Applied Energy 269 (2020) 115166

Contents lists available at ScienceDirect

Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

Fuel properties of hydrochar and pyrochar: Prediction and exploration with T

machine learning
⁎
Jie Lia, Lanjia Panb, Manu Suvarnaa, Yen Wah Tonga, Xiaonan Wanga,
a
Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore 117585, Singapore
b
Key Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China

H I GH L IG H T S G R A P H I C A L A B S T R A C T

• Datasets for hydrochar and pyrochar

were compiled by systematic litera-
ture review.
• Machine learning models with multi-
task prediction were developed and
optimized.
• Fuel properties of chars were pre-
dicted by optimal models with R of 2

~0.90.
• Feature impacts on targets were ex-
plored with model explainer based on
game theory.
• Performance of models was further
improved after feature re-examina-
tion.

A R T I C LE I N FO A B S T R A C T

Keywords: Conversion of wet organic wastes into renewable energy is a promising way to substitute fossil fuels and avoid
Biochar environmental deterioration. Hydrothermal carbonization and pyrolysis can convert wet organic wastes into
Waste to energy hydrochar and pyrochar, which are potential fossil fuel alternatives due to their comparable fuel properties.
Pyrolysis Machine learning (ML) has strong prediction ability after being trained with historic dataset and facilitates good
Hydrothermal carbonization
understanding of the impact of input features on output targets through a data-driven approach. In this study,
Machine learning
ML models for multi-task prediction of fuel properties of the chars were developed and optimized based on two
Multi-task prediction
datasets for hydrochar and pyrochar. Feature importance and correlation were explored based on optimized ML
model, and feature re-examination was conducted for model improvement. Results showed that support vector
regression model with optimal hyper-parameters exhibited better generalized performance for prediction of both
hydrochar and pyrochar properties with the best average R2 of 0.90 and 0.94. ML-based feature analysis in-
dicated that process temperature and carbon content in the feedstock were the significant features impacting fuel
properties of both chars, while nitrogen content was another important input feature for hydrochar and hy-
drogen content for pyrochar. The accuracy (especially for pyrochar), generalization ability, and computational
speed of models were further improved after feature re-examination. The intuitions obtained from feature
analysis provided meaningful insights to select input features for prediction performance improvement and
computational cost saving, and might guide experiments to produce chars with desired quality.

⁎
Corresponding author.
E-mail address: chewxia@nus.edu.sg (X. Wang).

