Accepted Manuscript

Review

Symbiotic relationship between hydrothermal carbonization technology and

anaerobic digestion for food waste in China

Ying Zhou, Nils Engler, Michael Nelles

PII: S0960-8524(18)30464-4
DOI: https://doi.org/10.1016/j.biortech.2018.03.102
Reference: BITE 19741

To appear in: Bioresource Technology

Received Date: 29 January 2018

Revised Date: 19 March 2018
Accepted Date: 20 March 2018

Please cite this article as: Zhou, Y., Engler, N., Nelles, M., Symbiotic relationship between hydrothermal
carbonization technology and anaerobic digestion for food waste in China, Bioresource Technology (2018), doi:
https://doi.org/10.1016/j.biortech.2018.03.102

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Symbiotic relationship between hydrothermal carbonization technology and

anaerobic digestion for food waste in China

Ying Zhou a, Nils Engler a, Michael Nelles a,*

a
University of Rostock, Faculty of Agricultural and Environmental Sciences,

Department Waste Management, Justus-v.-Liebig-Weg 6, 18059 Rostock, Germany

ABSTRACT

Food waste (FW) is traditionally disposed through landfills and incineration in China.

Nowadays, there are some promising methods, such as anaerobic digestion (AD) or

feeding and composting, which are being applied in pilot cities. However, the inherent

characteristics of Chinese FW may be regarded as a double-edged sword in the practical

applications of these disposal methods. To overcome these challenges, two modes of the

hydrothermal carbonization (HTC) process were reviewed as innovative strategies in

this article. Meanwhile, the “symbiotic relationship” between Chinese FW and HTC

technologies was highlighted. To improve treatment efficiency of FW, we should not

only try different methods and develop existing technologies, but also pay more

attention to the utilization and “1+1>2” synergistic effect of their combinations, such as

the combination of HTC and AD as a co-treatment method for saving on the

construction cost and avoiding redistribution of social resources.

Keywords

Food waste; Hydrothermal carbonization; China; Anaerobic digestion

* Corresponding author.
E-mail address: michael.nelles@uni-rostock.de
Postal address: Justus-v.-Liebig-Weg 6, 18059 Rostock, Germany

1
Contents
1. Introduction ........................................................................................................................... 2
2. Challenges for disposing food waste in China ...................................................................... 6
2.1 Characteristics of food waste ......................................................................................... 6
2.2 High organics ................................................................................................................. 7
2.3 High moisture................................................................................................................. 9
2.4 High Salinity ................................................................................................................ 10
3. Opportunities for application of hydrothermal carbonization ............................................. 11
3.1 Mechanism ................................................................................................................... 11
3.2 Process parameters ....................................................................................................... 13
3.2.1 Reactant media ........................................................................................................... 13
3.2.2 Mass ratio ................................................................................................................... 15
3.2.3 Temperature ............................................................................................................... 16
3.2.4 Retention time ............................................................................................................ 17
3.3 Characteristics of feedstock ......................................................................................... 18
3.4 Role as “Main Force”................................................................................................... 19
3.4.1 Production and application ......................................................................................... 20
3.4.2 Effect of disposal process ........................................................................................... 22
3.5 Role as “Assistance” .................................................................................................... 24
4. Conclusions ......................................................................................................................... 26
References ................................................................................................................................... 27

1. Introduction

In China, the population and demand for high quality food is increasing, which is

resulting in the generation of a large amount of FW. FW is the main part of municipal

solid waste (MSW) and is also the obstacle that needs to be taken into account for

proper and ecologically acceptable disposal. Because of its special original ingredient

2
and different degrees of sorting, disposal of FW is a complicated and difficult problem

that needs to be solved in many countries, not only in the developing countries, but also

in the developed countries. The Chinese Statistical Year Book (SYB) (2017) reported

that about 200 million tons of MSW were produced in 2016, which is equivalent to

approximately 10% of the world. Among them, FW accounted for 40-60% of MSW in

China, with the proportion increasing even more to 65% in the summer and autumn (Y.

Wang et al., 2016). Due to Chinese cooking methods and eating habits, the particular

composition of FW varies based on spatial differences and regional characteristics (X.

Hu et al., 2012). Overall, the main properties of Chinese FW can be summarized as high

in moisture, salinity, and organics. In particular, the lipid content is much higher than in

other regions of the world (Bi et al., 2016; Chen et al., 2013). These properties of

Chinese FW as well as the high ratio of FW in Chinese MSW have not only increased

the difficulties in their disposal, but also impede the value increment and energy

recovery of MSW. Therefore, waste sorting collection systems still have not yet been

implemented and adopted nationwide until now, despite the numerous favorable policies

implemented by the Chinese government (Wang et al., 2017). In the past, no more than

20% of FW could be properly treated and reused. The majority of FW was then sent to

landfills and incineration plants, while a portion of the rest was even turned into swill

and illegally recycled cooking oil (Wei et al., 2014). Until now, although the main

approach to treating FW is still disposal in landfills and incineration, some new methods

have been applied in pilot cities due to the 12th Five-Year Plan of China. The AD

3
method has accounted for 74.3% of the applications in pilot cities (Wu, 2015; Yan et al.,

