Journal of Cleaner Production 278 (2021) 123928

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Journal of Cleaner Production

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

Multi-task prediction and optimization of hydrochar properties from

high-moisture municipal solid waste: Application of machine learning
on waste-to-resource
Jie Li a, Xinzhe Zhu a, Yinan Li a, Yen Wah Tong a, Yong Sik Ok b, Xiaonan Wang a, *
a
Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, 117585, Singapore
b
Korea Biochar Research Center & Division of Environmental Science and Ecological Engineering, Korea University, Seoul, 02841, Republic of Korea

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

Article history: Hydrothermal carbonization (HTC) is a promising technology for valuable resources recovery from high-
Received 20 March 2020 moisture wastes without pre-drying, while optimization of operational conditions for desired products
Received in revised form preparation through experiments is always energy and time consuming. To accelerate the experiments in
20 August 2020
an efficient, sustainable, and economic way, machine learning (ML) tools were employed for bridging the
Accepted 23 August 2020
Available online 28 August 2020
inputs and outputs, which can realize the prediction of hydrochar properties, and development of ML-
based optimization for achieving desired hydrochar. The results showed that deep neural network
Handling editor: Prof. Jiri Jaromir Kleme
s (DNN) model was the best one for joint prediction of both fuel properties (FP) and carbon capture and
storage (CCS) stability of hydrochar with an average R2 and root mean squared error (RMSE) of 0.91 and
Keywords: 3.29. The average testing prediction errors for all the targets were below 20%, furtherly within 10% for
Waste-to-energy HHV, carbon content and H/C predictions. ML-based feature analysis unveiled that both elementary
Biochar composition and temperature were crucial to FP and CCS. Furthermore, a ML-based software interface
Hydrothermal carbonization was provided for practitioners and researchers to freely access. The insights and Pareto solution provided
Renewable energy
from ML-based multi-objective optimization benefitted desired hydrochar preparation for the potential
Carbon sequestration
application of fuel substitution or carbon sequestration in soil.
Multi-objective optimization
© 2020 Elsevier Ltd. All rights reserved.

1. Introduction (Girotto et al., 2015). These high-moisture MSW without proper

The ever rising in population, urbanization and living standards,
has generated large amounts of municipal solid waste (MSW) over
the past two decades, especially the high-moisture MSW, i.e.
sewage sludge, food waste, and animal manure, from the ever-
growing consumption and production of food and water. Approx-
imately 1.3 billion tons of MSW is generated globally every year,
from the food production and consumption procedures alone
Abbreviations: ML, Machine learning; DNN, Deep neural network; RF, Random
forest; SVM, Supporting vector machine; SVR, Supporting vector regression; PCC,
Pearson correlation coefficient; HTC, Hydrothermal carbonization; MSW, Municipal
solid waste; HHV, Higher heating value; C_char, carbon content in hydrochar; CR,
Carbon recovery; ER, Energy recovery; A, Ash content in feedstock; V, volatile
matter content in feedstock; t, Reaction time of HTC; T, Reaction temperature; WC,
Water content; FP, Fuel properties; CCS, Carbon capture and stability in hydrochar;
MOO, Multi-objective optimization.
* Corresponding author.
E-mail addresses: jllj@u.nus.edu (J. Li), chewxia@nus.edu.sg (X. Wang).
disposal will lead to several environmental problems, such as the
spread of antibiotic resistance genes (Xu et al., 2020), pathogen,
heavy metals, odor and CO2 emission (Yang et al., 2020). In recent
years, the concept of waste-to-resource conversion, specifically
pertaining to high-moisture wastes has gained extensive interest
owing to its benefit in terms of environmental protection, resource
recovery, and circular economy (Xue et al., 2019). However, the high
moisture (around 60e80 wt% water) and complex components of
sewage sludge, food waste and animal manure make them more
difficult to dispose, as compared to other biomass wastes, such as
horticultural and agricultural waste. Besides, substantial amounts
of energy, resources and labor are incurred in the pre-treatment
process, before they can be recycled and utilized.
Hydrothermal carbonization (HTC), a thermal conversion pro-
cess, is a promising technology to convert high-moisture MSW into
valuable product, i.e. hydrochar, without the requirement of pre-
drying of feedstock, thus aiding the economics of the operation,
also being energy efficient and comparable to other thermochem-
ical conversion processes. Hydrochar with high higher heating