https://doi.org/10.1016/j.apenergy.2020.115166
Received 31 January 2020; Received in revised form 15 April 2020; Accepted 6 May 2020
0306-2619/ © 2020 Elsevier Ltd. All rights reserved.
J. Li, et al.
1. Introduction
The depleting reserves of conventional energy sources, along with
their higher rate of consumption than generation have placed an in-
creased demand on the supply of non-conventional energy sources [1].
Various modes of renewable energy have been identified to substitute
fossil fuels, including solar, wind, geothermal, hydropower and bio-
mass. Among the above listed, biomass, specifically the ones derived
from the waste or residue of wood processing, agriculture and horti-
culture are the cheapest to be procured, as well as the most convenient
to be utilized. These kinds of biomass can be recycled and pelletized to
uniform shape and size for convenient storage, transportation, and
utilization [2,3]. Biomass derived from municipal solid wastes, such as
food waste, animal manure, sewage sludge etc., are potential but in-
tractable sources due to their high organic contents and inherent water
retention ability [4,5]. Additionally, the large amounts of high-moisture
organic wastes are considered as carriers of heavy metals, pathogens,
antibiotics, cacosmia, micropollutants, and CO2 emission, thereby
raising serious environmental concerns [6–8]. In such scenario, tech-
nologies that aim to recover energy and resource from these wet wastes
provide a solution to avoid environmental deterioration and reduce the
consumption of fossil fuels.
In the last decade, thermal treatment processes such as hydro-
thermal carbonization (HTC) and pyrolysis have gained significant in-
terest in the research community as potential technologies to recover
resource and energy from wet wastes, as well as eliminate the organic
containments, e.g. antibiotics, pathogens [9,10]. The high pressure and
temperature attained during the hydrothermal process, cause the spe-
cial structures of wet wastes to break down thoroughly, and the sub-
sequent dewatering process effectively releases the bonded water. For
example, the special structures of sludge, e.g. supra colloid with cells
and extracellular polymeric substances (EPS), can be disintegrated to
release the bonded water under HTC process [11]. It has been proved
by various researchers that hydrothermal conversion is one of the most
promising ways to enhance the dewaterability of sludge and pre-treat
other wet wastes, due to its high resource recovery potential, high de-
watering efficiency, low cost and easy operation [11,12]. Furthermore,
hydrochar, the solid phase obtained from HTC, is an energy-rich pro-
duct with high content of carbonaceous material. The hydrochar with
high calorific values has great potential to be used as a solid fuel to
substitute for fossil fuels. More importantly, in the case of HTC, around
60% of N in the feedstock is transferred to liquid product due to the
decomposition of N compounds, which benefits the hydrochar compo-
sition and results in lower NOx emission during hydrochar combustion,
as compared to the raw biomass wastes [12,13]. Alternately, pyrolysis
is another prevalent technology to convert wet biowaste into energy
and resource. Multiple valuable products including pyrochar, bio-oil
and biogas are produced during the pyrolysis process [14], and the
production of these, depend on the operational conditions. For ex-
ample, pyrochar with outstanding physicochemical characteristics can
be produced via slow pyrolysis (300–600 °C with a heating rate of
1–30 °C/min) [7]. As fuel sources, both pyrochar and hydrochar with
rich carbon content exhibit similar performance to that of coal [15,16],
and possess high energy densification due to the high degree of ar-
omatization [17]. However, not all pyrochar and hydrochar from wet
wastes have potential to compete against conventional energy sources,
primarily due to the wide range of their caloric values and energy
densification [7]. Therefore, it is essential to evaluate their fuel prop-
erties, such as caloric values and energy densification to determine their
potential as feasible energy sources.
Conventional methodology to gauge the fuel properties of hydro-
char and pyrochar from wet wastes would be to conduct HTC and
pyrolysis experiments, and thereafter assess the respective fuel char-
acteristics. However, this route is labor-intensive, time-consuming, and
expensive [18]. Substantial publications of lab and pilot-scale work on
HTC and pyrolysis in the recent years, have provided a significant
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Applied Energy 269 (2020) 115166
amount of data about these processes, and helped researchers to en-
hance their understanding on the existing process and unravel new
insights. In an era of data-centric analytics, machine learning (ML)
serves as a data-driven approach, which can learn exclusively from the
data without relying on rule-based programs [19,20]. In ML models, the
relevance between input features and output targets are achieved over a
training dataset. This relevance can be further generalized to make a
prediction of new data samples with the same set of input features [21].
For the ML application on waste to biochar, several works have been
published. Linear regression and random forest models were employed
to predict the solid yield and the energy recovery of HTC from organic
wastes with R2 below 0.80 and over 0.90, respectively [22,23]. Two ML
models with high accuracy was developed for biochar yield prediction
from pyrolysis of cattle manure [18]. However, the ML models lacked
generalization ability, as it was developed on a small dataset with only
33 experimental datapoints, obtained in specific lab-scale pyrolysis
process. Couple of other studies proposed the development of two ML
algorithms, i.e. adaptive neuro-fuzzy inference system and social-spider
optimization to predict the biochar yield from the same dataset as
above [24,25]. Although its prediction performance was enhanced, the
generalization of these models was once again limited, given the small
size of dataset. Besides, the input features of the above three studies
with small datasets only focused on the operational conditions, and did
not include any details on feedstock characteristics which are vital to
the char properties. Moreover, in our earlier work, we devised ML
models to predict the yield and carbon content of biochar derived from
dry organic wastes and biomass with improved performance by con-
sidering both feedstock properties and process conditions [20]. How-
ever, it was found that the training and optimization of the ML models,
