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Exploring on the optimal preparation conditions of activated carbon produced from solid waste produced from sugar industry and Chinese medicine factory

  • Zhen LiEmail author
  • Qiang Han
  • ZhiFan Zong
  • Qi Xu
  • KaiWei Wang
Article

Abstract

The waste biomass produced from sugar industry and Chinese medicine factory such as bagasse, reed root residue, pueraria residue and liquorice residue were selected as the raw material for the preparation of activated carbon with zinc chloride as activator. With the same activation time, the influence of temperature and impregnation ratio on the preparation of activated carbon was investigated and the reasonable preparation conditions of activated carbon were monitored and analyzed. The obtained activated carbon samples were characterized by scanning electron microscopy, Brunauer–Emmett–Teller, methylene blue adsorption, thermogravimetric analysis and nitrogen adsorption–desorption. Analysis from the experimental data, bagasse, reed root residue, pueraria residue are suitable for preparing activated carbon. For bagasse, the optimum preparation condition was 700 °C and the impregnation ratio was 1:1, the adsorption capacity of methylene blue reached 246.83 mg/g at the moment. For reed root residue, the optimum preparation condition was 600 °C and the impregnation ratio was 1:2, the adsorption capacity of methylene blue reached 268.07 mg/g at the moment. For Pueraria residue, the optimum preparation condition was 700 °C and the impregnation ratio was 1:2. The adsorption capacity of methylene blue reached 297.33 mg/g at the moment.

Keywords

Activated carbon Waste biomass Nitrogen adsorption–desorption Optimize 

Introduction

Activated carbon can be made from almost any organic material which are rich in carbon, such as coal [1], wood [2], and nut shells [3, 4]. These carbon-containing materials are converted into activated carbon by pyrolysis in an activation furnace. In recent years, more and more people choose to use biomass waste as activated carbon raw materials. The development of sugar industry and Chinese medicine industry has brought about a lot of biomass solid wastes, such as bagasse, reed root residue, pueraria residue, liquorice residue and other low-cost low-ash lignin materials. At present, these kinds of waste residue are used as agricultural fertilizers, biogas materials and animal food, with low utilization rate and high carbon emissions. Furthermore, due to the large amount of waste residue and easy fermentation, most of it has not been effectively reused, resulting in a lot of pollution and waste.

Activated carbon is a general term for carbon materials with developed pore structure, large specific surface area, abundant surface chemical groups and strong specific adsorption ability [5]. In isolation from the air,the organic material (shell, coal, wood, etc.) was heated to reduce the non-carbon components (carbonization) and reacted with the activator (activation), eroding the surface to produce a microporous structure [6].

Activation process is a microscopic process that the surface erosion of carbide occurs in the form of pitting. Therefore, carbonization could make the surface of activated carbon produce a large number of fine pores. Activated carbon is a very effective adsorbent, with the dual characteristics of physical adsorption and chemical adsorption, it could be selected through adsorption of various substances in the gas phase, liquid phase, to achieve decolorization purification, disinfection and deodorization and decontamination purification purposes. Almost all applications of activated carbon are based on its porous structure and surface chemical properties [1, 7].

The surface of activated carbon is rich in pore structure even a small amount of activated carbon has a huge surface area. The surface area of each gram of activated carbon can reach to 500–1500 m2 [6]. The adsorption performance of activated carbon depends not only on the physical (pore) structure of activated carbon, but also on the chemical structure of the surface of activated carbon. During the preparation of activated carbon, unsaturated chemical bonds were formed in the carbonization stage, which could react with heterocyclic atoms such as oxygen, hydrogen, nitrogen and sulfur to form different surface groups, thus affecting the adsorption performance of activated carbon.