2017). Based on different core technologies for the disposal of food waste, four models

have currently been formed in China. The “Beijing Model” focuses on anaerobic

digestion whereas the “Shanghai Model” opts for dynamic aerobic digestion. The

“Xining Model” is mainly feeding based while the “Ningbo Model” pays more attention

to the production of bacterial proteins, feed additives, and industrial oils and fats (Zhang

et al., 2016). Beyond that, more and more researchers have focused on other methods

including microbial fuel cells (ElMekawy et al., 2015), bio-pesticides (Zhang et al.,

2013), ethanol and lactic acid production (Liu et al., 2013; Yan et al., 2012), and even

some thermal conversion technologies such as pyrolysis, gasification (Digman and Kim,

2008) and hydrothermal process (Lu et al., 2012), which might be an opportunity for

FW disposal.

Currently, thermal conversion technologies, such as combustion, gasification,

pyrolysis, and carbonization, are commonly applied to organic waste treatment for the

purpose of waste to energy conversion (Park et al., 2011). In contrast to these

technologies, which require pretreatment of the high moisture raw materials to make

them dry enough, HTC has no limit on the water content of feedstock (He et al., 2014).

HTC technology is the thermochemical process through which waste with low energy

density is transformed into the target products. In this field, some researchers have

focused on the property of hydro-char, which is the main solid product, while others

have targeted the production of some special chemicals, which might affect the

4
following treatments. Especially in the solid phase, hydro-char may not be the superior

energy carrier compared with bio-oil and syngas from liquefaction and gasification. But

more and more researchers are paying attention to synthetic carbonaceous materials

based on the innovative concept of “black in the black” (Funke and Ziegler, 2010; M.-M.

Titirici et al., 2007). Although the application of HTC technology can be traced back to

1913, it is really a “new participant” in the sewage sludge treatment and bio-waste

management fields. Recently, a large number of studies have been carried out on

bio-waste, such as agricultural residues or manure and food waste, rather than on pure

carbohydrate and its derivatives (e.g. monosaccharide, disaccharide, and polysaccharide)

(Liu et al., 2010; Liu and Zhang, 2011; Wu and Zhang, 2012).

In China, a huge amount of FW must undergo treatment. Although the reduction of

FW should be prioritized first, the harmless of waste also needs attention (Masullo,

2017). However, in response to the call for a “zero waste economy,” resource recovery

and energy recycling will be the key factors that need to be taken into account (Song et

al., 2015). Fig. 1 reveals the relationship between FW and HTC technology. Since there

are many problems that need to be solved with the implementation of modern

engineering, HTC technology combined with AD as the co-treatment method has

attracted much more attention. Meanwhile, FW should not only be treated as “waste”

but can be used as a “carbon source” in the HTC treatment process in order to obtain

various functional hydro-char materials.

Fig. 1.

5
 Previously, reports mostly focused on the reaction efficiency, process optimization,

energy balance, or product improvement when HTC technology was applied as the

treatment strategy for FW. For the first time, this review considered the “symbiotic

relationship” between Chinese FW and HTC technology, by discussing FW components

and finding specific properties. This paper may also help in revealing and understanding

the “bottleneck problem” that must be faced during the practical applications of some

disposal methods, especially with AD. Furthermore, this review elaborates upon the

feasibility of HTC technology in the disposal of FW, emphasizing two modes of the

HTC process: “Main force” and “Assistance.” The roles FW plays in each mode are

discussed in order to provide a new awareness and view of the interactions between

Chinese FW and HTC technology.

2. Challenges for disposing food waste in China

2.1 Characteristics of food waste

“People are the foundation of the country. Food is the first necessity of man” is an old

saying in China. Thanks to this concept, China has created a splendid food culture over

thousands of years. However, in the meantime, a high amount of FW has inevitably

appeared as a problem. Fig. 2 (Chen and Gu, 2012; Gupta et al., 2015) clearly shows

that the ratio of FW in MSW ranges from 30% to 60% in China, while it is less than 30%

in other countries, except India. In fact, China has a lot of similar reasons as India does,

such as a big population, poor processing and packaging procedures, and improper

management. So FW definitely is a major part of MSW in China compared with the

6
situation in other countries. However, due to the incomplete combustion caused by the

mixture of FW with MSW, dioxins and other toxic and harmful pollutants might be

generated. So FW needs to be considered as an important factor of whether MSW is

handled efficiently. Moreover, because the materials and cooking methods used in

different regions vary, the composition of food waste is complex. The ingredients in

Chinese FW mostly consist of grains, vegetables, pericarp, plant oils, adipose, meat,

eggs, bones, and adulterants, such as paper and plastic. The details of these properties

are listed in Table 1 (Huang et al., 2016; Liu and Peng, 2015; Tan, 2012). Carbohydrates

are the main compounds in kitchen waste (KW) (solid phase), while the content in swill

(liquid phase) contains more proteins, adipose, salts and lipids (Yuan et al., 2006). The

analysis of the chemical components in Chinese FW has revealed several features,

which can be briefly summarized as high in moisture, organics, lipids, and salinity. The

high organic content may result in perishability and the generation of pathogenic

bacteria. The high lipid levels and high salinity are striking features of Chinese FW. On

the one hand, these could be beneficial for reuse of FW, but on the other hand, these

might become the bottleneck for some disposal methods.

