fig. 1. Simplified block flow diagram of the conceptual process.
strong propensity to react and polymerize. Catalytic fast pyrolysis (CFP)
involves the catalytic upgrading of pyrolysis vapors [2], either in situ
(catalytic upgrading within the fast pyrolysis reactor) or ex situ (catalytic
upgrading in a separate reactor immediately following the fast pyrolysis
reactor), with or without supplemental hydrogen (depending on the
process configuration and catalyst) [3,4].
Catalytic upgrading can significantly reduce the oxygen content and
associated reactive functional groups (sugars, acids, aldehydes etc.),
thus producing a more stable CFP oil or biocrude. The FP process also
produces solid char, while additional coke is deposited on the catalyst
for CFP. The char and coke are usually combusted for providing heat to
the endothermic pyrolysis reactions, and excess heat can be used for
process heat, steam generation, and electricity production. Permanent
gases formed in FP/CFP have heating value and, like the char, can be
similarly used for thermal and energy needs; in addition, the gases can
be used to produce hydrogen via steam reforming. Our conceptual
process uses hydrogen during CFP; hydrogen is also necessary for
downstream hydroprocessing of the CFP biocrude because this liquid
intermediate still retains oxygen (although the oxygen content is lower
than in non-catalytic pyrolysis oil); the proportion of oxygen remaining
in the CFP biocrude is dictated by the specifics of the CFP process and the
catalyst used. Thus, finishing steps, such as hydrotreating, are necessary
for near-complete deoxygenation of the CFP biocrude to infrastructure
compatible liquid hydrocarbon fuels/blendstocks. This final deoxygen­
ation process may involve standalone hydroprocessing or coprocessing
at a petroleum refinery. Coprocessing at a refinery can provide economic
advantages when using existing equipment and infrastructure.
In addition to the solid, liquid, and gaseous fuel/energy outputs,
valuable chemicals may be separated and purified from the gaseous and
liquid products. Once again, the types of products are dictated by the
choice of the CFP catalyst and its selectivity. The products may include
oxygenated chemicals, e.g., acetone and methyl-ethyl ketone (MEK), as
described in this article, or may be selective towards other products such
as olefins and aromatics [5,6]. Separation and purification of these
products may be capital and energy intensive, depending on the con­
centrations of desirable product molecules and the presence other
contaminants.
In this article we project economic and sustainability impacts using
three variations of our conceptual design of a CFP process with a fixed
bed ex situ reactor:
• Case A: Production of coproducts; co-hydrotreating the CFP biocrude
at a petroleum refinery
• Case B: Production of coproducts; hydrotreating at the biorefinery
(capital investment necessary for the hydroprocessing)
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Chemical Engineering Journal 451 (2023) 138485
• Case C: Co-hydrotreating at a petroleum refinery; no production of
coproducts (avoiding expenditure related to separation and purifi­
cation of chemicals)
1.1. Prior work and focus of this article
We previously published a detailed conceptual design-based techno-
economic analysis (TEA) for in situ and ex situ CFP using fluidized cat­
alysts [2] to establish effective goals for our research. We further
adapted the conceptual design for the TEA of a fixed bed ex situ CFP
reactor system [7]. Our research progress based on bench scale experi­
ments and their impacts on modeled production costs have been tracked
annually since 2014 [8,9] and details of our experimental research
progress were documented by Griffin et al. [10]; supply chain sustain­
ability was also tracked in a separate annually-updated report [11]. In
addition to our publications, we have posted sample Aspen Plus process
models and Excel-based economic models from our work on an NREL
website [12].
A comparative sustainability and economic analysis of the three
cases mentioned above (Cases A, B, C), informed by experimental work
in 2020–21, is the focus of this article. Sufficient high-level information
is provided to allow the reader to understand the material without
having to refer to the previous detailed publications. It should be
appreciated that the projections in this article are based on a conceptual
design informed by bench scale experiments, and there remain technical
and scale-up challenges for CFP technologies to achieve the maturity
necessary for broad implementation and continuous problem-free
operation at large scales.
2. Methods
2.1. Conceptual process
The CFP process design presented in this analysis includes a fast
pyrolysis reactor, hot gas filter, fixed bed ex situ catalytic upgrading
reactor, a condensation system, recovery of light oxygenated coproducts
from non-condensable gases, and hydroprocessing of the CFP biocrude
to hydrocarbon fuel blendstocks. The process model also includes
detailed heat integration with electricity production from excess heat,
hydrogen production from off gases, wastewater treatment and other
utilities. The process model was built in Aspen Plus [13]. A simplified
flow diagram is shown in Fig. 1.
2.1.1. Feedstock production and handling
Woody feedstock with a 50:50 wt% blend of clean pine and logging
A. Dutta et al.
residues was used as the modeled feedstock [14], reflecting the feed
mixture used in our bench scale experiments in 2020–21 [9]. The con­
ceptual model is based on a 2,000 dry metric tons (MT) per day of this
feedstock. The elemental analysis of the feed in the model was: C =
50.51 %, H = 5.99 %, N = 0.17 %, S = 0.03 %, O = 41.55 %, Ash ≤ 1.75
%; the modeled feedstock cost was $67.03/dry short ton ($73.89/dry
MT). The ash content in our experimental 50:50 blend was < 1 %.
Deliberate ash reduction for a consistent ash content of < 1 % for this
blend would add a small cost, with an increase in the modeled feedstock
cost to $70.15/dry short ton ($77.33/dry MT). The modeled moisture
content of the feed was 10 wt%.
2.1.2. Catalytic fast pyrolysis
The catalytic fast pyrolysis system design in our model includes (i) a
fast pyrolysis reactor system, (ii) a hot gas filtration system, and (iii) a
fixed bed ex situ catalytic vapor upgrading reactor system. Fast pyrolysis
of biomass takes place in an entrained flow reactor at approximately
500 ◦ C with short residence times of about 2 s. A portion of the gas
stream (remaining after downstream condensation and recovery of
condensables) is enriched with hydrogen and is used as the fluidizing
medium for the pyrolysis reactor. Heat required for pyrolysis is provided
by hot circulating sand from the char combustor. Upon pyrolysis the
biomass breaks down into gases and vapors, leaving solid carbonaceous
char. The char is separated from the vapor phase via cyclones. The solids
(sand and char) from the cyclones are sent to the char combustor where
the char is combusted in a fluidized bed to heat the sand, and the hot
sand is then sent back to the pyrolysis reactor. The vapor phase is sent to
a hot gas filter to remove particulates before the vapors enter a separate
(ex situ) fixed bed catalytic reactor with Pt/TiO2 catalyst operated at
approximately 400 ◦ C. The vapors are upgraded in the catalytic reactor,