The preparation of activated carbon can be divided into three types: chemical activation method, physical activation method and physico-chemical activation method. Chemical activation method is to prepare activated carbon through the process of carbonization, activation, chemical recovery, rinsing, drying and so on. Reagents such as phosphoric acid [8], zinc chloride [9], potassium hydroxide [10], sodium hydroxide [11], sulfuric acid [12], potassium carbonate [13], polyphosphoric acid and phosphate ester [8] could be used as activators. These chemicals all contribute to the activation of the raw material, although different chemical reactions occurred, some had erosion, hydrolysis or dehydration of the raw materials, and some had oxidation. Zinc chloride is one of the most widely used activator in the preparation of activated carbon by chemical activation method [14]. Impregnation with ZnCl2 causes the degradation of cellulose and dehydration during carbonization. These processes led to carbonization and aromatization of the carbon skeleton and thus form a preliminary pore structure. After the removal of zinc chloride with water, the pore structure is formed. In addition, some scholars believe that zinc chloride forms the skeleton of new carbon deposition during carbonization, and when it is washed away, the surface of carbon is exposed, forming the inner surface of activated carbon with adsorption [6]. Therefore, the chemical activation by zinc chloride (ZnCl2) improves the pore development in the carbon structure.

The most important characteristics of activated carbon is the specific surface area and adsorption ability which are determined by the preparation parameters of activated carbon, such as carbonization temperature, carbonization time and chemical impregnation ratio, putting influence on the pore development and surface characteristics of the prepared activated carbon. The impregnation ratio could determine the distribution of specific surface area and pore diameter, and carbonization time and temperature are important preparation variables for obtaining activated carbon [15] (Namasivayam and Kadirvelu 1997).

In this work, activated carbon was produced from 4 kinds of biomass solid waste (bagasse (BR), reed root residue (RR), pueraria residue (PR), liquorice residue (LR)) aiming to explore the reasonable conditions for preparing activated carbon, where Taguchi orthogonal experiment [16] and response surface method [17] were used to optimize the preparation conditions of ACs. The activated carbon samples were characterized by Scanning Electron Microscope (SEM), Brunauer–Emmett–Teller (BET), Thermogravimetric Analysis (TGA), nitrogen adsorption desorption and methylene blue adsorption.

Materials and methods

Materials

Different types of biomass solid wastes were collected including bagasse (BR) which provided by GuangXi COFCO JiangZhong Sugar CO., LTD., and reed root residue (RR), pueraria residue (PR), liquorice residue (LR) which were provided by GuangDong LianFeng Chinese medicine decoction pieces co. LTD. After being fully washed with distilled water and dried at 100 °C for 24 h, the waste residues were crushed and sieved to the size below 0.500 cm. Methylene blue (AR) and ZnCl2 (AR) were supplied by Fengchuan Chemical Reagent Co., Ltd., Tianjin, China. Nitrogen and air were supplied by Liufang Gases Chemical Reagent Co., Ltd., Tianjin, China. Deionized water was prepared by the laboratory.

Preparation of XACs

XACs were prepared under the conditions which included impregnation ratio (ZnCl2/Corncob, w/w), at 1:0.5, carbonization temperature 800 °C, and carbonization time 1.0 h. In each experiment, 3.0 g of waste residues were thoroughly mixed with 30 mL of ZnCl2 solution of different concentrations [18]. The mixtures were placed at ambient temperature for 12 h and then dried at 100 °C for 12 h getting the samples impregnated. Sequently, the impregnated samples were placed into Nickel containers which have been numbered. Then the sample-laden Nickel containers were put into a 316 stainless steel tubular reactor (SK3-5-12-6 Energy-saving vacuum tube furnace, HangZhou ZhuoChi Instrument co., LTD.) and heated at a rate of 10 °C min−1 to the preset temperature in the presence of N2. After being held at the presented temperature for 1 h, the AC samples were cooled and washed with 1.0 mol L−1 of hydrochloric acid solution at 50 °C for 30 min to remove the metal ions and the ash content. Then, the AC samples were washed with hot deionized water repeatedly until the pH of filtrate reached 7. The washed AC samples were dried at 80 °C in vacuum for 12 h and ground/sieved to the size ranging from 0.180 to 0.425 mm. The final AC samples were labelled as XAC, where X stands for the kind of waste residues.