Fig. 2.

Table 1.

2.2 High organics

A high organic content is one salient feature of Chinese FW. Since starches, proteins,

and lipids are the main organic compounds in FW, spoilage is difficult to prevent under

7
high moisture conditions. It not only leads to malodor, which is unpleasant for the

residents, but also generates pathogenic bacteria that are seriously bad to the health (Jin

and Wang, 2012).

Moreover, high organic content is a big hindrance for some treatment methods, such

as smash discharging, landfill, composting, and AD. Smashing and discharging FW into

the municipal sewer network (MSN) has been chosen as the solutions by more than 50%

residents in America (Marashlian and El-Fadel, 2005). Meanwhile, China‘s large

population density is a feature of most cities, which could result in a large amount of

FW with high organic content and lead to an additional load on the MSN and sewage

treatment plants. Thus, this method cannot be widely applied, because it would not be

able to meet the policy on resource and energy recovery, while also having negative

effects on the MSN (Battistoni et al., 2007). Landfilling is a major method used to

dispose of FW in China. If high concentrations of organic leachate leak from the landfill

without proper handling, it may cause pollution of the groundwater and surface water

(Bhatt et al., 2017). If the gaseous landfill emissions, in particular methane, are not

collected and used properly, it might become a burden on carbon reduction efforts.

Moreover, volatile organic compounds created from the landfill process may further mix

with hazardous air pollutants and do harm to people (Saral et al., 2009). So, China aims

to realize a “zero landfill” policy for its FW by 2020. Actually, not only China, but

many countries have also taken the appropriate measures to limit landfill use. For

example, Singapore forbade disposal of FW in landfills in 2005. Sweden only permits

8
less than 5% organic content of FW to be disposed of by landfill. Germany has

prohibited the landfilling of organics since 2005.

For the AD process, since carbohydrates are easily degradable organic materials, high

carbohydrate content may lead to excessive acidification, which might be harmful to the

stability of the AD process (Hao et al., 2017). Except that, high lipid content is another

factor limiting AD. Because long-chain fatty acids are difficult to hydrolyze, it not only

restricts the hydrolysis rate but also accumulates within the system (Karthikeyan and

Visvanathan, 2013). Furthermore, high lipid content leads to oils covering the surface of

the FW, forming a layer that creates an anaerobic state inside and decreases the pH so it

is a bad candidate for composting (Arvanitoyannis and Kassaveti, 2007; Schwalb et al.,

2011). If the lipids appear in higher concentrations, composting may not be able to

reach the reaction temperature, resulting in lower efficiency for sterilization purposes

(Luo et al., 2014). In addition, it might become an influencing factor on the reaction rate

and quality of the products.

2.3 High moisture

Normally, moisture accounts for more than 77% in Chinese FW. This means there are

less choices for the industrial arts and more difficulties in the pretreatment process. It

affects mostly the incineration method, which is a proven technology that is chosen by

many countries. Although incineration can meet the requirement of minimization of up

to 60%-80% of waste volume, Chinese FW contains high moisture and low heating

values, which causes additional fuel consumption during its burning (Edo et al., 2016).

9
Moreover, adding combustion additives may lead to the production of dust and toxic

pollutants, which are bad for the environment and ecology. Although incineration

accounts for 37.5% of harmless treatments (reported by SYB-2017), it is difficult to

promote nationwide. The main reason is that the residents fear dioxins, even if it meets

emission criteria (Hong et al., 2017). For example, there were 44 waste disposal projects,

including 10 waste incineration power plants, which were planned for construction in

Beijing in 2009. However, due to the residents opposing their construction, they were

postponed indefinitely.

2.4 High Salinity

The salinity of KW and swill in FW are both at high levels. This is the potential

disadvantage in feeding and composting them. In the literature reported, when the

salinity of feed is higher than 1.8%, it affects the health, growth, and development of

adult livestock. Unfortunately, the salt content of the produced feed based on the

existing patterns is twice the threshold amount (Nong et al., 2014). For composting,

deterioration in the quality of the fertilizer might occur due to the high salt content

(Chan et al., 2016). This may result in plant cell dehydration and inhibit seed

germination, especially if the level of soluble salts is high, as the electrical conductivity

will be reduced (X. Wang et al., 2016). Moreover, long term use of these fertilizers will

lead to soil salinization (Wong et al., 2009). By contrast, high chili and acetic acid

content, which are additives used in cooking, such as in Sichuan and Shanxi province,

could do harm to the biological treatment process.