rendering the product stream less reactive prior to the following
condensation step.
2.1.3. Condensation system, with coproducts recovery and purification
The vapors are first condensed in a direct-quench tower where the
light organic condensate from downstream is used as the quench liquid.
A heavy organic phase condenses out and is drawn as the bottom
product. The uncondensed vapors are then partially condensed via in­
direct heat exchange before they enter a second direct-quench
condenser tower. The bottom condensate separates into organic and
aqueous phases in a decanter. The light organics are used as the quench
liquid in both direct-quench condensation towers via partial recycle, and
the remaining light organics are drawn. The light and heavy organic
product streams from the two condensers are mixed. This mixed organic
biocrude contains 16.6 wt% oxygen and retains 35.7 % of the carbon
contained in the biomass. The aqueous phase contains dissolved
carbonaceous species, retaining 1.8 % of the carbon in biomass. The
aqueous phase is sent to wastewater treatment where the carbon is
combusted in a Regenerative Thermal Oxidizer (RTO). All our modeled
values were informed by bench-scale experiments.
Non-condensable gases and lighter species remain uncondensed in
the gas/vapor stream from the top of the second direct-quench
condenser. The light condensables contained 13 % of the biomass car­
bon. Light oxygenates made up most of these condensables with acetone
(4.3 %), acetaldehyde (3.5 %), and MEK (1.4 %) retaining the largest
proportions of biomass carbon. Acetone and MEK are commercial
chemicals, and hence we studied their recovery and purification to
chemicals grade. The vapor phase after the condensation system was
sent to an adsorption/desorption system with silica gel. This was
modeled based on preliminary experiments showing that nearly 100 %
of acetone and MEK can be captured from the vapor stream. The puri­
fication of acetone and MEK from the remaining condensable com­
pounds was modeled. The speciated composition of the desorbed stream
was modeled using the UNIFAC-DMD [15] predictive property method
in Aspen Plus. Multiple distillation columns and a few decantation steps
allowed 70 % and 39 % modeled recoveries of the desorbed acetone and
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Chemical Engineering Journal 451 (2023) 138485
MEK with purities of 97.7 % and 99.6 % respectively. Note that these
results are based on preliminary proof-of-concept experiments; more
experimental research is necessary to improve our understanding of the
adsorption/desorption system and validate the modeled purification of
acetone and MEK from the desorbed stream.
As mentioned earlier, the gas stream after the adsorption stage was
partially recycled to the pyrolysis reactor for fluidization. The remaining
stream was sent to a water–gas shift reactor to convert carbon monoxide
and supplemented steam to hydrogen. Hydrogen was recovered in a
pressure-swing adsorption (PSA) system for use within the process. The
off gases from the PSA were used as fuel gas, and a smaller fraction sent
to the steam reformer for hydrogen production; off-gas use in the con­
ceptual process is dictated by hydrogen production requirements, with
the excess off-gases being combusted for additional heat for steam
generation and electricity production.
2.1.4. Hydroprocessing
The following sub-sections describe the process designs for the
standalone hydroprocessing scenario (Case B) and the cost bases for
refinery co-hydrotreating (Cases A and C). Relevant bench-scale exper­
iments that informed our assumptions are also mentioned.
2.1.4.1. Standalone hydroprocessing. Standalone hydroprocessing of
CFP biocrude at a biorefinery is modeled as a combination of three
operations: (i) hydrotreating, (ii) hydrocracking, and (iii) distillation.
The biocrude is first sent to a single step hydrotreater operating at
400 ◦ C and 13 MPa, where the biocrude is deoxygenated to < 1 wt%
oxygen [10]. The hydrotreated product is then sent to a distillation
system with two columns where gasoline, diesel, and heavier-than-
diesel fractions are separated. The heavier fraction is sent to a hydro­
cracker, where the heavy molecules are hydrocracked to diesel and
gasoline range molecules. The hydrocracker is modeled at 420 ◦ C and
13.5 MPa [2]. The cracked product stream is fed to the same distillation
system for separation into the gasoline and diesel fuel blendstocks. After
the products from the hydrotreater and hydrocracker are condensed,
these operational areas recycle their hydrogen-rich gas streams to their
respective reactors. The model maintains a hydrogen purity of 90 mol%
in the recycled gas to the hydrotreater and hydrocracker by purging a
portion of the gases and enriching the stream with supplemental
hydrogen. Hydrogen production and consumption (both for hydro­
processing and CFP) play a significant role in the economics and sus­
tainability of the process. This standalone hydroprocessing design is
presented with details in our 2015 design report [2].
2.1.4.2. Refinery Co-hydrotreating. Bench scale experiments were con­
ducted to understand the feasibility of effective deoxygenation of the
CFP oil in a co-hydrotreating environment. A 10:90 vol% ratio of CFP
biocrude and straight-run diesel (SRD) were fed into bench-scale
hydrotreater. These bench scale experiments were conducted at PNNL
and NREL for at least 50 h each, at 8.3 MPa, 340 ◦ C over a NiMo/
alumina catalyst. The results demonstrated effective hydrotreating of
the CFP biocrude with approximately 95 % carbon efficiency for bio­
crude conversion, without adverse impacts on the catalyst. Longer term
studies are necessary along with further scale-up and research ad­
vancements for potential future industrial implementation; we used the
bench scale performance to inform our TEA for a potentially successful
future implementation of co-hydrotreating at a petroleum refinery. Co-
hydroprocessing continues to be an active area of research [16].
Refinery co-hydroprocessing will likely follow a different set of steps
compared to the standalone hydroprocessing steps described above. For
biocrudes with > 10 wt% oxygen, the stoichiometry of deoxygenation
and associated hydrogen consumption are expected to dominate any
hydroprocessing economics. Hydrogen consumption, dictated by stoi­
chiometry, will be comparable for similar levels of deoxygenation, hy­
drogenation, and carbon efficiencies for biocrude in both standalone and
A. Dutta et al.
refinery co-hydroprocessing scenarios. In our co-hydroprocessing TEA,
we envisioned the reuse of refinery equipment without significant
additional capital expenditure; this will be one of the biggest incentives
for future petroleum refinery coprocessing of biocrudes. Initial intro­
duction of biocrudes in low proportions can help gain understanding
before higher proportions of biocrude are introduced. Since we expect
hydrogen costs to be the dominant cost for biocrude hydroprocessing,
we used the hydrotreating hydrogen consumption from our detailed
standalone model as the basis for prorating all refinery operating costs
associated with biocrude processing, including natural gas for hydrogen
production, electricity, steam, and catalysts; note that our preliminary
co-hydrotreating results indicated < 0.5 wt% oxygen in the product