Optimization of preparation conditions for XAC

In this work, the preparation parameters of XAC were optimized to maximize the adsorption capacity of methylene blue and AC yield by Taguchi orthogonal method and the idea of RSM (response surface method) with two independent factors, carbonization temperature and impregnation ratio. Factors and levels of response surface experiment method are shown in Table 1, and the detailed information of XAC preparation conditions is shown in Table 2.
Table 1

Factors and levels of RSM

Variable

No.

Levels

− 1

0

+ 1

Carbonization temperature/°C

A

600

700

800

Immersion ratio

B

0.5

1.0

2.0

Table 2

Experiment conditions of XAC preparation

Experiment

Influencing factor

Carbonization temperature/°C

Impregnation ratio

1

600

0.5

2

600

1

3

600

2

4

700

0.5

5

700

1

6

700

2

7

800

0.5

8

800

1

9

800

2

XACs characterization

The pyrolysis behavior of the waste residues was investigated using a thermogravimetric analyzer [19] (TG209F3, NETZSCH, GER).

The morphological structures of XACs were observed using a field-emission scanning electron microscope (SEM) (Nanosem 430, FEI, USA).

The textural characteristics of XACs were determined by physical N2 adsorption–desorption at 77 K using an auto-adsorption system (Autosorb-iQ2-MP, Quantachrome, USA). The specific surface area (SBET) was calculated through N2 adsorption isotherm using Brunauer–Emmett–Teller (BET) equation. The external surface area (Sext) was determined using t-plot method. The microporous specific surface area (Smic) was calculated through the difference between SBET and Smic. The total pore volume (Vt) was defined as the liquid N2 volume adsorbed at the relative pressure of 0.99.

Adsorption value of methylene blue of each XAC samples was determined according to the standard of “Test methods of wooden activated carbon Determination of methylene blue adsorption” formulated by CSBTS (state bureau of quality and technical supervision), China [20].

Results and discussion

Pyrolysis behavior of different waste residue

Generally, pyrolysis and activation occurred during the preparation of biomass activated carbon. The pyrolysis behavior of the fore residues is given in Fig. 1 using TG analyzer. All the straws used in this work exhibited similar TG and DTG curves.
Fig. 1

TG (a) and DTG (b) curves of waste residues

The pyrolysis of these 4 waste residues could be divided into 3 stages according to the weight loss (Fig. 1a). The 1st stage occurred at 25–250 °C during which the weight loss was less than 10%. The weight loss could be attributed to the moisture removal. Most of the weight loss happened in the 2nd stage which occurred at 250–400 °C. The weight losses were 60% for pueraria residue, 58% for reed root residue, 60% for liquorice residue, and 58% for bagasse. The corresponding endothermal peaks for this stage (Fig. 1b) of these 4 waste residues were all in the range of 300–350 °C which could be attributed to the pyrolysis of biomass components such as cellulose, hemicellulose and lignin. There was no separation peak of pueraria at this stage, which indicated that pueraria mainly contained lignin, while the remaining bagasse, licorice, and pueraria contained more hemicellulose [21, 22, 23]. Temperature over 400 °C corresponded to the 3rd stage with small weight loss which may be attributed to the slow gasification of small number of intermediate products of pyrolysis.

Figure 1 indicates that most carbonization of the four waste residues was completed below 600 °C. Figure 1a also shows the AC yield at 800 °C according to the residue weight fraction. It indicated that the AC yield sequence of 4 waste residues was RR > LR > PR > BR, among which RR yield was the highest, about 28.04%, while BR yield was the lowest, about 18.62%.

Characterization of XACs

The N2 adsorption–desorption isotherm could be determined to evaluate the porosity of the XACs [24]. Figure 2 shows the N2 adsorption–desorption curve and the BJH pore size distribution of XACs which were prepared at 800 °C when be impregnation ratio was 1:0.5.
Fig. 2

Characterization of different XACs

The pore diameter distribution (Fig. 2b) of PAC and RAC samples showed an obvious peak distribution in the range of mesoporous and microporous (< 0.6 nm) which provided high specific surface area [25]. It indicated that there were almost no micropores in LAC, and the pore size distribution was mainly mesoporous and microporous, while the pore diameter distribution of LAC showed different characteristics that the pore diameter was larger than 0.6 nm. The pore size distribution of BAC was similar to LAC, but according to BJH analysis, BAC had a distribution peak at 0.6 nm, indicating that there were mesoporous holes of about 0.6 nm in BAC.