exclusively for predicting each target was a time-consuming and com-
putationally expensive process, which was also the universal limitation
in all previous ML studies which primarily developed single-task pre-
diction models.
Motivated by these abovementioned limitations, in this study, we
aimed to develop ML models to simultaneously predict four different
fuel properties of hydrochar and pyrochar from high-moisture wastes,
including yield, higher heating value, energy recovery efficiency, and
energy densification. Compared to most other studies on ML applica-
tions for biochar, a key novelty of this study was the development of
simultaneous multi-task prediction models with good prediction per-
formance, based on two medium-size datasets containing a compre-
hensive list of input features. These multi-task ML models tended to be
highly efficient, as they required less time and computational costs,
compared to single-task prediction [26]. To achieve this goal, an ex-
tensive list of publications related hydrochar and pyrochar prepared
from HTC and pyrolysis of sludge, food waste and manure were re-
viewed and two separate datasets were compiled for hydrochar and
pyrochar, respectively. The input features containing elementary com-
ponents (C, H, N, O), proximate analysis information (fixed carbon, ash
and volatile matter contents) of feedstock, and operational conditions
of HTC (temperature, residue time, and water content in reactor) and
pyrolysis (temperature, heating rate and residue time) were taken into
consideration to develop ML models for the prediction of multiple
targets (yield, HHV, ER, and ED). Lastly, the feature re-examination was
explored to further improve the ML models based on the feature im-
portance of input features and their correlations with these targets
achieving from ML explainer combining with game theory. Given the
impetus garnered by data-driven analytics in recent years, the strategies
and ML models developed in this study can help understand the desired
properties of chars to better estimate their application and guide ex-
periments based on the model inference.
J. Li, et al.
2. Methodology
2.1. Data collection and pre-processing
During the data collection process, a systematic review of literature
on HTC and pyrolysis processing using sewage sludge, food waste and
manure as the feed sources was conducted. Published papers on the
abovementioned topic were thoroughly searched through databases
(e.g. ScienceDirect, ISI Web of Sciences, Google Scholar and
Engineering Village) with keywords such as food waste, sludge,
manure, hydrothermal carbonization, pyrolysis and hydrochar etc. A
total of 64 peer-reviewed papers were finally identified, without any
constraint on the publication date, and from these papers, data was
extracted and compiled. The original datasets are provided in supple-
mentary material.
The following strategies and assumptions were incorporated during
the data collection and pre-processing:
(1) A total of 248 data points on hydrochar and 165 data points on
pyrochar were gathered from 38 and 26 published papers with a
total of 24 kinds of sewage sludge, 41 kinds of food waste, and 33
kinds of manure.
(2) All the data were impartially accepted, without any authors’ bias
and were meticulously screened to avoid duplicate entries.
(3) The input set of features included feedstock properties determined
by proximate analysis including fixed carbon (Fc), ash (A), volatile
matter (V) and element composition (C, H, N, O). All data of these
properties were dry-based values.
(4) Parameters including hydrothermal reaction time (Ht), temperature
(HT), water content (WC), pyrolysis temperature (PT), pyrolysis
heating rate (PHR), and reaction time at the desire temperature (Pt)
comprised of the process related input features.
(5) Hydrochar and pyrochar fuel characteristics including yield, higher
heating value (HHV), energy recovery efficiency (ER) and energy
densification (ED) were labelled as output targets. The details for
their calculations are shown in supplementary material.
(6) The data points were systematically collected from the tables or
extracted from the figures in the shortlisted literatures.
(7) In order to achieve a uniform range among the variables, all the
data of input features and output targets were normalized using Eq.
(1):
xi − μ
x i∗ =
s (1)
where x i is the value of input feature i; x i∗ is the normalized value of
initial x i ; μ is the mean of x i ; and s is the standard deviation of x i .
Lastly, the total data points were divided into two parts. Ninety
percent of the total data points were randomly selected and labelled as
training data, and the remaining data points were labelled as test data
for the final evaluation of the developed models. During the training
process, the ten-fold cross-validation method was applied to tune the
hyper-parameters of different models for the improvement of their
prediction capability [27].
2.2. Modelling methods and hyper-parameter tuning
In this work, two state-of-the-art machine learning algorithms,
namely supporting vector machine (SVM) and random forest (RF), were
used to predict the fuel characteristics of hydrochar and pyrochar. SVM
and RF have been widely used in energy domain for prediction of an-
nual electricity consumption [27], global incident solar radiation [28],
and battery capacity [29] etc.
A variant of SVM popularly known as support vector regression
(SVR) was used in this study (Fig. 1a), which suits applications in the
case of linear and nonlinear regression problems [28]. SVM makes use
of an adaptive, margin-based loss function called the kernel function,
3
Applied Energy 269 (2020) 115166
which is the algorithm’s underlying principle. The types of kernel
functions used in SVM models include linear, sigmoid, polynomial
(poly), radial basis function (rbf) and exponential radial basis function
(erbf). This function transforms the input data points (which could be
linear or non-linear in nature), from its original n-dimension space to a
higher dimensional feature space [28]. This takes into effect by placing
a linear hyper plane between two types of sample data points, such that
the hyper plane maximizes the margin of data separation.
RF is a form of ensemble learning method, which works on the
principle of building and combining a multitude of decision trees to
improve its generalization and prediction capabilities [29]. A decision
tree is non-parametric in nature and consists of two types of nodes,
namely the decision nodes and leaf nodes. The decision node evaluates
each sample data point on the basis of a test function and passes it on to
other branches of the tree depending on its features. During the