samples, indicating successful conversion of the oxygenated CFP inter­
mediate to hydrocarbons. The costs were estimated using information
provided by Kaiser, Gary, and Handwerk [17] for different hydro­
processing units at petroleum refineries; the various operating costs
were correlated with reported hydrogen consumptions. A key difference
between the standalone and co-processing cases is in the source of
hydrogen. While biorefineries can use biogenic off gases for hydrogen
production, it is assumed that most current petroleum refineries will use
natural gas derived hydrogen.
2.1.5. Hydrogen consumption and production
Both the CFP and hydroprocessing operations require hydrogen in
our conceptual design; for the specific model assumptions in the
standalone hydroprocessing configuration, hydrogen consumptions
were 260 (CFP), 143 (hydrotreating), and 104 (hydrocracking) in units
of gH2/GGE fuel produced; these correspond to 4534 (CFP), 2489
(hydrotreating), and 1805 (hydrocracking) scf/barrel gasoline equiva­
lent fuel produced. Steam reforming of off gases from CFP is sufficient to
provide all the hydrogen necessary for both operations in the standalone
biorefinery case (Case B). For the refinery coprocessing cases a smaller
proportion of the off gases can meet the hydrogen demand for CFP;
hydroprocessing, when deferred to the petroleum refinery, uses natural
gas derived hydrogen. Three hydrogen recycle loops exist in our
standalone design: (i) CFP fluidizing gas recycle loop, (ii) hydrotreating
gas recycle loop, (iii) hydrocracking gas recycle loop. A water gas shift
(WGS) reactor followed by a PSA is used to produce hydrogen from
carbon monoxide and supplemental steam in the CFP loop; however, the
hydrogen produced via WGS is not sufficient, and needs to be supple­
mented by hydrogen from the steam reformer. Similarly, the hydro­
treating and hydrocracking loops need makeup hydrogen to maintain
the 90 mol% hydrogen purity specified in the model. The steam reformer
uses a portion of the off gases as the reformer feed and the remainder as
reformer fuel. The steam reformer is also followed by a WGS reactor to
increase hydrogen production and PSA to allow the production of high-
purity hydrogen. For refinery co-hydrotreating, we assume the use of a
conventional natural gas steam reforming system for hydrogen pro­
duction [17].
2.1.6. Steam and electricity generation
The excess high-quality heat from char and off gas combustion is
used for steam generation, followed by electricity production [2]. A
higher proportion of off gases are available for energy uses at the bio­
refinery when hydroprocessing is deferred to the petroleum refinery,
because that lowers the hydrogen demand at the biorefinery. As a result,
more electricity is produced at the biorefinery in the coprocessing cases
when compared to the standalone case.
2.1.7. Heat integration
Significant heat integration is necessary in this process to improve
overall energy efficiency. A detailed pinch analysis and the design of a
heat exchange network for ex situ CFP was presented in our 2015 design
report [2]. For subsequent modifications of our model, such as in the
cases discussed in this paper, we scaled our process heat exchange costs
using the total process heat exchange network duty. We verified
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Chemical Engineering Journal 451 (2023) 138485
thermodynamic legitimacy by checking that a minimum approach
temperature between hot and cold streams is maintained in all our
models.
2.1.8. Other utilities
As mentioned earlier, our design includes a regenerative thermal
oxidizer (RTO) to combust the carbon in the aqueous waste stream. This
design was used to avoid uncertainties related to biological methods for
wastewater treatment, given that CFP products can vary and contain
numerous compounds, and may raise questions about the effectiveness
of biological treatment. Additional utilities such as air coolers, a cooling
water system, and chilled water are included in our design and costs.
2.2. Process modeling
An integrated process model was developed in Aspen Plus [13].
Biomass was represented as a non-conventional component. Since fast
pyrolysis processes produce thousands of compounds, and products are
not completely speciated, we used surrogate compounds to represent FP
and CFP products. A list of compounds is available in Appendix F of
reference [2]. The Peng-Robinson method with Boston-Mathias modi­
fication (PR-BM method in Aspen Plus) was used as the thermodynamic
method in most of the model (UNIFAC-DMD was used for coproduct
purification modeling, as mentioned previously). Steam tables were
used where water was the primary component, such as in the steam
system. Pinch analysis was done in an Excel spreadsheet by importing
information about temperatures and heat duties from the Aspen Plus
model. The model design methods are documented in detail in our 2015
design report [2]. Subsequent model modifications since the 2015 report
covered changes necessary to represent new experimental configura­
tions and results. While the lighter compounds are usually well quan­
tified by analytical methods like GC–MS and those compounds are also
available in Aspen Plus databanks, properties of some heavier surrogate
compounds (e.g., Table F-2 in reference [2]) needed to be estimated in
Aspen Plus after specifying their structures. Pseudo-components were
not used for representing hydrocarbon fuel products; these products
were represented by surrogate compounds spanning the boiling ranges
seen in experimental distillation. While a yield reactor block (RYIELD in
Aspen Plus) was used to represent the breakdown of biomass in the fast
pyrolysis reactor, the subsequent reactors (fixed bed ex situ pyrolysis
vapor upgrading, hydrotreater, and hydrocracker) were represented by
stoichiometric reactors (RSTOIC in Aspen Plus). Relevant surrogate re­
actants and products were chosen in the RSTOIC reactors. Kinetic
models were not used since experimental data metrics such as product
distillation ranges, elemental analyses, measured gaseous products etc.
could be conveniently represented using surrogate molecules in stoi­
chiometric reactors, instead of having to constantly change kinetic
models to represent the different experimental results obtained during
our research.
2.3. Economics
Flow rates from the Aspen Plus model were imported into an Excel
spreadsheet for economic calculations. Most of the equipment was
costed using Aspen Capital Cost Estimator (ACCE); custom equipment
such as the CFB system for fast pyrolysis were costed with inputs from an
engineering firm [2]. The results are presented in 2016 US dollars; the
Chemical Engineering Plant Cost Index [18], PPI industry sub-sector
data for Chemical Manufacturing [19], and a US labor index [20]
were used to convert our available cost information to a 2016 US$ basis.
Equipment costs for specific versions of the model are derived by scaling
base equipment costs using flow rates from the model. Details of unit
cost bases for calculating variable operating costs are presented in a
previous report (Table 7 in [9]). Note that our analysis is based on
mature plant assumptions with 90 % onstream time and 30-year plant
life, and do not include uncertainties and substantial additional costs
A. Dutta et al. Chemical Engineering Journal 451 (2023) 138485