https://doi.org/10.1016/j.jclepro.2020.123928
0959-6526/© 2020 Elsevier Ltd. All rights reserved.
2 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928
value (HHV) and carbon content (C_char) could be as alternative of
fossil fuels (Wang et al., 2016). Additionally, hydrochar with stable
carbon content could be used as a fertilizer, conditioner or reme-
diation agent for soil improvement and carbon sequestration (Ok
and Tsang, 2019). However, the production of hydrochar with
desired properties is a tedious and high-cost process as it involves
numerous iterations of experimental efforts to find optimal oper-
ating conditions for different types of high-moisture wastes. The
routine experimental strategy is the classical one-factor-at-a-time
(OFAT) optimization approach which is quite labor-intensive,
time-consuming and involves running numerous experimental
trials followed by subsequent hydrochar characterization (Cao
et al., 2016). Therefore, development of computational models for
predicting the properties and maximizing the desire properties of
hydrochar with corresponding experimental conditions provided is
indeed helpful for supplementing or expediting experiments in an
economic and efficient way.
Machine learning (ML), a key sub-group of artificial intelligence,
is a data-driven approach used to predict target variables of inter-
est; which in turn is dependent of numerous input variables by
developing mapping function based on historical data. With the
advances in data and computing technologies, ML has been applied
in waste-to-resource domains. Tao et al. (2020) employed ML
model for fast characterization of waste and biomass based on
infrared spectroscopy with 120 data samples for aiding upstream
sorting. A neural network (NN) model was developed by Ismail
et al. (2019) to predict the carbon and phosphorous recovery
from HTC of poultry litter with reaction time and temperature as
inputs. They achieved a R2 > 0.90 in prediction model with 21
experimental data points. Jiang et al. (2019) employed three ML
models for prediction of adsorption performance of activated car-
bon co-activated by HTC and pyrolysis with 30 datapoints and
found that random forest model was the best suited for their study
with a R2 > 0.99. Our previous work also applied ML models to
predict energy related properties (J. Li et al., 2020), yield, carbon
content (Zhu et al., 2019a), and the heavy metals adsorption ability
of chars (Zhu et al., 2019b). It is worth a mention that, while all the
above ML studies were unique in their own way, their small data-
sets might lead to a lack of generalization ability for the developed
ML models. This is also the universal shortcoming in most ML
works in this domain. Moreover, the aforementioned ML models
only considered the operational parameters or mono type of
feedstock as input features to predict the char properties. Addi-
tionally, most of above works are limited to predicting a single
target and thus require the development of multiple models to
predict various properties of interest. This further adds to the time,
effort, and computational cost associated with repetitive modelling
activities. Besides, the ML work on waste conversion only focused
on model development and prediction, without substantial atten-
tions on practical applications of these models. Therefore, the
prediction results from ML models are insufficient to make signif-
icant contributions to experimentalists and practitioners.
Motivated by the above-mentioned limitations of published
works, in this study, we developed a multi-task ML model to predict
various hydrochar properties simultaneously based a medium-size
dataset containing various types of features. To promote the prac-
tical implication and application of the ML model accessible to
scientists and practitioners in this field, a software user interface
embedded ML model was developed for free access. Moreover, ML-
based multi-objective optimization (MOO) was proposed to maxi-
mize the desired properties of hydrochar with corresponding
experimental conditions provided to accelerate the experiments. In
detail, eight characteristics including yield, energy recovery (ER),
carbon recovery (CR), HHV, carbon content (C_char), and atomic
ratios (H/C, O/C and N/C) were identified as the multi-task learning
targets. The fuel properties (FP, including HHV and ER) and carbon
capture (C_char and CR) and carbon stability (represented by
atomic ratios) were considered owing to its significance for deter-
mining the application of hydrochar. Three ML algorithms were
employed and optimized to obtain an accurate model for the multi-
task prediction of hydrochar characteristics. The impacts of prop-
erties of feedstock, operational parameters of HTC on the hydrochar
characteristics was explored base on optimal ML model. Further-
more, a ML-based software for multi-prediction of hydrochar
properties was developed, and the ML model was successfully in-
tegrated with MOO model for maximizing the FP and CCS stability
of hydrochar based on different applications.
2. Methodology
2.1. Data collection and pre-processing
Literatures review on HTC of sewage sludge, food waste, and
manure was first conducted to compile the dataset. The keywords,
including food waste, sludge, manure with the combination of
hydrothermal carbonization or hydrochar, were used for literature
retrieval in Web of Sciences, Scopus, Google Scholar since 2010. The
data related to feedstock properties, i.e. element composition (C, H,
N, O), fix carbon (Fc), ash (A), volatile matter (V), and the HTC
conditions, including reaction time (t), temperature (T), and water
content (WC), were extracted from the tables and figures in the
published literatures. The data pertaining to the characteristics of
hydrochar including yield, HHV, C_char, CR, ER, N/C, H/C, and O/C,
were accordingly gathered and calculated. A dataset with 248 data
points from 38 published papers was compiled finally. The details
about the dataset are provided in the supplementary materials
(Tables S4 and S5).
To obtain a uniform range among the variables, the input fea-
tures and output targets were normalized using Eq.(1):
xi  m
x*i ¼ (1)
s
wherexi is the value of input feature i; x*i is the normalized value of
initial xi ; m is the mean value of xi , and s represents its standard
deviation.
The Pearson correlation coefficient (PCC) was employed as a
measure of vector similarity to understand the preliminary corre-
lation between the input and output variables (Zhu et al., 2019b).
The correlation coefficient value, rxy , was calculated according to
equation (2):
Pn Pn
ðx  xÞ ðy  yÞ
rxy ¼ qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
P
i¼1 i ffi qi¼1
P
i
ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
ffi (2)
n
i¼1 ðxi  xÞ2 n
i¼1 ðyi  yÞ2
where rxy is the value of PCC for a feature to target or target to
target; x and y are the mean of input feature x and output target y.
The range of rxy is from 1 to 1, where 0 means no linear corre-