10
3. Opportunities for application of hydrothermal carbonization

3.1 Mechanism

Hydrothermal conversion refers to feedstock reacting in liquid media under high

temperatures and corresponding pressure conditions, creating target products that can be

classified as belonging to the solid, liquid, and gas phases. With temperatures above 100℃

and below 700℃, the main products will be transformed from the solid phase to the gas

phase, which can also be regarded as a carbon transformation pathway (Libra et al.,

2011). Compared with liquefaction and gasification, HTC technology is a low

temperature hydrothermal conversion that could also be defined as wet pyrolysis. HTC

conversion is an exothermal reaction that is accompanied with the removal of functional

groups. Although products are distributed throughout the three phases during the HTC

process, the main focus is the carbon-like solid, which is called the “hydrochar”,

together with some soluble organic compounds in liquid and gas. It is a complex

reacting network that includes many parallel chemical reactions; however, the details

are not clear yet. So, the general mechanisms have been identified as five main

procedures, including hydrolysis, dehydration, decarboxylation, condensation,

polymerization, and aromatization. In the beginning, the ingredients are hydrolyzed to

become oligomers and monomers, most of which could also be regarded as water

soluble organic compounds, such as organic acid, furan-like compounds, and phenols,

etc.. The rate of hydrolysis is based on the behavior of these fragments, as how they are

diffused and transformed would influence the subsequent mechanisms. During the

11
hydrolysis process, dehydration and decarboxylation occrs parallel with the

condensation and polymerization, which are not started in order during the whole

process. The intermediates might be highly valued byproducts, such as

hydroxymethylfurfural (HMF), while others might be insoluble fragments. Further

aromatization via the intrinsic dehydration of the polymers may contribute to the

hydrochar (Marta Sevilla and Fuertes, 2009). Throughout the whole process, a

hydrophobic aromatic nucleus can be formed that may end up with a hydrophilic shell

outside the nucleus after growth.

Actually, the type of feedstock plays an important role in controlling the

intermediates in the HTC process, such that it can influence the structures and

morphologies of the final products to a large extent (Deng et al., 2016). FW is a mixture

and its main components are carbohydrates, lignin, proteins, and lipids. The

decomposition pathways of FW in the HTC process are illustrated in Fig. 3. Compared

to lignin, the carbohydrates include starch, cellulose, and hemicellulose, which can be

easily hydrolyzed under HTC conditions. Glucose and xylose are the main

intermediates, while the final organics mostly consist of HMF and furfural in the liquid

phase (Lichtenthaler and Peters, 2004; Moreschi et al., 2004; Rogalinski et al., 2008).

Lipids from plant oils and animal fat are minor components in FW that are difficult to

dissolve in water unless under supercritical conditions, so they may also be hydrolyzed

into glycerol and fatty acids. The mechanism of FW disposal through HTC technology

can be investigated according to the basic ingredients, but whether the intermediates or

12
byproducts can interact with each other still requires further study.

Fig. 3.

3.2 Process parameters

Based on the reaction mechanisms, the process parameters that influence the HTC

processes are observed. Mostly, the water content of the raw materials is above 50 wt%.

This liquid water at subcritical state not only acts as the reactant, but as the solvent and

catalyst (Pavlovič et al., 2013). The pH value decreases during the HTC process

spontaneously because of the byproduct generated. The starting value should be lower

than 7 to make sure that the specific products can be obtained. The temperature is

always within the range of 150℃ to 350℃ while the retention time has no clear

limitation. According to the unknown reaction rates under different conditions of the

various raw materials, most published studies reported times between 1h to 72h (Funke

and Ziegler, 2010). Table 2 lists the recent studies on process parameters for food waste

disposal.

Table 2.

3.2.1 Reactant media

HTC is a general thermochemical method that differs from pyrolysis and gasification

in the main factors of temperature and reactant media. HTC media requires the liquid

state and the feedstock needs to be submerged at all times. Usually, subcritical and

supercritical water are the ideal media choices in HTC conversion, although some

researchers have tried other liquid streams instead. Subcritical and supercritical water

13
have many advantages compared with water at normal pressure levels. During the HTC

process, with temperatures ranging from 150℃ to 350℃, the water is in subcritical

condition. The density drops with the rising temperature, thus the properties of the water

change. Non-polar water dominates the whole process as it easily dissolves organic

compounds. Since the organics mostly come from hydrolyzed feedstock, this property

of non-polar water as well as the increase in the diffusion coefficient are beneficial, not

only to the reaction efficiency, but also to the interaction between the functional groups.

For example, the hydrogen bonds can be easily cleaved under these conditions (Hatcher

and Clifford, 1997). Moreover, when the temperature is below the critical point, the

ionic reactions, rather than the free radical reactions, dominate (Tran et al., 2016). The

ionic reactions promote char formation, so it influences not only carbon distribution, but

also the final products (Behar et al., 2003).

In some studies, the replacement of pure water with other reactant media, such as

process water, activated sludge, and landfill leachate, have also been reported. For

example, using recycled water in pomace disposal has increased the mass yield of the

solid phase, whereas the properties of hydrochar, such as its elemental composition and

heating value, were not changed (Kabadayi Catalkopru et al., 2017). When applying

activated sludge and landfill leachate to MSW, the liquid sources contributed to the

carbon distribution, solid properties, and liquid quality. Additionally, they may also have

increased the sustainability of the carbonization process (L. Li et al., 2014). Therefore,

the reactant media plays an important role in HTC conversion, whether it is pure water

14
or other liquid streams.