learning process, as the volume of data fed to the decision tree in-
creases, the multitude of trees increases - generating hundreds or even
thousands of decision trees [29,30]. The underlying principle in
random forest is the combination of all the decision trees developed
during learning process, through a process called bagging or bootstrap
aggregation (Fig. 1b). Each of the individual tree acts as a regressor,
and the final prediction of the random forest model is derived as the
mean of the outputs of all the individual decision trees, with minimum
variance and improved generalization of prediction ability.
In this study, both the SVR and RF regression models were devel-
oped using the scikit-learn library in python programming language
(Python 3.6). The prediction accuracy of SVR is mainly related to the
epsilon (ε), kernel function, and regularization parameter (rp) [31]. The
function of the width of ε-insensitive zone, is controlled by epsilon,
while fitting the training data. Regularization parameter in the loss
function controls the trade-off to achieve low error during the training
and testing process. Therefore, the hyper-parameters including the
regularization parameter, epsilon, and kernel function were tuned to
optimize SVR model. The final performance of the RF was the average
prediction error of the trees [32]. For the hyper-parameter tuning of RF,
both of the number of trees and the maximum depth of each tree were
adjusted from 1 to 20 to achieve the optimized model.
2.3. Model training and evaluation of multi-task learning
Machine learning models are classically viewed as an optimization
problem, where the goal is to define a loss function (also known as cost
function), which is then minimized so that the model is optimized. The
loss function typically represents the deviation of the predicted values
(derived from the ML model) to that of the actual experimental values.
The loss function of multi-task learning (Ltotal ) as presented in this work
is given by Eq. (2) [33]:
m
Ltotal (W ) = ∑ λt Lt [h (xit ; wt ), yit ]
t=1 (2)
where m represents the total number of tasks. h is the hypothesis
function of machine learning model. W = [w1,w2 ...wm ] is a matrix made
of parameter vectors (wt ) of hypothesis function learned by minimizing
Ltotal . λt is a scalar coefficient for weighting the importance of loss for
different targets, which is set to be the same for each target in this work.
Lt means the loss function of ML models for task t. x it and yit represent
the values of input and output variables for task t, respectively. i in-
dicates the ith data point used in the training process.
The accuracy of model predictions for both SVR and RF were
evaluated in terms of coefficient of determination (R2) and root mean
square error (RMSE). Conceptually, the higher the R2 and lower the
RMSE, the greater is the model accuracy [18]. These were calculated as
described in Eqs. (3) and (4):
J. Li, et al.
Fig. 1. Illustration of (a) Support Vector Regression and (b) Random Forest models.
n t t 2
∑i = 1 (Y pred , i − Yexp, i )
Rt2 = 1 − n t t 2
∑i = 1 (Yexp , i − Yexp, ave )
n t t 2
∑i = 1 (Y pred , i − Yexp, i )
RMSEt =
n (4)
t t
where Y pred , i and Yexp, i are the predicted and the experimental values of
t
target t, respectively, while Yexp , ave is the average of all experimental
values of target t. n is the total number of data points and RMSEt re-
presents the root mean squared error of target t.
2.4. Evaluation of feature impacts on targets
Once the ML models are built and their prediction performance
evaluated, interpretation of the models, especially determining feature
importance is the next gradual step. This is often considered as a
challenging task, given the black-box nature of most ML models. Model
agnostic methods present a possible solution to explain these complex
ML models [34]. An extension of the Shapely values from game theory,
SHAP (SHapley Additive exPlanations) is a useful methodology to gain
insights on the outcome of machine learning predictions [34,35]. The
shapely value is a concept in cooperative game theory to distribute both
gains and costs to players/factors, in which two or more players/factors
are involved to achieve the payoff or outcome [36,37]. Therefore this
value represents the average marginal contributions of one player/
factor to the payoff of a strategy with all the combinations and per-
mutations considered [37].
Conventionally, feature importance in any ML model is determined
across the entire dataset. In contrast, the SHAP methodology allocates
each feature variable an importance value for every single prediction
data point, thereby offering local interpretability. The accumulated
SHAP values also determine how much each feature contributes, either
positively or negatively, to the target variable, thereby making them
globally interpretable. As reported in literature, calculating the exact
SHAP value is not a straightforward process [35]. However, by in-
tegrating the additive feature attribution method, the SHAP values can
be approximated. In this work, we have used the model-agnostic ap-
proximation method of Kernel SHAP, which employs a specific type of
weighted linear regression, called the Linear LIME (Local Interpretable
Model-agnostic Explanations) [38]. Thus, Kernel SHAP is a unified
approach which uses Shapely values in conjunction with the Linear
Applied Energy 269 (2020) 115166
LIME to compute feature importance that can meaningfully interpret
the outcome of a given machine learning model [34,38].
(3)
3. Results and discussion
3.1. Analysis of input features and output fuel characteristics of chars from
wet wastes
A descriptive analysis of input features and output targets, derived
from the compiled datasets is presented in Fig. 2. The data analysis of
feedstock composition including proximate analysis and element com-
position is shown in Fig. 2a. The medians of organic components of C
(carbon) and V (volatile) in dry-based wastes were 42.39% and 73.18%,
respectively, which indicated that alternative fuel with rich C might be
produced from these types of high-moisture waste. In the case of HTC,
HT, Ht, and WC were considered in the operation process, and the
medians of these operational parameters were 220 °C and 60 min and
87.5% respectively (Fig. 2b). Compared to HTC, the median of Pt in
pyrolysis was the same as Ht, while the PT was 500 °C which was much
higher than HT (Fig. 2c). Another important operational parameter
considered in pyrolysis was PHR due to its significant impact on pro-
ducts. The reason for the omitting of WC in pyrolysis was that only a
few literatures reported the impact of WC on pyrochar, as most of wet