lation, and a negative or positive value means negative or positive
correlation, respectively.
Additionally, during the model building process, the total data
points were divided into two random parts (Fig. S1a). Nine-tenth of
the total data points, i.e. 223 randomly selected data points, were
labelled as training data, while the remainder one-tenth (25 data
points) were labelled as test data for the final evaluation of the
developed model. In the training process, the 10-fold cross vali-
dation was applied to tune the hyper-parameter of the different
models to improve the prediction capability (Payam et al., 2009).
 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928
2.2. Modelling methods and hyper-parameter tuning
In this work, three state-of-the-art ML tools, including random
forest (RF), supporting vector machine (SVM), and deep neural
network (DNN) were developed to predict the characteristics of
hydrochar (Figs. S1bed). In ML models, the relevance between
input features and output targets can be achieved from a training
dataset. This relevance can be further generalized to make a pre-
diction from other new input features (Wu et al., 2013). The SVM
algorithm can handle both regression and classification problems
with the help of statistical learning theory (Shataee et al., 2012).
The hyper-parameters including the penalty parameter, epsilon,
and kernel function were tuned to develop the supporting vector
regression (SVR) model in this work. RF, based on decision trees, is
another effective ML method to explore the nonlinear correlation
between the inputs and outputs (Breiman, 2001). The number of
trees and maximum depth of each tree in RF were adjusted from 1
to 100 and 1 to 20, respectively. DNN is a neural network with two
or more hidden layers, one input layer and one output layer (Hinton
et al., 2012). The main hyper-parameters, including the number of
hidden layers, neurons in each layer, the learning rate of RMSprop,
and the dropout rate, were tuned to obtain the optimized DNN
model. The detailed introduction and hyper-parameters tuning
strategies for the three ML models are presented in Table S1-S3.
2.3. Model training and evaluation of multi-task learning
ML problems are mostly formulated as a minimization of loss
function on a training set of data. Loss function indicates the
discrepancy between the values predicted by the ML model and the
actual experimental values. The loss function of multi-task (Ltotal )
adopted in this study is as specified (BenTaieb and Hamarneh,
2017):
X
m    
Ltotal ðWÞ ¼ lt Lt h xti ; wt ; yti
t¼1
where m represents the number of tasks; h is the hypothesis
function of machine learning model; W ¼ [w1 ,w2 : : :wm ] is a ma-
trix made of parameter vectors (wt ) of hypothesis function learned
by minimizing Ltotal ; lt is a scalar coefficient for weighting the
importance of loss for different targets, which is equal for every
target in this work. Lt means the loss function of ML models for task
t; xti and yti represent the values of input and output variables for
task t; i is the ith data point used in the training process.
The goodness of fit for the RF, SVR, and DNN models were
evaluated with determination coefficient (R2), as well as root mean
squared error (RMSE) (Zhu et al., 2019b). Besides, the percentage
error (% error) and mean absolute percentage error (MAPE, %) were
employed to analyze the distribution of the prediction accuracy,
which helps to evaluate model performance (Severson et al., 2019).
These were calculated according to Eqs.(4)e(7):
Pn  t t
2
i¼1 Ypred;i  Yexp;i
R2t ¼ 1   2
Pn
i¼1
t
Yexp;i  Yexp;ave
t
vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
uP  2
u n
t i¼1 Y tpred;i  Y texp;i
RMSEt ¼
n
3
t
Ypred;i t
 Yexp;i
%error ¼ t
 100 (6)
Yexp;i
100 X
n Yt t
 Yexp;i
MAPE ¼
pred;i
(7)
n i¼1 t
Yexp;i
t
where Ypred;i t
indicates the predicted value of target t; Yexp;i means
t
the experimental value of target t; n is the data amount. Yexp;ave is
the average of all experimental values of target t.RMSEt represents
the root mean squared error of target t.
2.4. Method of feature importance analysis
ML models continue to show strong performances in the pre-
diction abilities, while interpretation of these very same models is a
challenging task. Fortunately, permutation importance analysis can
help to understand the contributions of input features in the pre-
diction models effectively, for any “black-box” estimator (Islam
et al., 2019). The algorithm of permutation importance is similar
to that of the random forest (Breiman, 2001). It replaces the input
feature with random noise (shuffling a feature column) each time,
and then re-trains the estimator to see what the relative change of
the score (accuracy, R2, etc.) is when one feature is shuffled. The
higher positive value of permutation importance indicates that the
feature has higher importance. The value of feature importance
close to zero means that the feature under consideration is less
likely to impact the model prediction, thereby having a lower
relevance. A negative value of feature importance means better
prediction performance can be obtained with shuffled (or noisy)
data.
2.5. Method of optimization for hydrochar properties
Fuel alternative and carbon sequestration in soil are two main
(3) applications of hydrochar. HHV and ER are two important proper-
ties for evaluating the potential of hydrochar as a fuel alternative.
Moreover, hydrochar can also be used in soils for carbon seques-
tration. Herein, properties of carbon including C_char, CR, and
atomic ratios are crucial to estimate the carbon capture and storage
stability of hydrochar in soils. Therefore, it is meaningful to opti-
mize the feedstock compositions and operational conditions of HTC
to achieve the hydrochar with desired properties based on the
application requirement. To obtain hydrochar with high HHV and
ER, or the one with high C_char, CR, and cabon stability, multi-
objective optimization was conducted using the weighted sum
method based on the developed ML model. The optimization tool,
based on trust region methods (Conn et al., 2000), in SciPy package
was used via python to combine with ML model for multi-objective
optimization of different targets (Fig. 1).
For maximizing fuel properties (FP) of hydrochar, both HHV and
ER were considered, and they were treated equally in the multi-
objective optimization:
max FP ¼ m1 HHV þ m2 ER (8)
(4)
For maximizing of carbon capture and storage (CCS) stability of
hydrochar, the C_char content and CR were employed to evaluate
the carbon capture potential of hydrochar. The atomic ratios, i.e. H/
C, O/C, and N/C, were thus identified to represent the carbon stor-
age stability in hydrochar, and lower atomic ratios represented
(5) higher carbon stability. In other words, the carbon storage stability
was positively correlative to the minus atomic ratios (Liu et al.,
2020), therefore the negative sign was set before atomic ratios to
4 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928