3.2.2 Mass ratio

The mass ratio, which also can be called the solid load, refers to the ratio of the

feedstock to the reactant media. It is a significant parameter for the substrate. This

parameter not only influences polymerization and shifts the reaction network, but also

impacts the physical property and yield of the hydrochar. The initial ratio is a factor of

the concentration of monomers in the liquid phase. When the monomers are present at

high concentrations, the polymerization can be promoted and products in the liquid

phase can be reduced (Marta Sevilla and Fuertes, 2009). If the reaction takes a long time

to approach solution equilibrium, a higher mass ratio is unfavorable for increasing the

concentration of monomers (Racovalis et al., 2002). Meanwhile, if there is not enough

time for polymerization, a large number of feedstock might react incompletely, even

leading to a high initial ratio (Jain et al., 2016). For solid products, under high solid load

conditions, the reported results mostly showed a large size of microspheres and high

production of char. The intermolecular dehydration and aldol condensation might be the

reason for the larger sized char obtained with the polymerization mechanism. Otherwise,

the retention time and mass load are also co-factors. Normally, a high mass load leads to

large sized products; however, if the retention time is too short for the absolute reaction,

the size reduces. Comparatively, large sizes might be obtained with a low concentration

of feedstock, unless the load is close to zero and the intermediates have mostly

dissolved, which could also be regarded as the substrate in the following condensation

15
reaction (Romero-Anaya et al., 2014).

3.2.3 Temperature

Temperature is a key point in the HTC process, as it controls the degradation

conversion, determines the reaction rate, and influences the distribution of the products

to some extent. Hydrolysis is the first stage of the HTC process, while different

components in the substrate reveal specific behaviors based on the temperature.

Cellulose, hemicellulose, starch, lignin, and even the lipids and proteins are all main

components of FW. Hemicellulose and starch can be easily dissolved, starting at 160℃

and 200℃ respectively (Kumar and Gupta, 2008). Lignin and cellulose begin to

hydrolyze at 200℃ and 220℃ (Funke and Ziegler, 2010). Lipids could contribute fatty

acid and glycerol at higher temperatures and proteins degrade slowly into amino acids.

For the temperatures listed in Table 2, most researchers chose ranges from 220℃ to

250℃ as the reaction parameters applied to FW. With the increase in temperature, the

chemical bonds are cleaved to a large extent, while monomers or oligomers, such as

glucose, xylose, and cellobiose, etc., are produced (Möller et al., 2011). Different

components may impact each other due to the temperature influence. For example, the

crystalline structure of cellulose might be stable at lower temperatures together with

lignin (Falco et al., 2011). Under HTC conditions, when the temperature is less than

280℃, some studies reported similar conclusions about cellulose and starch. The ratio

of O/C and H/C in the hydrochar drops with increases in temperature and the influence

of carbon distribution is evident to some extent (Marta Sevilla and Fuertes, 2009). The

16
size of physical structure of hydrochar is also changed by the temperature. The reason is

the nucleus and polymers are linked by oxygenated functional groups during the

nucleation growth process, and the functional groups are formed through different

degrees of reactions, which is governed by the temperature (M Sevilla and Fuertes,

2009). Additionally, the properties of the reactant media are changed by the increasing

temperature, which has already been discussed above.

3.2.4 Retention time

The retention time is also an important factor through the whole process, although it

varies with the temperature, so it still needs to be considered in the studies. The quantity

of some functional groups or intermediates vary as the time increases. As the time

lengthens, hydroxyl groups dehydrate and the concentration of lactone in the liquid rises.

However, oxygenated functional groups may increase first to a turning point and then

drop during the conversion. The reason for this might be the groups stabilized in the

surface or decomposed as gas products over a longer retention time (He et al., 2013).

However, with the same retention time but increased temperatures, the peak of the

product may appear at higher temperatures (Zhang et al., 2014). However, these

observations may not be appropriate for all raw materials. Other mass ratios and various

combinations of temperatures and duration times may lead to different results (Cao et al.,

2013). Besides the chemical reaction mechanism, it also contributes to the yields and

properties of the target products. Usually, solid products decrease when the retention

time is long enough (Hoekman et al., 2011). But if the yield increased, then the reason

17
mostly is due to the precipitation of the undissolved matters which may be produced

from the polymerization of the soluble oligomers with further reactions (M. M. Titirici

et al., 2007). There is no limit on the retention time and the duration varies from hours

to days, whereas short durations may not be more than one hour long. Table 2 provides

evidence for applying HTC to FW. Based on the different sources, most researchers

used retention times ranging from 20min to 2h. When HTC is applied as a pretreatment

method, time is often limited to less than 1h.

3.3 Characteristics of feedstock

Feedstock has no specific limitation in the HTC process, only preferring carbon rich

materials that can be transformed into a high energy density char. However, the high

moisture content in feedstocks, which contains 75% to 90% water or even higher, is

more suitable than those in which the water content is not more than 40% because

feedstock with low water content has no preponderance for energy recovery in this

process (Libra et al., 2011). In contrast to dry pyrolysis, which is not applicable when

the moisture of feed is between 50-70%, HTC technology is wet pyrolysis that has

certain energetic advantages. So, the HTC reaction does not need any dewatering

pretreatments, which can save on costs compared to other thermal treatments, such as

incineration, gasification, and dry pyrolysis. In the case of HTC technology, it would be

a good method for treating FW in this respect, because it can meet the need of

converting high water content substrates into high energy and valued products.