Fig. 2. Steps within farm to wheels system boundary for LCA.

Table 1
Equipment and installation costs at biorefinery (2016 US$).

incurred for pioneer plants. Financing includes 40 % equity with 10 %
internal rate of return, and 60 % debt repaid over 10 years with 8 %
annual interest; a 21 % income tax rate was assumed. Other financial
details such as depreciation, startup assumptions etc. are available in our
previous report (Table 1 in [9]).
2.4. Lifecycle analysis (LCA)
GHG emissions is the key environmental metric reported in this
study; it includes CO2, CH4, and N2O emissions with 100-year Global
Warming Potential bases of 1, 30, and 265, respectively [21]. Fig. 2
shows the five key steps within the LCA system boundary: (1) biomass
production includes fertilizer and energy inputs, and GHG emissions
include N2O and impacts of land-use changes; (2) biomass preprocessing
logistics accounts for fuel and energy consumed during all preprocessing
operations, including harvesting, processing such as size reduction and
drying, storage, and transportation; (3) biomass conversion via CFP is
detailed in this paper, and GHG emissions are accounted based on the
inventory of material and energy flows from the Aspen Plus process
models for the three cases; (4) fuel distribution primarily accounts for
emissions from transportation of the biofuel for retail; (5) fuel com­
bustion accounts for final emissions when the biofuel is used in a vehicle
(note that all the carbon in the produced fuel is biogenic). Mega-joule
(MJ) is our energy-based functional unit for the use of biofuels in ve­
hicles. The 2021 release of the Greenhouse gases, Regulated Emissions,
and Energy use in Technologies (GREET®) model [22] was used for our
LCA. The GREET model is sponsored by the U.S. Department of Energy
and is publicly available.
The three cases presented here involve variations only within the
biomass conversion step shown in Fig. 2; assumptions for all other steps
are consistent across the three cases.
Coproducts in some of the CFP conversion strategies may have sig­
nificant emissions impacts and affect the fuel carbon intensity. We used
a displacement method to address the acetone and MEK coproducts in