of data statistics related to the elementary analysis, food waste

contained the highest contents of carbon, hydrogen and oxygen
and the lowest nitrogen, while the elementary contents in sludge
exhibited an opposite tendency (Fig. 2aeb). For the proximate
analysis, the median of water contents in sludge and food waste
were closed to each other and close to 90%, while it was about 70%
in manure. Furthermore, the volatile and fixed carbon contents in
food waste was the highest with an ash content of 5% which was
significantly lower than that in sludge (30%) and manure (18%). The
highest ash content in sewage sludge was mainly rooted in the
original source of the wastewater and its treatment process (Li
et al., 2017). For the HTC conditions, the most common tempera-
ture was 200e250  C, and the time was between 60 and 90 min.
As for the output targets, the median of hydrochar yield from
sewage sludge was the highest (65%), leading to a lowest carbon
Fig. 1. Strategy of integration of machine learning model with multi-objective opti-
content and HHV (Ma et al., 2019). However, the median of carbon
mization for hydrochar properties. and energy recovery from the three wastes to hydrochar were quite
close. Besides, three kinds of chemical reactions (dehydration,
decarboxylation, and demethylation) probably happened in the
maximize the CCS. HTC process of high-moisture wastes, which could be inferred from
the plot of O/C vs. H/C. Hence, the Van Krevelen diagrams of the
max CCS ¼ m3 ðCchar þ CRÞ  m4 ðH = C þ O = C þ N = CÞ (9) three kinds of hydrochar with the chemical reactions vectors was
In the ML model, ten input variables, including C, H, N, O, Fc, A, V, shown in Fig. 3def. All the three chemical reactions were founded
t, T and WC, had to be optimized to maximize the EP and CCS, and in the HTC of sludge, while the dehydration was the prominent
the constrain as below: reaction in the HTC of food waste and manure. The possible reason
was that the main component of the food waste and manure was
C þ H þ N þ O þ A ¼ 100% (10) lignocellulosic biomass whose dominating reaction in HTC is
dehydration (Toufiq Reza et al., 2018).
A þ V þ Fc ¼ 100% (11)

3.2. Variables correlation and hyper-parameter tuning of ML

LB of various types of wastes  C; H; N; O; Fc; A; V
 UB of various types of wastes
LB of operational conditions  t; T; WC
 of operational conditions
where m1, m2, m3, and m4 are the weighting factors of different ob-
jectives which are treated equally in the optimization of FP and CCS
(all m set as 0.5). The LB and UB of various types of wastes, and
operational condition are achieved from the boxplot analysis of
collected dataset, with their values depicted in Table 1.
3. Results and discussion
3.1. Statistical analysis of feedstock and hydrochar characteristics
Fig. 2 shows the descriptive statistics of data about the proper-
ties of sewage sludge, food waste and manure. Based on the median
models
A preliminary correlation between the input features and
output targets was investigated based on the Pearson correlation
coefficient (PCC). According to the PCC matrix of features to targets
(Fig. 4), both the HHV and C_char of hydrochar were positively
correlated with the C, H and V contents of the feedstock, while they
had strong negative correlations to the ash content. In addition, the
N/C ratio of hydrochar was markedly positively relative to N con-
tent of feedstock and negatively concerned with the O content.
However, the relationship between the input features and other
targets including yield, ER, CR, H/C, and O/C did not show signifi-
cant linear correlation with the input features. On the other hand,
most of the targets had significant correlation amongst each other.
The HHV and C_char had a strong positive relevance between each
other, as well as the yield, ER, and CR. Furthermore, the yield was
positively correlated to the ER and CR, and negatively related to the
HHV and C_char. The atomic ratios also had a certain correlation to
each other, and the H/C and O/C were negatively correlated to HHV

Table 1
LB and UB of variables for various types of wastes, and operational conditions achieved from the boxplot analysis of collected dataset.

Items Sewage sludge Food waste Manure

LB UB LB UB LB UB

Elementary compositions C (%) 21.86 51.20 39.00 61.94 34.26 46.40

H (%) 3.22 6.44 3.02 8.01 4.83 6.30
N (%) 1.32 9.58 0.21 11.47 3.20 4.39
O (%) 16.05 29.06 10.97 47.49 30.97 41.22
Proximate compositions V (%) 46.67 84.59 72.55 88.60 39.40 81.51
Fc (%) 0.00 10.23 0.73 25.51 1.09 29.30
A (%) 15.41 49.85 0.80 20.40 5.10 17.40
Operational conditions t (min) 5.00 240.00 5.00 240.00 5.00 240.00
T (oC) 140.00 330.00 140.00 330.00 140.00 330.00
WC (%) 75.00 96.20 75.00 96.20 75.00 96.20
 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928 5

Fig. 2. Violin plot of data statistics about (a and b) elementary and (c and d) proximate analysis of the three high-moisture wastes, and (e and f) hydrothermal carbonization
conditions (Note: The data about those wastes were collected from the published literatures, and 16 kinds of sewage sludge, 21 kinds of food waste, and 11 kinds of manure were
gathered in this work; the data of these properties is dry-based values; O ¼ 100-C-H-N-Ash).