Furthermore, after HTC conversion, high moisture feedstocks can achieve the goal of

18
reduction of the liquid volume (Li et al., 2013). This might be a solution for a big

problem that must be faced in China, in which there is currently no effective way for

reusing or treating a large amount of the processed water after AD disposal of Chinese

FW.

In addition, high organics is one characteristic of Chinese FW which can be the

reason behind the generation of pathogens and putrid smell during its collection and

transport or even after undergoing biological treatment methods. Because the

temperatures of the HTC process ranges from 150℃ to 350℃ while the sealed reactor

maintains the autogenous pressure, sterile conditions that do not release bad odors can

be realized during the whole process (Phuong et al., 2015). Thus, it can be seen that

HTC technology is appropriate for the disposal of Chinese FW for the purposes of

hygienic protection, not only in the process but also for the products. Fig. 4 illustrates

the adaptability between the specialty of HTC feedstock and the characteristics of

Chinese FW, which is the root cause for the opportunity of using HTC as a treatment

method for FW.

Fig. 4.

3.4 Role as “Main Force”

In the beginning, HTC technology was used in coal petrology to achieve natural

coalification. The first patent for this technology, called “wet carbonization,” was

applied to peat bogs and can be dated back to 1850 (by Vignoles) (Lau et al., 1987).

Next, Friedrich Bergius initially used this method on cellulose in 1913, before more and

19
more researchers focused on the economic energy feedstocks, such as hemicellulose,

lignin, saccharide, and their derivatives. The latest investigations have focused mainly

on high water content wastes, such as sewage sludge, manure, and wet biomass in

attempts to obtain value-added chemicals and recover nutrients. Furthermore, it can also

be regarded as an innovative solution for the disposal of some carbon rich wastes, which

aim to obtain target products, such as functional carbonaceous materials, or to achieve a

specific processing effect.

3.4.1 Production and application

Because the HTC reaction is a carbonization process, the main solid product derived

from this technology should be the hydrochar, which can replace fossil fuels. In contrast,

the byproduct is in the liquid state. It might be the bio-oil produced at high temperatures

from HTC technology, the value-added chemicals obtained from the specific

intermediates, or the nutrients recovered from the processed liquor. Additionally, the

yield of the products and energy efficiency of the whole process are also hot points.

Malaták et al. (Malaťák and Dlabaja, 2016) stated that the water content should be less

than 15% wt. in solid fuel to be able to meet the requirements of combustion. The

hydrochar obtained through the HTC process can be used as fuel for incineration in

boilers, with 66% wt. of carbon content and a heating value of about 26.6MJ/kg, which

is more than the value of lignite. Bhuiyan et al. (Bhuiyan et al., 2014) analyzed the

components of the liquid products produced by HTC reaction with food garbage,

indicating that valuable chemicals, such as furan, furfural, and HMF, might be collected

20
as basic synthetic materials. Mahmood et al. (Mahmood et al., 2016) focused more on

the energy efficiency of HTC conversion for FW, proving that the efficiency decreased

from 94% to 74% when the temperature increased from 150℃ to 350℃. Meanwhile,

they found that the target product can be controlled by choosing the parameters—for

instance, bio-oil prefers lower temperatures, while hydrochar needs to balance the

energy in the whole process. Except that, Kaushik et al. (Kaushik et al., 2014) reported

that by adding specific compositions of enzymes in the HTC conversion process of FW

might be a good choice for a balanced co-production of hydrochar and bio-oil.

In the case of the applications of the downstream products, some researchers adjusted

the properties of the hydrochar by controlling different process parameters, such as the

carbon content, heating value, microcrystalline structure, and morphological size, so as

to obtain functional materials that could be used as adsorbents, catalysts, solid additives,

and ion exchangers (Wu et al., 2016). Xu et al. (Xu et al., 2015) stated that hybrid

carbon sources can enhance the production and fluorescence of carbon containing

fluorescent nanodots (CFDs). So they applied HTC technology on Chinese kitchen

waste at 180℃ for 6h to facilely synthesize CFDs which have a high selectivity for

Fe3+ ions based on fluorescence quenching. F. Zhang and Q. Wu (Zhang and Wu, 2012)

assumed that iron salts play an important role in affecting the organic pathway and

limiting the reduction of nutrients. Adding ferric salts to change the yield and properties

of the hydrochar, the solid products from the HTC processing of Chinese FW reveal

adaptability in the catalytic fields. In addition, Parshetti et al. (Parshetti et al., 2014)

21
reported that the hydrochar produced from urban FW at 250℃ can be used as

adsorbents to remove dyes, such as Acridine Orange and Rhodamine 6G, from

wastewater. They also proved that hydrochar can meet the requirement of adsorption

through a lower degree of carbonization process. Kaushik et al. (Kaushik et al., 2014)

also founded that the hydrochar obtained at 350℃ from FW showed a homogenous

distribution of microspheres. This product has the potential to improve surface areas,

which can be regarded as an adsorbent that can be used to remove environmental

pollutants.