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A. Dutta et al. Chemical Engineering Journal 451 (2023) 138485

Table 2
Total capital investment calculations (2016 US$).
Case A Case B Case C

Total Purchased Equipment Cost (TPEC) $142,560,000 $163,840,000 $135,900,000

Installation factor 2.064 2.030 2.118
Total Installed Cost (TIC) $294,270,000 $332,620,000 $287,800,000

Other direct costs

Land (not depreciated) $1,610,000 $1,610,000 $1,610,000
Warehouse 4.0 % of ISBL $6,360,000 $7,640,000 $6,090,000
Site development 10.0 % of ISBL $15,910,000 $19,110,000 $15,220,000
Additional piping 4.5 % of ISBL $7,160,000 $8,600,000 $6,850,000
Total Direct Costs (TDC) $323,700,000 $367,970,000 $315,950,000

Indirect costs % of total direct cost (excl. land)

Prorated expenses 10.0 % $32,370,000 $36,800,000 $31,600,000
Home office and construction fees 20.0 % $64,740,000 $73,590,000 $63,190,000
Field expenses 10.0 % $32,370,000 $36,800,000 $31,600,000
Project contingency 10.0 % $32,370,000 $36,800,000 $31,600,000
Other costs (startup and permits) 10.0 % $32,370,000 $36,800,000 $31,600,000
Total indirect costs 60.0 % $194,220,000 $220,780,000 $189,570,000

Fixed Capital Investment (FCI) $517,920,000 $588,750,000 $505,520,000

Working capital 5.0 % of FCI (excluding land) $25,900,000 $29,440,000 $25,280,000
Total capital investment (TCI) $543,820,000 $618,190,000 $530,800,000

TCI/TPEC 3.815 3.773 3.906

FCI Lang Factor = FCI/ISBL TPEC 6.997 6.415 7.574
TCI Lang Factor = TCI/ISBL TPEC 7.347 6.735 7.953

Table 3 Table 4
Fixed operating costs (2016 US$). Production summary.
Cost Item Factor Case A Case B Case C Product Unit Case A Case B Case C

Salaries $3,440,000 $3,440,000 $3,440,000 Gasoline Blendstock million liters/y 87.0 87.0 90.3
Benefits and 90.0 % of total $3,100,000 $3,100,000 $3,100,000 Diesel Blendstock million liters/y 76.5 76.5 74.1
overhead salaries (after Total Gasoline Equivalent million LGE/y 168.5 168.5 169.3
adding 10 %) Acetone million kg/y 19.2 19.2 0.0
Maintenance 3.0 % of fixed $15,540,000 $17,660,000 $15,160,000 MEK million kg/y 3.3 3.3 0.0
capital Electricity kW 26,407 8242 34,284
investment
(FCI a)
Insurance 0.7 % of fixed $3,620,000 $4,120,000 $3,540,000
and taxes capital Table 5
investment Cost contributions towards the total MFSP.
(FCI a)
Cost Item Case A Case B Case C
Total fixed operating costs $25,700,000 $28,320,000 $25,240,000
(2016$/year) cents/GGE cents/GGE cents/GGE
(cents/LGE) (cents/LGE) (cents/LGE)

Feedstock 108.2 (28.6) 108.2 (28.6) 107.7 (28.4)