Detailed surface area and porosity volume of the XACs are presented in Table 3. In general, the surface area and pore volume were depending on micropores,and consistent with the isotherms and the pore size distribution provided in Fig. 2b.
Table 3

Textural properties of XACs

Sample

Specific surface area (m2 g−1)

Pore volume (cm3 g−1)

SBET

Smic

Sext

Vt

BAC

175.311

147.267

28.043

0.131449

RAC

729.802

480.69

249.112

0.477544

PAC

622.797

572.975

49.822

0.361823

LAC

21.465

10.063

10.402

0.041615

By comparison with specific surface area, pore volume and pore diameter distribution, the following rules were obtained: PAC > BAC > LAC. Among the 4 XACs, the RAC exhibited the largest specific surface area, pore volume and pore size distribution, thus may have better adsorption properties.

SEM (Fig. 2c) shows that RAC and PAC have uniform pore structure with small pore diameter, BAC has slightly larger pore diameter, and the structure of LAC is loose and almost no regular pore structure, which was caused by different reactivity and distribution of different components.

Effect of factors on activated carbon prepared

The experimental variables were controlled by Taguchi orthogonal method. Table 4 shows the influence of the two independent factors, carbonization temperature and impregnation ratio, on the adsorption capacity of methylene blue and AC yield of BAC, RAC, PAC and LAC samples.
Table 4

AC yield and methylene blue absorption of XACs

XAC type

Carbonization temperature (°C)

AC yield (%)

Methylene adsorption (mg/g)

Impregnation ratio

Impregnation ratio

1:0.5

1:1

1:2

1:0.5

1:1

1:2

BAC

600

45.24

55.04

50.12

119.55

180.66

218.09

700

39.90

40.98

42.65

92.78

264.83

250.50

800

32.02

30.23

37.27

71.99

243.45

247.09

RAC

600

32.5

35.5

34.3

175.16

243.62

268.07

700

32.1

35.3

32.6

162.94

248.63

249.52

800

25.9

24.4

24.2

105.19

243.45

257.53

PAC

600

33.3

39.7

33.7

23.81

199.46

311.39

700

32.3

33.9

34.1

62.65

141.39

297.33

800

30.9

31.6

32.3

52.83

180.50

235.56

LAC

600

58.4

44.1

16.3

16.74

30.78

45.07

700

60.9

42.8

29.6

49.37

57.04

60.58

800

41.5

38.3

24.9

20.10

132.42

220.13

The influence of impregnation ratio

In this part, adsorption capacity of methylene blue and AC yield of XACs at different impregnation ratio is discussed when the carbonization temperature are at 600 °C, 700 °C and 800 °C.
  1. 1.

    The influence of impregnation ratio on AC yield.

     
It could be seen from Fig. 3, among the four activated carbons, LAC has the highest AC yield at low impregnation ratio, up to 60.9%, while bagasse as raw material has a higher AC yield. As shown in Fig. 3, for BAC, RAC and PAC, the AC yield increases with the increase of impregnation ratio, but when the impregnation ratio reaches 1:2, the growth of AC yield slows down and even decreases.
Fig. 3

Influence of impregnation ratio on AC yield

This phenomenon is due to the fact that zinc chloride has a protective effect on the carbon skeleton when the impregnation ratio is relatively low, and because of the short activation time, the burning loss of activated carbon is difficult to occur. At the same time, in the activation process, zinc chloride has the function of catalytic dehydroxy and dehydration, which causes the hydrogen and oxygen in the raw materials to be expelled as water vapor. In addition, this process can inhibit the production of tar, avoid clogging pores, thus producing XACs with porous structure. However, if the impregnation ratio is raised to a certain value, the AC yield will not continue to increase due to the limited carbon content in the raw material itself, and excessive zinc chloride will enhance the dehydration, which may cause the decline of the AC yield when the impregnation ratio reaches 1:2.