3.4.2 Effect of disposal process

FW disposal contributes to greenhouse gas (GHG) emissions, which contains CO2,

CH4, and N2O, that could cause global warming to some extent. The global warming

potential (GWP) of landfills or incineration is about twice as much as from composting

and AD (Kim and Kim, 2010). To surmount this negative impact on the environment, a

large amount of work has been done to attempt to solve the problems resulting from

these disposal methods. For instance, AD has been used as a pretreatment method

together with incineration, which can reduce the 70kg CO2eq/t-waste of GWP (Takata et

al., 2012). Composting and AD technology have also been combined in order to achieve

the goal of reducing 70% more of GHG than through incineration (Khoo et al., 2010).

Owing to the differences that exist in the FW management methods, such as system

boundaries and considered substitution, it is difficult to compare their exact contribution

to GWP (Yano and Sakai, 2016). However, when HTC technology is applied to FW, it

22
does have more advantages for CO2 reduction, because its chemical mechanism leads to

specific carbon distribution. Typically, carbon is distributed mainly in the hydrochar,

accounting for 50% to 80%, compared to its content in the liquid phase ranging from 5%

to 20% and even less than 5% in the gas phase (Libra et al., 2011). This ratio is

consistent with the proportion of the mass in the products and can also reveal the

performance of the carbon emission reduction. Li et al. (Li et al., 2013) focused on FW

and packaging materials (PMs), which is also a part of MSW in daily life. The results

showed that the majority of the carbon remained solid, with more than 70% from FW

sources and more than 74% from PMs, while smaller fractions of the carbon was in the

gas phase, which was limited to 10% or less. Also, they reported that the initial solid

proportion was the crucial impacting factor on the carbon migration.

Putrescibility is a symbolic feature of FW. Chinese FW is rich in water, oils, salts, and

nutrients, which can offer suitable conditions for the growth of pathogens and microbes.

Currently, more and more disposal methods prefer to regard FW as the “recycling of

carbon sources” and expect to recover energy from it. So, the hygienic properties of

products play an important role in the application to avoid the secondary pollution of

human life. In the case of HTC technology, the products are able to meet this demand.

Sancho et al. (Sancho et al., 2004) reported that thermal method of over 65℃ for 20min

can achieve a sufficient level of sanitization. By contrast, Chen et al. (Chen et al., 2012)

tested FW containing select indigenous microbes and found complete sterilization could

be achieved through the hydrothermal method at 120℃ for 40min. Normally, when the

23
temperature of the HTC process is higher than 150℃, the products of this conversion

are sufficiently hygienic and safe. However, the process water releasing from this

process is still a problem. So, disposing this process water should aim at harmless for

the environment or realize pollution reduction through a simple post-treatment. Malaták

et al. (Malaťák and Dlabaja, 2016) reported that increasing the retention time can

minimize the negative impact of germination by testing the processed liquid. Also, the

liquid byproducts of FW from HTC conversion are harmless to agriculture according to

their phytotoxicity test. Beyond that, using bio-treatment on the malodorous substances

in discharged liquid revealed they were harmless to both the environment and human

health (Bhuiyan et al., 2014).

3.5 Role as “Assistance”

The HTC process can be used either as a method to obtain target products, or as a

coupling approach to assist other technologies in order to achieve the desired effect.

Although AD is widely used as a promising management strategy for FW disposal in

China, there are still some challenges in the process to be solved. Currently, most AD

pilot plants are under-performing and are unable to recover the investment or gain profit.

Therefore, as a pretreatment method, hydrothermal technology might be helpful for

solving specific problems in the AD process. Compared with other pretreatments,

despite the high heat demand and high cost of the devices possibly being the

weaknesses of hydrothermal technology, it does have many advantages, such as

scalability and sanitation (Carrere et al., 2016). However, pilot scale applications have

24
only been successful in the sanitation of animal byproducts, such as the “Suzhou Jiejin

Food Waste Recycling Project” in Jiangsu province, while other possibilities are still at

the lab scale stage.

As the main parts of MSW, FW is one of the hot topics in AD application in China.

There are many problems involved with applying AD to FW, such as operational

stability, hydrolysis rate, retention time, volatile fatty acid (VFA) production, biogas and

hydrogen yield, and bacterial activity, etc. Many studies have tried to couple short-term

hydrothermal pretreatment (SHTP) with different kinds of AD processes, such as single

stage AD (SSAD) and two stage AD (TSAD), and investigated the influence of the

pretreatment FW in the following AD process. SHTP can lead to the degradation of FW,

promoting the initiation of CH4 production and the stability of the feed utilization

during the AD process (Jia et al., 2017). The potential of hydrogen production could be

improved by SHTP. One reason might be that it limits the inhibition of the long-chain

fatty acids from the high lipid content in FW (Lee and Chung, 2010; Ma et al., 2011).