the current process; the displacement method was applied because of the
Natural Gas 0.2 (0.1) 0.1 (0) 0.1 (0)
modest amounts of these coproducts relative to the yields of the fuel Catalysts 9.1 (2.4) 15.5 (4.1) 9 (2.4)
products. The displacement method assigns an emission credit from Sand 0.6 (0.2) 0.6 (0.2) 0.6 (0.2)
avoiding the emissions associated with producing incumbent acetone Other Raw Materials 3.9 (1) 4 (1) 1.4 (0.4)
and MEK from fossil resources. There are other coproduct accounting Waste Disposal 3.2 (0.8) 3.3 (0.9) 3.3 (0.9)
Purchased Electricity 0 (0) 0 (0) 0 (0)
methods that could be used in this analysis; some of those other options Fixed Costs 57.7 (15.2) 63.6 (16.8) 56.4 (14.9)
are discussed in further detail by Cai et. al. (Section 2.1 in reference Refinery Co- 22.6 (6) 0 (0) 22.4 (5.9)
[11]). hydrotreating Cost
Chemical Coproduct − 54.7 (-14.4) − 54.7 (-14.4) 0 (0)
Credit
3. Results and discussion Electricity Coproduct − 27.4 (-7.2) − 8.5 (-2.3) − 35.4 (-9.3)
Credit
Process economics and GHG results, calculated using the methods Capital Depreciation 58.2 (15.4) 66.2 (17.5) 56.5 (14.9)
discussed above, are presented in this section. Average Income Tax 12.4 (3.3) 13.9 (3.7) 12.2 (3.2)
Average Return on 89.2 (23.6) 100.9 (26.7) 86.7 (22.9)
Investment
Total MFSP 283.3 (74.9) 313 (82.7) 320.9 (84.8)
3.1. Process economics

Table 1 shows the Total Purchased Equipment Cost (TPEC) and Total
Installed Cost (TIC) by areas of operation. Note that the hydroprocessing
capital costs are eliminated in the two cases with refinery co-
hydrotreating (Case A and Case C); those cases also require a smaller
hydrogen plant, consistent with the lower hydrogen requirement at the
biorefinery. Hydrogen and other operating costs for co-hydrotreating at
the petroleum refinery are shown later. Also note that coproduct
recovery and purification was eliminated in Case C; the costs under
“Pyrolysis vapor quench, condensation, and coproduct recovery” are
thus lower than the other cases. The steam system costs are lower in Case
B with less electricity production because a larger proportion of the off
gases are used for hydrogen production.
Various factors shown in Table 2 were applied to the TIC to derive

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A. Dutta et al. Chemical Engineering Journal 451 (2023) 138485

Table 6 towards the MFSP are shown in Table 5. Note that we present results in
Refinery co-hydrotreating operating cost estimates. liters gasoline equivalent (LGE) for non-US readers.
Cost Item Case A Case C Table 6 shows a breakdown of the refinery co-hydrotreating line item
listed in Table 5.
cents/GGE (cents/ cents/GGE (cents/
LGE) LGE) Fig. 3 provides a snapshot comparison of the three cases. Contribu­
tions towards the MFSP by operational areas, and expenditure categories
Fuel Natural Gas 16.2 (4.3) 16 (4.2)
Power Use 4 (1) 3.9 (1)
(shown in the legend) are included. The significant impact of coproduct
Steam Credit − 0.1 (-0.02) − 0.1 (-0.02) credits (54.7 cents/GGE or 14.4 cents/LGE) on Case A and Case B are
BFW to Steam 0.0002 (0.00004) 0.0002 (0.00004) shown. Differences in standalone vs co-hydroprocessing costs need to be
Cooling Water Circulation 0.005 (0.001) 0.004 (0.001) interpreted using a combination of the differences in the hydro­
Catalyst 1.6 (0.4) 1.6 (0.4)
processing area and the hydrogen plant. Higher steam and power
Royalties 0.9 (0.2) 0.9 (0.2)
Total Refinery Coprocessing 22.6 (6) 22.4 (5.9) (electricity) credit in Case C is because no coproducts are recovered, and
Cost those compounds are used with the off gases as energy sources.