waste feedstocks was dried prior to introduction in the pyrolysis re-
actor.
During the statistical analysis and inference of the hydrochar and
pyrochar properties, derived from HTC and pyrolysis of wet organic
waste, it was observed that these chars exhibited good fuel properties,
including a similar atomic ratio to coal, high calorific value and good
energy densification. Fig. 2d-f depicts the fuel characteristics of the char
derived from HTC and pyrolysis of wet wastes. The scatter plot of ER as
a function of yield, along with the violin plots of operational conditions
(i.e. temperature and time) as insets, is shown in Fig. 2d. It is quite
evident from the scatter plot that the ER for the hydrochar data points
exhibited a positive linear correlation with yield, while the pyrochar
data points were slightly scattered. This could be attributed to the wide
range of operational temperature of pyrochar preparation. Further-
more, both the yield and ER of hydrochar were higher than that of
pyrochar, thereby indicating that the HTC process could recover more
char and retain most of its energy (more than 60%) as compared to
pyrolysis. A possible explanation to this phenomenon could arise from
4
J. Li, et al.
Fig. 2. Statistical data visualization of (a) feedstock composition, (b) operational condition of hydrothermal carbonization, (c) operational condition of pyrolysis, and
fuel characteristics including (d) ER vs. Yield, (e) Van Krevelen diagram, and (f) ED vs. HHV of char from wet wastes (A: Ash; Fc: Fixed carbon; V: Volatile matter; Ht:
Hydrothermal reaction time; HT: Hydrothermal temperature; WC: Water content; PT: Pyrolysis temperature; PHR: Pyrolysis heating rate; Pt: Pyrolysis reaction time;
ER: Energy recovery efficiency; Yield: Mass percentages of hydrochar or pyrochar obtained from wet wastes; ED: energy densification; HHV: Higher heating values).
the fact, that the operational temperatures in the HTC process
(~200 °C) were much lower as compared to the pyrolysis process
(~500 °C). It is well reported in literature that higher pyrolysis tem-
perature leads to a greater decomposition of organic components [39],
and increases energy transfer to the biogas and bio-oil constituents –
which are the co-products of pyrolysis process in addition to pyrochar.
The O/C and H/C atomic ratios of organic wastes, hydrochar, and
pyrochar are important parameters to help assess their fuel properties
for energy application [40]. Literatures stated that chars with low O/C
and H/C atomic ratios possessed high content of aromatic compounds,
stable carbon configuration, and good fuel properties owing to the high
degree of carbonization [39,41]. The O/C and H/C can be visualized in
a Van Krevelen diagram to indicate the chemical reactions during dif-
ferent thermal treatments, including decarboxylation, dehydration, and
demethanation, whose vectors are shown in Fig. 2e. According to the
directions of the above three types of reaction, the decarboxylation
reaction was the dominant reactions during the HTC process, while
both dehydration and demethanation were the main reactions in pyr-
olysis. From the Van Krevelen plot, it can also be inferred that the
atomic ratios of most hydrochar were close to that of peat and lignite,
while most of the pyrochar showed similar atomic ratios with coal and
anthracite due to its lower H/C and O/C ratios. These results are in
concordance with the earlier findings reported by Zhou et al. [39].
Fig. 2f represents the scatter plot of HHV versus ED, with a nearly
positive linear relationship. Most of the hydrochar and pyrochar had
HHV and ED values greater than 10 MJ/kg and 1.0, respectively. This
confirmed that the energy in wet wastes was condensed by both the
HTC and pyrolysis process. On comparing both the chars, the pyrochar
had a steeper slope for ED as a function of HHV, suggesting a faster
increasing of ED with the increasing of HHV as compared to hydrochar.
3.2. Model development and hyper-parameter tuning
To this aim, two ML models (RF and SVR) were developed and their
hyper-parameters were tuned based on the ten-fold cross-validated-
average RMSE to predict of hydrochar and pyrochar properties, based
on the dataset described in Section 2.1. Fig. 3 represents the contour
5
Applied Energy 269 (2020) 115166
plots for the hyper-parameter tuning of the ML models. The transition
in the color of the contour plot from red to blue indicates model con-
vergence during the hyper-parameter tuning processes. While tuning
the hyper-parameters of the RF model for the hydrochar dataset, the
number of trees = 14 and maximum depth = 8 were identified as
optimized parameters, to obtain a lower RMSE of 0.16. A further in-
crease in both the number of trees and its maximum depth did not
lower the RMSE significantly. Similar trends were observed in the case
of the RF model developed for the pyrochar dataset. where the number
of trees = 10 and maximum depth = 10 were identified as optimized
parameters to obtain a minimum RMSE of 0.071.
In the case of SVR model, three hyper-parameters, namely, kernel
function, regularization parameter and epsilon were tuned for optimi-
zation. For the hydrochar dataset, in the case of linear kernel function,
the RMSE values decreased until epsilon = 0.5, and then increased with
the increase of epsilon, but showed no significant decrease in RMSE
values when the regularization parameter was increased. However, in
the case of poly and radial basis function (rbf) as kernel functions, the
RMSE values reduced significantly, with a decrease in the epsilon value
along with simultaneous increase in regularization parameter value.
The minimum average RMSE were 0.31, 0.25 and 0.17 for linear, poly
and rbf under tuned regularization parameter and epsilon, respectively.
The above results indicated that rbf function with the regularization
parameter of 50 and epsilon of 0.1 exhibited the best prediction per-
formance of hydrochar properties. For the pyrochar prediction model,
the average RMSE values showed a similar trend as described in the
above-mentioned hydrochar model, during the hyper-parameter tuning
process (Fig. 3b). The final minimum average RMSE of 0.062 was ob-
tained under the optimal condition of rbf function with the regular-
ization parameter and epsilon to be 10 and 0.1, respectively.
3.3. Model evaluation
Once the ML models were developed and optimized as described in
Section 3.2, they were evaluated for the robustness of their multi-task
prediction capability on the test dataset. The original experimental data
versus the predicted values of the hydrochar and pyrochar are
J. Li, et al. Applied Energy 269 (2020) 115166