The other reason might be sterilization. Hydrogen generating bacteria, such as

Clostridium, can protect themselves by forming spores. In contrast, hydrogen

consuming bacteria are unable to survive without special spores in FW (Z. Hu et al.,

2012). By coupling with SHTP, Jia et al. (Jia et al., 2017) found that the lag phase time,

which is not only the rate-determining step but also controlling the methanogenic stage,

could be shortened in the TSAD process. Furthermore, the proteinoids were

prominently degraded, and because of the improved hydrolysis of the dissolved organics,

25
the ethanol and methane yields were increased. Li et al. (M. Li et al., 2014) tested

various temperatures in pretreatments to see which could affect the protein conversion

and solubility of organics to consequently change the results in AD. In addition, the

author also reported that coupling SHTP with AD can improve the hydrogen yield.

Furthermore, they proved 90℃ to be the suitable process parameter for pilot scale

applications, by balancing the energy and H2 production. In addition, Li et al. (Li and

Jin, 2015) also reported that the temperature of SHTP should not be higher than 120℃,

as it would be better for economic efficiency and may retain enough nutrients for the

AD process. Meanwhile, the distribution of VFA in AD is influenced by the temperature

and retention time of SHTP. Hydrothermal technology is not only suitable for

pretreatment, but also for reusing output (Malaťák and Dlabaja, 2016). A large number

of the processed water resulting from the AD process is a big problem that demands to

be solved. During the post-treatment process of HTC, the separation of solid and liquid

products can minimize the initial volume produced.

4. Conclusions

In terms of symbiosis relationships between Chinese FW and HTC technology, on

one hand, FW might not be the best feedstock compared with other carbon-rich sources,

but disposing it could obtain value-added products and contribute to carbon reduction.

On the other hand, due to operate conditions and device cost limitation, HTC might not

be the main disposal method, but combination with AD as an “assist” do play a crucial

role in whole process. While, how to balance the pros and cons in symbiosis

26
relationship, so as to achieve harmless and maximum energy recovery, is the emphasis

in the further studies.

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Fig. 1. Relationship between food waste and HTC technology

35
Fig. 2. Ratio of food waste in municipal solid waste in different Chinese cities and other
countries

36
Fig. 3. Pathways for decomposition of main component of food waste in HTC process

37
Fig. 4. The adaptability between HTC technology and food waste in China

38
Table 1. Physicochemical properties of food waste in China
General Composition Main Components b Ultimate analysis/ Nutrients
b
Moisture 77-95 Food residue 75-90 Cb 42.05-47.67
Salt b 0.5-3 Grease 2-17 Nb 1.91-3.89
a b
Crude Protein 13-27 Bone 5.2 O 30.22-34.87
Crude Lipid a 17-42 Wood 1.0 Hb 5.25-5.94
a b
Crude Cellulose 2.6-6.5 Paper 0.8 S <0.55
Plastic 0.7 Cl b 0.21
Metal 0.1 C/N 10-30
Ca >0.0048
P >0.0042
K >0.0018
a
Crude protein, crude lipid and crude cellulose were given in in wt% on the basis of dry weight.
b
Moisture, salt, C, N, O, H, S, Cl, C/N and physical composition were given in wt%.

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Table 2. Research in process parameters for food waste in HTC conversion
Source of feedstock Process Parameters Reference
Temperature is 140℃；Retention time is 20min；
Mixed FW with Rice and
Mass ratio is 1:30 (Li et al., 2016)
Potato

Temperature is 150℃ and 250℃；Retention time

(Kaushik et al.,
FW from campus canteen is 20min；Mass ratio is 1:1
2014)

Temperature is 150℃ and 250℃；Retention time

(Mahmood et al.,
FW from campus canteen is 20min；Mass ratio is 1:4
2016)

Temperature is 175℃, 190℃, 225℃, 260℃；

Retention time is 30/60/90/120min；Mass ratio is (Erdogan et al.,
FW (orange pomace)
1:8 2015)

Temperature is 180℃, 200℃, 220℃；Retention

Mixed FW from MSW time is 30min；Mass ratio is 1:1 (Kim et al., 2012)

Temperature is 180℃ and 220℃；Retention time

FW (grape pomace) (PetroviL et al.,
is 1h ；Mass ratio is 1:5
from landfill sites 2016)

Temperature is 200℃ and 250℃；Retention time

Mixed FW from MSW is 1h ；Mass ratio is 1:9 (Smith et al., 2016)

Temperature is 215℃；Retention time is 10min；

(Malaťák and
FW from campus canteen Mass ratio is 1:9
Dlabaja, 2016)

Temperature is 225℃；Retention time is

FW (grape pomace) 10/30/60min；Mass ratio is 1:4 (Pala et al., 2014)

Temperature is 225℃, 250℃, 275℃；Retention

FW from restaurant time is 96h；Mass ratio is 1:2 (Li et al., 2013)

Temperature is 250℃；Retention time is 20min；

(Parshetti et al.,
Urban FW Mass ratio is 1:3
2014)

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HIGHLIGHTS
 Food waste can be regarded as an obstacle in disposal or as carbon source to reuse.
 HTC can play a role as “Main Force” or “Assistance” in food waste disposal.
 Knowing symbiotic relationship can help to solve dilemma of MSW disposal in
China.

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