3.2. Lifecycle analysis results

Table 7
Energy sources and consumption (MJ/dry metric ton) for the production and The modeled woody biomass feedstock for this process is a 50:50 mix
preprocessing of woody biomass feedstock constituents.
(by weight) of clean pine and logging residue. Mixed and diversified feed
Clean Pine (50 %) Logging Residue (50 %) constituents offer greater flexibility and can help improve overall
Silviculture 168 availability, reduce costs, and offer sustainability benefits. Collection,
Diesel 100 % transportation, and various preprocessing steps are necessary to make
Harvest and collection 163 the feedstock compatible for use in the CFP conversion process [14].
Diesel 100 %
Modeled energy sources and consumption for the production and pre­
Landing preprocessing 28 216
Diesel 100 % 100 % processing this woody feedstock blend is shown in Table 7.
Receiving and handling 0 13 Key process inputs, reflecting consumption, and outputs (products),
Electricity 100 % 100 % are shown in Table 8. Except for the fuel products (gasoline and diesel)
Storage 12 10 that are shown in units of energy per mass of biomass, the remaining
Diesel 100 % 100 %
Preprocessing 1,468 1,385
metrics are shown per MJ of the fuel products.
Natural gas 72 % 77 % As discussed previously, the impact of coproducts was accounted
Electricity 28 % 23 % using the displacement method; coproducts included chemicals (acetone
and MEK) in Cases A and B, and surplus electricity in all three cases
(Fig. 3 and Table 8). The modeled lifecycle GHG emissions shown in
total direct costs (includes TIC, land, warehouse, site development and
Fig. 4 are for the renewable hydrocarbon fuel blendstocks, after ac­
additional piping). Additional factors were applied to the total direct
counting for coproducts. Aside from conversion steps (including co-
costs to estimate indirect costs. The direct and indirect costs were added
hydrotreating and coproducts in relevant cases, and remaining bio­
to get the fixed capital investment (FCI). Working capital was added to
refinery conversion operations), all other steps within the LCA system
the FCI to get the total capital investment (TCI).
boundary (Fig. 2) remained constant across the three modeled cases. The
Fixed operating costs include salaries and benefits, maintenance,
modeled GHG emissions in g CO2e/MJ for categories that remained
insurance, and taxes; costs are listed in Table 3.
constant in Fig. 4 were Silviculture etc. (5.1), Fieldside Preprocessing
Product summaries for the three cases are shown in Table 4. Note
etc. (4.1), Depot Preprocessing (17.4), and Fuel Transportation (0.8).
that the GGE basis was 116,090 Btu/gallon (32.36 MJ/liter) using a
Petroleum refinery co-hydrotreating emissions, relevant for Cases A and
lower heating value (LHV) basis [22]. There were some model changes
C, was ~ 29 g CO2e/MJ; this value is relatively large primarily due to the
in Case C because of alterations to the condensation system since light
use of natural gas, with additional contributions from using grid elec­
coproducts are not recovered in this case.
tricity. Chemical coproducts, acetone and MEK, relevant for Cases A and
After capital and operating costs were calculated, the total LHV of
B, accounted for a credit of 19.1 g CO2e/MJ, because they displace
the produced liquid hydrocarbon fuels in GGE was used to calculate a
existing chemicals with higher GHG emissions associated with current
Minimum Fuel Selling Price (MFSP) in $/GGE; a discounted cash flow
production processes. Surplus electricity generated additional credits
rate of return (DCFROR) approach was used with the financial as­
based on the displacement of electricity from the US grid (with an
sumptions discussed in Section 2.3. Operating cost contributions
average GHG emission intensity of 440 g CO2e/kWh). The electricity

Fig. 3. Comparison of cost contributions by operational areas.

7
A. Dutta et al. Chemical Engineering Journal 451 (2023) 138485

Table 8 sources in the biorefinery conceptual design.

Key process inputs and outputs. Overall lifecycle fuel GHG emissions were about 21.5, 3.9, and 35.0 g
Case A Case B Case C Unit CO2e/MJ for Cases A, B, and C, respectively; they translate to GHG
emission reductions of 77 %, 96 %, and 62 %, respectively, over pe­
Products
Gasoline Fuel 4186.8 4186.8 4303.1 MJ/dry troleum gasoline. In Case B, the avoidance of the GHG emissions asso­
metric ciated with the co-hydrotreating at a petroleum refinery (using natural
tonne gas for hydrogen production) significantly reduces the carbon intensity
Diesel Fuel 4186.8 4186.8 4070.5 MJ/dry compared to Case A. In Case C, the foregone coproduct displacement
metric
tonne
credit from light oxygenates, acetone and MEK, increases the lifecycle
Total Fuel 8257.3 8257.3 8373.6 MJ/dry fuel GHG emissions to 35.0 g CO2e/MJ, despite an increase in copro­
metric duced electricity by about 30 % over Case A (increased electricity from
tonne using the light oxygenates as an energy source).
Biomass to Fuel 45.1 % 45.1 % 45.3 %
(energy efficiency,
LHV basis) 4. Conclusion