Fig. 3. Violin plot of data statistics about (a) yield, (b) carbon content and carbon recovery, (c) higher heat value and energy recovery, and (d, e, and f) Van Krevelen diagram of
hydrochar from these high-moisture wastes. (Note: A total of 248 data with 78 kinds of sewage sludge hydrochar, 108 kinds of food waste hydrochar, and 62 kinds of manure
hydrochar prepared from different high-moisture wastes were collected from the published literatures, and all the data on waste and hydrochar are presented in Tables S4 and S5).

and C_char. To summarize, most of the targets had correlations to
each other, thereby indicating the feasibility to adopt multi-task ML
predictions (Ben-David and Schuller, 2003).
To establish a ML model with high prediction performance of
hydrochar properties, multi-task learning models from three ML
algorithms as described in Section 2.2 were developed and their
hyper-parameters were tuned based on the 10-fold cross-validated
RMSE values (Fig. 5). In the case of RF, the mean 10-fold cross-
validated RMSE values decreased significantly with the increase
of the maximum depth of the trees from 1 to 10, and then plateaued
when the maximum depth was above 10. The RMSE values also
declined when the trees number rose from 1 to 10, and then
6 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928

Fig. 4. Correlation matrix of features and targets obtained through Pearson correlation coefficient method (248 pieces of data were used to investigated the Pearson correlation
coefficient of features to targets and targets to targets; A: ash content; Fc: fixed carbon content; V: volatile matter content; t: reaction time; T: temperature; WC: water content; ER:
energy recovery; CR: carbon recovery; HHV: higher heat value; C_char: carbon content in hydrochar).

Fig. 5. Hyper-parameter tuning of (a) RF, (b) SVR, and (c and d) DNN (RF: Random forest; SVR: Support vector regression; DNN: Deep neural network).