Fig. 3. Hyper-parameter optimization of machine learning models for energy properties prediction of (a) hydrochar and (b) pyrochar (RF: Random forest; SVR:
Support vector regression).

Fig. 4. Multi-task predicted data versus the original experimental data of (a) hydrochar and (b) pyrochar based on the optimized machine learning models with
training and testing datasets (RF: Random forest; SVR: Support vector regression).

Fig. 5. Plots of predicted data versus original experimental data for each target of (a) hydrochar and (b) pyrochar with histograms of datasets at the top and right of
each sub-figure (Yield: Mass percentage of hydrochar or pyrochar obtained from wet wastes; ER: Energy recovery efficiency; HHV: Higher heating values; ED: Energy
densification; RF: Random forest; SVR: Support vector regression).

presented in the form of scatter plots in Fig. 4. Specifically, Fig. 4a
represents a comparative evaluation between the RF and SVR models to
predict the fuel characteristics of the hydrochar. It is evident from the
plot that, both the training and test data points predicted by the SVR
model were denser than RF. Also, the average R2 for the four targets
(based on training and testing datasets) derived from the SVR model
were found to be 0.96 and 0.91, both of which were greater as
compared to the average R2 (0.94 and 0.79) of the RF prediction. This
result suggested a better and more robust multi-task prediction per-
formance of SVR due to its higher prediction accuracy of both the
training and test datasets. Furthermore, the details about the prediction
performance for each fuel characteristic of hydrochar and pyrochar
with the histograms of datasets at the top and right of each sub-figure
are shown in Fig. 5. The average R2 of the SVR model for yield, HHV,