The inclusion of coproducts can have beneficial impacts on biocon­

By-products
Excess Electricity − 0.13750 − 0.04291 − 0.17759 MJ/MJ version. From an environmental standpoint, displacing coproducts that
MEK − 0.00057 − 0.00057 0.00000 kg/MJ are currently produced from fossil sources and/or have high GHG
Acetone − 0.00353 − 0.00353 0.00000 kg/MJ emissions can improve the overall sustainability. The economics also
improve if the coproducts have a higher price on a mass basis compared
Petroleum Refinery Consumption for Co-Hydrotreating to the produced fuels; in addition, any oxygenated coproducts are
Fuel NG 0.3995 0.0000 0.3947 MJ/MJ beneficial because the associated mass of oxygen is also saleable and
Power Use 0.0155 0.0000 0.0154 MJ/MJ
deoxygenation/hydrogenation costs are avoided. Recovery and purifi­
Steam − 0.0097 0.0000 − 0.0093 MJ
natural cation challenges, and associated costs, are also important consider­
gas/MJ ations for coproducts because pyrolysis derived streams can contain
Cooling Water 0.0309 0.0000 0.0266 Liter/MJ many species. Gaseous coproducts at standalone biorefineries may also
Makeup be problematic because of high transportation costs.
Hydrotreating 0.0106 0.0000 0.0106 g/MJ
Catalyst
Refinery co-hydroprocessing of biocrudes using existing equipment
Hydrocracking 0.0027 0.0000 0.0025 g/MJ is economically attractive. However, there are many research questions
Catalyst that still need to be addressed before significant volumes of oxygenated
biocrudes can be included within mainstream refinery operations. Initial
Biorefinery Resource Consumption results presented in this article are promising, but methodical scientific
Sand makeup 0.10445 0.10445 0.10483 g/MJ research is necessary for successful adoption. It should be noted that our
Natural Gas 0.00320 0.00123 0.00176 MJ/MJ estimates for co-hydrotreating are based on preliminary experimental
Fixed-Bed VPU 0.00005 0.00005 0.00005 g/MJ
Catalyst
results extrapolated to a successful future implementation; cost and GHG
Hydrotreating 0.00000 0.01063 0.00000 g/MJ emission estimates will change with further understanding and with
Catalyst refinery coprocessing variations to achieve specific fuel qualities for
Hydrocracking 0.00000 0.00264 0.00000 g/MJ different end uses.
Catalyst
Natural gas used for hydrogen production is a substantial contributor
ZnO (reforming 0.00002 0.00001 0.00001 g/MJ
cleanup) towards GHG emissions during refinery co-hydroprocessing of biocrude.
HDS (reforming 0.00001 0.00000 0.00000 g/MJ Use of biogenic off gases from pyrolysis for hydrogen production can
cleanup) significantly reduce GHG emissions. In this regard, biogenic coproducts
Steam Reforming 0.00004 0.00001 0.00002 g/MJ can offer GHG benefits and that can help offset some of the impacts of
Catalyst
Shift Catalyst 0.00005 0.00002 0.00003 g/MJ
fossil-derived hydrogen used during co-hydroprocessing. Alternate and
PSA Adsorbent 0.00131 0.00050 0.00072 g/MJ emerging hydrogen production technologies may facilitate more sus­
Solvent 1 (coproduct 0.07260 0.07260 0.00000 g/MJ tainable co-hydroprocessing in the future. Location of the biorefinery
purification) near a petroleum refinery may also enable the use of hydrogen from
Solvent 2 (coproduct 0.00190 0.00190 0.00000 g/MJ
biorefinery off-gases for co-hydroprocessing, thus lowering GHG
purification)
50 wt% Caustic 0.09545 0.09535 0.09554 g/MJ emissions.
Net Water Makeup 0.03480 0.04844 0.03121 Liter/MJ The results of the work emphasize the need for continued novel
No. 2 diesel fuel 0.00199 0.00199 0.00198 MJ/MJ analysis and research on coproducts to enable low-cost and sustainable
biofuels, developing further understanding of refinery coprocessing, and
Combustor Feed Stream Heating reducing the carbon intensity of hydrogen production. In addition, it
Values highlights the importance of considering both economic and GHG
Char Combustor 0.36 0.36 0.36 MJ/MJ
reduction aspects into comprehensive comparative analysis to identify
Reformer Fuel 0.87 0.66 0.94 MJ/MJ
Combustor
our best options for biomass resource utilization.

Declaration of Competing Interest

credits were 16.8, 5.3, and 21.7 for Cases A, B, and C respectively; more
electricity was produced when off-gases were not used for hydrogen
production for standalone hydroprocessing (Cases A and C), and addi­
tional energy was available from light oxygenated molecules not
recovered as chemical coproducts in Case C. Emissions from the
remaining conversion steps at the biorefinery were ~ 1 g CO2e/MJ;
these emissions were low because most of the associated CO2 emissions
were from biogenic carbon, and there was very little use of fossil energy
The authors declare the following financial interests/personal re­
lationships which may be considered as potential competing interests:
Products or companies are named solely for descriptive clarity, and this
neither constitutes nor implies endorsement by NREL/ANL/PNNL/INL
or by the U.S. government.

8
A. Dutta et al.
Fig. 4. Contributions towards lifecycle GHG emissions.
Data availability
Sample models from previous related work have been published and
the link is provided as a reference in this article.
Acknowledgements
This work was authored in part by the National Renewable Energy
Laboratory, operated by Alliance for Sustainable Energy, LLC, for the U.
S. Department of Energy (DOE) under Contract No. DE-AC36-
08GO28308; Argonne National Laboratory, managed by UChicago
Argonne, LLC, under DOE Contract No. DE-AC02-06CH11357; Pacific
Northwest National Laboratory, managed and operated for DOE by
Battelle, under DOE Contract No. DE-AC06-76RLO-1830; and Idaho
National Laboratory, operated for DOE by Battelle Energy Alliance
under contract DE-AC07-05ID14517. Funding provided by U.S.
Department of Energy Office of Energy Efficiency and Renewable En­
ergy Bioenergy Technologies Office. The views expressed herein do not
necessarily represent the views of the DOE or the U.S. Government. The
U.S. Government retains and the publisher, by accepting the article for
publication, acknowledges that the U.S. Government retains a nonex­
clusive, paid-up, irrevocable, worldwide license to publish or reproduce
the published form of this work, or allow others to do so, for U.S. Gov­
ernment purposes.
Author contributions
AD: TEA & process modeling, initial draft, final editing; HC: LCA
work and initial version of related text; MST: TEA & refinery modeling,
review/edits; CM: CFP experimental lead; KI: NREL hydrotreating (HT)
lead, CFP experiments, review/edits; HW: PNNL HT lead, review/edits;
9
Chemical Engineering Journal 451 (2023) 138485
DMS: PNNL HT experiments; LO: LCA work; DSH: feedstock modeling;
ANW: coproducts recovery experiments; JAS: NREL thermo-catalytic
conversion lead & overall guidance; MBG: NREL CFP experimental
project lead, CFP catalyst development, review/edits.
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