plateaued under the condition of the maximum depth >2. There-
fore, 10 trees with a maximum depth of 10 were adopted as the
optimized hyper-parameters of RF. For the SVR model, the radial
basis function (rbf) possessed the best performance due to its
lowest 10-fold cross-validated RMSE values as compared to the
linear and poly functions. The RMSE values decreased first and then
increased with the increasing value of the penalty parameter, while
they changed minimally with the elevation of epsilon values.
Therefore, the SVR model with rbf, 0.1, and 10, as the kernel func-
tion, epsilon value, and penalty parameter value, respectively, were
set as the final parameters of the optimized model. For DNN, the
RMSE dropped initially, and then rose with the increasing number
of neurons and learning rate. The plausible reason was that too
many neurons in DNN could lead to overfitting on training data
(Saxe and Berlin, 2016). Another result was that the RMSE value
decreased slightly with the number of hidden layers 2, and the
smallest RMSE was obtained when the dropout rate was 0.1. Hence,
the optimized hyper-parameters of DNN were 2 hidden layers
equipped with 128 neurons in each with 0.001 as learning rate and
0.1 as dropout rate. The results of the tuned hyper-parameters for
all the three models are presented in Table S6.
3.3. Validation of the optimized ML models with test data
A comparative evaluation among the three optimal models was
performed with the remainder one-tenth test data to evaluate their
prediction accuracy for the multi-task prediction of hydrochar
characteristics. Moreover, single-task learning with the same
hyper-parameters of each model was devised and compared with
multi-task learning. Both R2 and RMSE were determined as the
assessment criteria for the prediction accuracy of models. The value
of R2 closer to 1.0 or the smaller RMSE value means a better accu-
racy of prediction. As shown in Table S7 and Fig. 6, the multi-task R2
of RF was higher compared to that of the single-task for the pre-
diction of C_char, ER, CR, and H/C, while the single-task R2 for other
targets prediction was much higher (Table S7). However, the RF
models exhibited unsatisfied performance (Fig. 6a). Although the
performance of single-task prediction for RF could be improved
 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928
Fig. 6. Prediction performance of (a) average R2 and (b) average RMSE for the eight targets in the three different optimized models (RF: Random forest; SVR: Support vector
regression; DNN: Deep neural network).
after tuning the hyper-parameters for each task one by one, this
process was time-consuming and computationally expensive. For
the optimized SVR model, all the R2 of multi-task were above 0.85
(Table S7), and its average R2 was 0.90 which was significantly
higher than that of single-task prediction. For the optimal DNN
model, the average R2 of single and multi-task prediction of the
optimized DNN model were 0.87 and 0.91, and the multi-task
prediction performance was slightly better than SVR. Also, both
the SVR and DNN models with multi-task prediction exhibited a
small mean RMSE (Fig. 6b). By comparing the three optimal models,
the DNN was the best owing to its highest R2 and lowest RMSE
value. Similar result was obtained by Date and Kikuchi who
investigated the metabolomics using various ML models (Date and
Kikuchi, 2018).
Furthermore, Fig. 7 depicts the predicted values of the opti-
mized DNN model for each task versus the original experimental
data in the form of scatter plots. The distributions of the percentage
error of the training and testing data to the predicted values are
shown as an inset with scatter plots. A tight and compact cloud of
points around the 45-degree line and a higher relative frequency of
percentage error near zero indicated a strong and reliable predic-
tion performance for the targets by the model. For the prediction of
training data, the R2 of all the targets were as high as 0.99.
Furthermore, almost all the percentage error values of training data
points for all the targets located at the range of 10%e10%, inferring
that the optimized DNN model had an excellent prediction per-
formance for the training dataset. However, the distribution of the
plotted points for the test data was more scattered and the ranges
of percentage errors were greater, as compared to that of the
training data. The R2 values for all targets were relatively smaller
and RMSE values higher compared to the training dataset. It indi-
cated that the prediction performance of the DNN model showed a
slight attenuation for the test dataset. However, its accuracy of
multi-prediction was competitive, as well as the size of dataset and
the consideration of various types of high-moisture wastes and
input features, as compared to some other related ML works on this
topic (Table 2).
In detail, for the yield prediction, although a few data points
were not concentrated on the 45-degree line (Fig. 7a), the R2 value
of yield prediction was 0.90. The points of HHV and C_char were
gathered tightly (Fig. 7bec), and their R2 values were as high as
0.95. As can be seen, most of the predicted HHV values of hydrochar
were more than 10 MJ/kg, suggesting that most hydrochar could be
used as fossil fuel substituent for heat or electricity generation
(Porteous, 2005). The R2 values for ER and CR prediction were 0.88
and 0.90 (Fig. 7dee), and the R2 for the H/C, O/C, and N/C pre-
dictions were 0.89, 0.91, and 0.89, respectively (Fig. 7feh). The
hydrochar with both O/C and H/C ratio below 0.2 and 0.4 could stay
7
much longer and be more beneficial for carbon sequestration in soil
(Brassard et al., 2018). Based on the mean absolute percentage error
(MAPE) for testing dataset (Fig. 7), the DNN model exhibited an
acceptable MAPE for the eight output targets (all less than 20%),
especially for the prediction of HHV, carbon content, and H/C ratio
of hydrochar, of which the MAPE were below 10%. ML models as
these, serve as important tool to determine various applications of
hydrochar and evaluate the valuable resource recovery from HTC of
wet MSW before taking actions based on above accurate prediction
values of hydrochar characteristics. To accentuate the application of
this work, towards a more practical implication, a software for the
hydrochar properties prediction was developed so that the
outcome of the models could be readily understood by relevant
experimental researchers (Fig. A1). One issue to be addressed is
that the robust prediction performance is still not good enough due
to the limited size of dataset, which is a universal limitation for
most of the ML works on this topic, as seen in Table 2. Furthermore,
the developed ML models were static models because of the dataset
attribute, and dynamic models can be developed if the related data
is readily available. Additionally, the C degradation in soils is rela-
tive to the microbial community and activity, and the physico-
chemical properties of soil, e.g. pH, cation exchange capacity and
porosity, which would be affected by physicochemical properties of
biochar (porous structure, functional groups, adsorption ability,
organic matter mobility and so on) (Ahmad et al., 2014). These
factors will be considered in future work to explore the half-life of
carbon in soil with ML method.
3.4. Analysis of feature importance based on DNN
Permutation importance method was employed to determine
the feature importance for each target from optimal DNN model, as
shown in Fig. 8. The temperature and N content played almost the
same important role in the yield, ER and CR prediction owing to
their close correlations with each other (Fig. 5). The temperature of
HTC is a significant factor, because it affected the degree of thermal
degradation of waste, which further influenced the yield, ER, and
CR of hydrochar (Danso-Boateng et al., 2015). However, as per this
study, the N content was another critical factor for the prediction of
yield, ER and CR of hydrochar. This result may provide useful in-
sights to experimentalists in this field, to produce a high yield of
hydrochar with high energy and carbon recovery. From the above
results, the yield, ER, and CR depended on both properties of
feedstock (especially elemental composition), as well as the oper-
ational HTC conditions.
In terms of the prediction of the other two relevant targets, i.e.
HHV and C_char (Fig. 5), HHV is generally correlated to the carbon
content of hydrochar (Liu et al., 2019), and the trend of feature
8 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928

Fig. 7. Multi-task predicted data versus the original experimental data based on the optimized DNN for (a) yield prediction, (b) energy recovery prediction, (c) carbon recovery
prediction, (d) higher heating value prediction, (e) carbon content in hydrochar prediction, (f) H/C atomic ratio prediction, (g) O/C atomic ratio prediction, and (h) N/C atomic ratio
prediction.

importance to the two targets were quite similar. The carbon,
hydrogen, and ash content of feedstock were the three most sig-
nificant features. The HHV of hydrochar was dominated by the
carbon and hydrogen content since almost all the heat was
generated by the oxidation of carbon and hydrogen (Yu et al., 2018).
For the C_char, the carbon content of waste was the most significant
feature, and ash was another crucial factor. The ash content of
feedstock might affect its decarboxylation and aromatization re-
action in the HTC process (Buss et al., 2019). In addition, the HTC
process conditions, e.g. T, t, and WC, had slight impacts on the HHV
and C_char (Fig. 8). Hence, the HHV and C_char were mainly
determined by the feedstock properties instead of operational
conditions of HTC.
As for the atomic ratio, temperature was identified as the most
 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928 9

Table 2
Comparison of machine learning works on waste to resource systems with published work.