6
J. Li, et al.
ER, and ED of hydrochar in the test dataset were 0.88, 0.96, 0.92, and
0.89, respectively (Fig. 5a).
For the pyrochar dataset (Fig. 4b), both the RF and SVR models had
the same average R2 (0.97) and similar RMSE for the training dataset.
However, the average R2 of RF and SVR model were found to be 0.75
and 0.88, respectively, in the test dataset. The above result indicated
that SVR facilitated a better prediction performance than RF. Further-
more, according to the plot of predicted vs. actual data for each target
in Fig. 5b, the prediction of SVR for the yield, HHV, ER, and ED of
pyrochar in the test dataset had R2 of 0.88, 0.95, 0.79, and 0.91, re-
spectively. It was intrinsic that the prediction performance of ML
models was lower in test dataset as compared to the training dataset.
However, the predicted performance of optimized SVR models was
sufficient and comparable to exhibit a good generalization of fuel
properties prediction for both hydrochar and pyrochar. In this study, it
was evident that the SVR model outperformed the RF model in both the
cases of hydrochar and pyrochar prediction studies.
3.4. Impacts of input features on the fuel characteristics of the char
In order to determine the impacts of the input variables, including
the elementary and proximate analysis data of the wet wastes and the
operational conditions of HTC and pyrolysis, on the fuel characteristics
of hydrochar and pyrochar, the ML model explanation was investigated
using a game theory approach namely SHAP. This analysis was only
conducted for the SVR model which had outperformed the RF model in
this study. The impacts of each input feature on the respective output
target of hydrochar and pyrochar are illustrated in Fig. 6a and b. The
Fig. 6. Impacts of input features on each individual characteristic and overall characteristics of hydrochar (a and c) and pyrochar (b and d) based on the explanation
of SVR model using SHAP values.
7
Applied Energy 269 (2020) 115166
contribution of every input data point on the targets was quantified as
SHAP value. A positive SHAP value indicates that the input feature
contributes positively to the predicted value. A point of red color re-
presents a higher original value of the input feature, while blue for
lower value. If the color of the data points belonging to an input feature
turns from blue to red with the increase of SHAP value, it is inferred
that the input feature has a positive impact on the output target. Fur-
thermore, Fig. 6c and d depict the stacks of mean absolute SHAP values
of each input for the four characteristics of hydrochar and pyrochar. A
higher sum of mean absolute SHAP values for the four outputs indicates
a greater impact during the multi-task prediction process.
As depicted in Fig. 6a, the impacts of inputs on various targets were
different. For the yield prediction, N content, temperature of HTC (HT)
and C contents were identified as the three most significant variables,
where both N content of the wet wastes and HT had a negative impact
on the yield of the hydrochar. The C content showed no obvious
monotonicity with yield, and either a low or high C content could be
associated with high yield. As for the HHV prediction, the HT, C and H
contents were the top three impactful inputs features, and each of them
had a positive impact on the HHV of hydrochar. In the case of ER
prediction, N, C and water contents emerged as the three most im-
portant input features, where the N content was negatively correlated
to ER, while both C and WC contents exhibited a non-monotonicity.
Lastly, for ED prediction, the top three positive features were HT, O and
Fc contents. Furthermore, the HT, N and C contents were determined as
top three important features for the overall impact on the four targets
investigated in the hydrochar dataset (Fig. 6c). It was reasonable that
HT and C content were identified as significant features because HT
J. Li, et al.
Table 1
The comparison of prediction performance of fuel properties belonging to hydrochar and biochar ML models developed on the basis of all features and selected
features.
Test performance Hydrochar
R2 RMSE
All features Updated feature All features Updated feature
Yield (%) 0.88 0.86 7.83 8.49
HHV (MJ/kg) 0.96 0.95 1.39 1.43
ER (%) 0.92 0.90 6.22 6.86
ED 0.89 0.89 0.09 0.09
Average 0.91 0.90 3.89 4.22
affected the degree of thermal degradation of wastes, and C was the
main source of energy [42,43]. However, another interesting finding in
this study was that the N content was also one of the critical factors for
the energy properties of hydrochar, especially for the prediction of yield
and ER. In general, the importance of elementary compositions ac-
counted for 48% of the four features together (Fig. 6c), indicating that
this feature category was the foremost to fuel properties of hydrochar.
Compared to hydrochar, the impact of input features on fuel prop-
erties of pyrochar showed subtle yet comparable differences. In detail,
temperature (PT), heating rate (PHR) of pyrolysis, and C content of
waste were identified as the three most significant variables impacting
the yield prediction of pyrochar and were negatively correlated as seen
in Fig. 6b. Heating rate was a rare and distinct feature impacting pyr-
olysis yield, which was not investigated in the case of HTC. From a
process perspective, this can be well understood from the fact that HTC
operates in lower temperature regimes (~200 °C), whereas the different
types of pyrolysis (fast or slow) with a higher temperature (~500 °C)
are heavily dependent on its heating rate [44]. It is well cited in lit-
erature that a lower heating rate i.e. slow pyrolysis, yields char as the
main product, whereas fast pyrolysis yields more of bio-oil [44]. Thus,
it is proved that the findings in this work are in good agreement with
the ones published in literature. For HHV of the pyrochar, the tem-
perature and C content were the two important positively correlated
features, following a similar trend to that of HTC. However, the ash
content was standout among the top three features for pyrochar in
terms of HHV, in contrast to the H content for HTC. This may be at-
tributed to the fact that the H content in pyrochar is lower than that in
hydrochar due to a higher degree of dehydration and demethanation in
pyrolysis [45], while most of the ash remains intact in the pyrochar,