Waste conversion Types of feedstock Dataset Machine learning Model Type of Testing R2 References
process size task

Waste sorting Biomass and organic wastes 120 SVM Single >85% for Tao et al.
classification (2020)
Pyrolysis Biomass 264 Multiple linear regression Single 0.28 Tang et al.
264 RF Single 0.92 (2020)
137 Multiple linear regression Single 0.35
137 RF Single 0.94
Pyrolysis Algal 91 Extreme gradient boosting Single 0.84 Pathy et al.
(2020)
Pyrolysis Biomass 538 RF Multi 0.45e0.87 Cheng et al.
(2020a)
Pyrolysis Biomass and organic wastes 245 RF Single 0.80e0.85 Zhu et al.
128 0.76e0.85 (2019a)
Pyrolysis Cattle manures 33 NN Single 0.80 Cao et al.
Least squares support vector machine Single 0.96 (2016)
Adaptive Neuro-Fuzzy Inference with Social-Spider Single 0.98 Ewees et al.
Optimization (2017)
Adaptive Neuro-Fuzzy Inference with Particle Single 0.98 Aziz et al.
Swarm Optimization (2017)
Pyrolysis Organic wastes 165 SVR Multi 0.92e0.97 (J. Li et al.,
RF Multi 0.75 2020)
HTC 248 SVR Multi 0.86e0.90
RF Multi 0.79
HTC Organic wastes 649 RF Single >0.90 (Li et al., 2020)
475 RF Single >0.90
HTC Organics 340 Multiple linear regression Single 0.63e0.79 Li et al. (2015)
Regression tree Single 0.63e0.88
HTC þ pyrolysis Straw 30 Linear Regression Single 0.098e0.99 Jiang et al.
SVR Single 0.98e0.99 (2019)
Random Forest Single 0.99
HTC Poultry litter 21 NN Multi >0.90 Ismail et al.
(2019)
HTC Organic wastes 248 RF Multi 0.8e0.95 Li et al. (2019)
Hydrothermal Microalgae, crops/forest residues, and 800 Multiple linear regression Multi 0.16e0.60 Cheng et al.
treatment Organic wastes - Regression tree Multi 0.29e0.75 (2020b)
- RF Multi 0.70e0.90
HTC Food waste, sludge, and manure 248 RF Multi 0.55e0.91 This work
SVR Multi 0.88e0.96
NN Multi 0.88e0.95

Fig. 8. Feature importance to the eight output targets of the optimized DNN prediction (A: ash content; Fc: fixed carbon content; V: volatile matter content; t: reaction time; T:
temperature; WC: water content; ER: energy recovery; CR: carbon recovery; HHV: higher heat value; C_char: carbon content in hydrochar).

important feature for the H/C and O/C prediction. The groups process might lead to a reduction of oxygen and hydrogen in
containing H and O tend to disintegrate from the original molecular hydrochar (Danso-Boateng et al., 2015). The C, H, and O content in
structure of the feedstock via dehydration and decarboxylation in the feedstock were other important features for H/C and O/C pre-
the HTC reaction with temperature rising (Liu et al., 2019). This diction. In addition, the N content was the most dominating feature
10 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928

for the prediction of N/C, which was far outweighed any other Table 3
features. Interestingly, the temperature had no obvious influence Pareto solutions of input variables and output targets based on the maximum fuel
properties (FP) and carbon capture and storage (CCS) stability.
on the N/C prediction. The reason for the result may be that most of
the N of feedstock was absorbed and remained in the hydrochar Items Pareto solution of maximum Pareto solution of maximum
(Toufiq Reza et al., 2018), and the C_char was not dominated by FP CCS

temperature as well. To sum up, the significant feature to predict H/ Sludge Food waste Manure Sludge Food waste Manure
C and O/C was temperature, and N content in the feedstock was the C (%) 51.20 61.94 46.40 51.20 61.94 46.40
most important for N/C prediction. H (%) 3.22 3.02 4.83 3.22 3.02 4.83
N (%) 9.58 11.47 3.20 5.27 8.11 3.20
O (%) 16.05 10.97 31.35 24.86 14.34 39.81
3.5. Post ML-based multi-objective optimization of hydrochar V (%) 69.82 72.55 73.21 76.98 75.42 81.51
properties Fc (%) 10.23 14.85 12.57 7.57 11.98 12.73
A (%) 19.95 12.60 14.21 15.45 12.60 5.76
t (min) 5.00 5.03 5.00 30.95 15.14 58.74
To achieve a desired hydrochar, the optimal DNN model, as a
T (oC) 221.00 286.71 204.51 298.58 328.15 329.99
bridge between input variables and output characteristics of WC (%) 75.00 75.00 75.02 87.78 96.15 75.06
hydrochar, was further employed to integrate with optimization Yield (%) 69.53 69.26 79.78 64.70 65.04 45.52
model for maximizing desired properties, and providing corre- HHV (MJ/kg) 28.09 35.90 20.66 26.79 34.12 24.91
ER (%) 103.89 111.28 94.21 95.56 106.50 70.56
sponding operational conditions for experiments. For the hydro-
C_char (%) 67.36 81.69 51.37 66.51 82.74 65.53
char as a fuel alternative, two of its essential fuel properties (FP), CR (%) 91.51 105.98 91.41 90.61 102.27 64.65
namely, HHV and ER, were maximized. The Pareto curves of HHV H/C 0.61 0.11 1.20 0.54 0.09 0.89
vs. ER of hydrochar from sludge, food waste and manure are O/C 0.00 0.00 0.39 0.02 0.00 0.16
depicted in Fig. 9a. It was observed that the maximum HHV and ER N/C 0.12 0.12 0.05 0.07 0.09 0.04

obtained from food waste were the highest, followed by sludge and
manure. It seemed deviant for the maximum ER over 100%, while it
was reasonable considering prediction errors of the ML model
caused by its lack of generalization ability. According to the Pareto
solution for the input variables (Table 3), the C and H content were
located on the upper boundary of the constrain, indicating that
higher contents of C and H in the feedstock would lead to better fuel
properties. This finding corroborated the earlier analysis of feature
importance, as presented in Section 3.4, where C and H were
identified as the two most important features for HHV (Fig. 8).
Besides, the Pareto solution for the N content and WC were also at
their boundaries because they were two most important factors for
ER (Fig. 8). Moreover, the T needed to trade off to get the best FP of
hydrochar from various high-moisture wastes, because T had a
positive effect on HHV while negative impact on ER.
For the application of hydrochar in soils for carbon sequestration
and soil remediation, its potential in terms of carbon capture and
storage (CCS) stability was considered. The C_char, CR, and atomic
ratios of the hydrochar were identified as objectives to indicate the
CCS stability for optimization. As depicted in Fig. 9b, the Pareto
curves exhibited the carbon capture vs. carbon storage stability of
hydrochar derived from different wastes based on multi-objective
optimization. The food waste served was the most promising
feedstock to prepare a hydrochar with high CCS performance, pri-
marily due to its highest C content and lowest H and O contents as
compared to sludge and manure (Fig. 8). In terms of operational
conditions, the t, T, and WC for CCS maximization were much
higher than these for the FP (Table 3). The chemical reactions,
including dehydration, decarboxylation, and demethylation were
enhanced in the HTC process with higher values of operation
conditions, especially the T due to its significance to both atomic
ratios and CR (Fig. 8). This enhancement was beneficial to the car-
bon stability owing to its promotion of aromatization of hydrochar.
In this study, based on the outcome of the ML-based optimization,
optimal formulation and its solutions were devised and identified
to maximize FP or CCS stability of hydrochar. The insights derived
from the optimized models, could aid in presenting experimental
guidance to produce hydrochar with desired properties; while it
should be admitted that the lack of experiments verification for the
Pareto solution from ML-based optimization is another limitation
for this work.
4. Conclusions
Multi-task prediction model and software with high accuracy of
hydrochar properties prediction were developed, and successfully
integrated with MOO model for optimizing the hydrochar proper-
ties. The optimal DNN model with 2 hidden layers (128 neurons on
each), learning rate of 0.001 and dropout rate of 0.1 exhibited the
highest accuracy for the multi-task prediction of the eight charac-
teristics of hydrochar. The average R2 and RMSE of the optimized
DNN model were 0.91 and 3.29, respectively, and the R2 for all the

Fig. 9. Pareto curves of (a) HHV vs. ER and (b) carbon capture vs. carbon storage stability of hydrochar derived from sludge, food waste and manure.
 J. Li et al. / Journal of Cleaner Production 278 (2021) 123928
eight targets were above 0.88, contributing to satisfactory testing
MAPE (<20%). According to the ML-based feature importance
analysis, both operational conditions and feedstock compositions
were important to the prediction of FP and CCS performance of
hydrochar, especially elementary compositions and temperature.
The Pareto solutions of input variables for maximizing FP or CCS of
hydrochar based on different application were achieved from the
ML-based MOO model. The model-based feature importance and
Pareto solutions can provide useful guidance for desired hydrochar
preparation with labor, time and cost saving. In future work, the
dataset integrating both hydrochar preparation and application
features will be compiled, and the experimental validation will be
conducted to improve the generalization ability of ML models.
CRediT authorship contribution statement
Jie Li: Conceptualization, Methodology, Data curation, Investi-
gation, Writing - original draft, Software, Visualization. Xinzhe
Zhu: Investigation, Formal analysis, Software, Writing - review &
editing. Yinan Li: Software, Writing - review & editing. Yen Wah
Tong: Resources, Writing - review & editing. Yong Sik Ok: Writing -
review & editing. Xiaonan Wang: Supervision, Project adminis-
tration, Funding acquisition, Resources, Validation, Writing - re-
view & editing.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgment
This work was supported by the National Research Foundation,
Prime Minister’s Office, Singapore under its Campus for Research
Excellence and Technological Enterprise (CREATE) program (Grant
Number R-706-000-103-281 and R-706-001-102-281). The authors
acknowledge the Singapore RIE2020 Advanced Manufacturing and
Engineering (AME) Programmatic grant “Accelerated Materials
Development for Manufacturing” by the Agency for Science, Tech-
nology and Research under Grant No. A1898b0043 and the IAF-PP
grant “Cyber-physical production system (CPPS) towards contex-
tual and intelligent response” by the Agency for Science, Technol-
ogy and Research under Grant No. A19C1a0018.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.jclepro.2020.123928.
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