and this in turn could negatively impact the HHV of the pyrochar [46].
In terms of ER in pyrolysis, the top three important features were PT, H,
and O contents, all of which were markedly different compared to the
important features in HTC. The PT and H content had negative influ-
ence on the ER, whereas the O content was positively correlated. In the
case of ED prediction of pyrochar, the top three features identified were
O, H and ash contents. The O content was negatively correlated with
ED, whereas the other two had a positive influence. The differences in
the impact of input features on targets variables of the chars from HTC
and pyrolysis might be attributed to their difference in the degree of
thermal decomposition of feedstocks, mainly due to the gap of their
operational temperatures. In summary, the PT, C and H contents were
determined as the three most important input parameters impacting the
four target variables investigated under the pyrochar dataset, and ele-
mentary composition was again identified as the most important fea-
ture category to determine the fuel properties of pyrochar, accounting
for 46% of importance (Fig. 6d).
3.5. Feature re-examination for model improvement
The ML models developed for fuel properties prediction of hydro-
char and pyrochar, as described in Sections 3.2 and 3.3, included three
8
Applied Energy 269 (2020) 115166
Pyrochar
R2 RMSE
All features Updated feature All features Updated feature
0.88 0.97 5.86 3.36
0.95 0.96 1.37 1.38
0.79 0.92 9.40 6.84
0.88 0.93 0.09 0.10
0.88 0.94 4.18 2.92
categories of input features namely elementary, proximate and opera-
tional conditions with a total of ten input features. Actually, it was
reported that not all the input variables in a ML framework contribute
to the model building process [47]. A similar observation was identified
in this study, during the SHAP value analysis as seen Fig. 6. Some
features might be redundant to add to the computational cost of ML
models, without having a significant impact on the prediction perfor-
mance. In the case of hydrochar, it was found that the Ht was the least
important feature in the determination its four fuel properties, which is
evidently seen in Fig. 6a and 6c. Therefore, it was removed from the
model to improve the model generalization ability and reduce the
computational cost. Similarly, the three features including Pt, V, and N
content in the pyrolysis process were discarded due to their negligible
significance in the model prediction, as determined by SHAP values
(Fig. 6d). For the purpose of this study, the process of removing re-
dundant variables based on the inference of SHAP was termed as
“feature re-examination”. Post feature the re-examination, the SVR
models were re-devised with the same hyper-parameters as described in
Section 3.2, but only included the updated input features.
The comparison of prediction performance of the ML models based
on initial set of features and post feature re-examination in the test
dataset is presented in Table 1. The results showed that the average R2
of the ML model post feature re-examination for fuel properties pre-
diction of hydrochar decreased marginally from 0.91 to 0.90 with the
slight reduction of R2 specifically for yield, HHV, and ER prediction.
Although its prediction accuracy marginally reduced after feature re-
examination, the generalization ability and computation process could
be improved. In the pyrolysis process, the performance of fuel proper-
ties prediction for pyrochar, significantly increased from an average R2
of 0.88 to 0.94 with a much smaller average RMSE value. In detail, the
R2 of yield, ER, and ED increased from 0.88, 0.79, and 0.88 to 0.97,
0.92, and 0.93, respectively. The above results suggested that the fea-
ture re-examination based on SHAP values provided useful insights on
the selection of the input features, and thereby aided the improvement
of prediction performance, model generalization ability, and compu-
tational process. The inference drawn from the feature re-examination
process can also aid towards an informed data collection process, from a
futuristic perspective.
4. Conclusions
Two types of machine learning models with multi-task prediction
capability were developed and optimized based on two datasets, com-
prising of 248 kinds of hydrochar and 166 kinds of pyrochar, respec-
tively. Support vector regression model with optimal hyper-parameters
showed better prediction performance for both datasets as compared to
random forest model. The final average R2 of the support vector re-
gression model with feature re-examination were 0.90 and 0.94 for the
four target variables of the hydrochar and pyrochar, respectively.
Moreover, the impacts of input features on the properties of char were
explored based on the optimized model. Process temperature and C
J. Li, et al.
content of waste were two significant features that were ranked con-
sistently high for most of the fuel properties (target variables) for both
the chars. N and H contents in the feedstock were also found to have
significant impact the hydrochar and pyrochar, respectively. The pre-
diction accuracy (especially for pyrochar), generalization ability and
computational speed of models were further improved by discarding
redundant input variables based on the results of the ML-based feature
analysis. Lastly, limited datasets and lack of experimental validation of
the model predictions were the two limitations of the present work,
which will be investigated in our future studies.
CRediT authorship contribution statement
Jie Li: Conceptualization, Methodology, Formal analysis, Writing -
review & editing, Visualization, Data curation. Lanjia Pan: Formal
analysis, Data curation. Manu Suvarna: Methodology, Formal analysis,
Writing - review & editing. Yen Wah Tong: Writing - review & editing.
Xiaonan Wang: Conceptualization, Writing - review & editing,
Supervision.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgement
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,
Technology and Research under Grant No. A1898b0043 and the IAF-PP
grant “Cyber-physical production system (CPPS) towards contextual
and intelligent response” by the Agency for Science, Technology and
Research under Grant No. A19C1a0018.
Appendix A. Supplementary material
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.apenergy.2020.115166.
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