However, for LACs the AC yield decreases significantly with the increase of impregnation ratio within the experimental temperature range. This may be related to the structure or property of the raw material itself, which can be inferred from the pore size distributions, furthermore the adsorption capacity of methylene blue will be analyzed next.
  1. 2.

    The influence of impregnation ratio on adsorption capacity of methylene blue.

     
As shown in Fig. 4, in the sample of the same raw material, the activated carbon with an impregnation ratio of 1:2 is the strongest adsorption ability to methylene blue, which is suitable for the four kinds of waste residues.
Fig. 4

Influence of impregnation ratio on adsorption capacity of methylene blue

As an activator, zinc chloride could etch the raw materials and change the internal structure of them. With the increase of impregnation ratio, the content of zinc chloride gradually increased compared to the whole, and the zinc chloride played a significant role in improving the performance of activated carbon and the adsorption ability of XAC to methylene blue. However, when the impregnation ratio exceeded a certain value, increased the proportion of zinc chloride would lead to excessive activation, leading to changes in the structure of activated carbon and the connection or disappearance of pores, leading to a decrease in the adsorption performance of activated carbon, which may reduce the adsorption capacity of XAC [26].
  1. 3.

    Analyzed by SEM.

     

The morphological structures of XACs were observed using a field-emission scanning electron microscope (SEM) [27] (Nanosem 430, FEI, USA).

Impregnation ratio was regarded as an independent variable, whose influence on AC preparation process was manifested by SEM pictures as below. Taking 600 °C as an example, the SEM of XACs prepared by different waste residues at different impregnation ratio is shown in Fig. 5a. The pictures showed the impact of impregnation for different raw materials. It can be found from the SEM pictures that the pore structure of activated carbon prepared by these waste residues increases with the concentration of activator at 600 °C. However, when the concentration of activator continued to increase, excessive erosion of activated carbon would cause partial pore structure collapse.
Fig. 5

SEM of XACs on different impregnation ratio

The SEM of BACs prepared at different carbonization temperatures and impregnation ratios is shown in Fig. 5b. The influence of impregnation ratio was discussed at the condition of same material and different carbonization temperatures.

As for the impregnation ratio, the SEM pictures show clearly that an appropriate increase in temperature and impregnation ratio is conducive to the formation of pore structure, but an excessive temperature and impregnation ratio will lead to excessive erosion and pyrolysis of activated carbon structure.

The influence of carbonization temperature

In this part, adsorption capacity of methylene blue and AC yield of XACs at different carbonization temperatures is discussed when the impregnation ratio was at 1:0.5, 1:1 and 1:2.
  1. 1.

    The influence of carbonization temperature on AC yield.

     
As shown in Fig. 6, that LAC has a higher AC yield, followed by BAC, while PAC and RAC have a relatively close AC yield. The highest AC yield of all the samples was LAC which was prepared at 600 °C and 700 °C with an impregnation ratio of 1:0.5, reaching 58.4% and 60.9%. At 800 °C, the AC yield of LAC was 16.3% when the immersion ratio was 1:2, which was the lowest among the samples. The AC yield of RAC was also lower when the carbonization temperature was 800 °C, with the values of 25.9%, 24.4% and 24.2% at each immersion ratio.
Fig. 6

Influence of carbonization temperature on AC yield

It also can be seen from the figure, with the increase of carbonization temperature, the AC yield of XACs at each impregnation ratio showed a downward trend. When the carbonization temperature was from 600 to 700 °C, the temperature change had little effect on the AC yield, while the temperature reached 800 °C, the AC yield curve of all the impregnation ratio decreased significantly.

Dehydrogenation and deoxidation reaction of the raw material occurred under the action of activator zinc chloride, whose progress was related to temperature. With the continuous increase of carbonization temperature, the reactions in waste residues are strengthened and more components were degraded and lost, so the yield of activated carbon decreased. When the temperature reached 600 °C, most biodegradable components had been exhausted, so the AC yield would not continue to increase; therefore, the plateau area appeared above 600 °C which can be seen in the figure. When the temperature reached 800 °C, affected by the high temperature, the micropores and mesoporous holes in the waste residues melt and collapsed to form mesoporous holes. The debris formed by the collapse of the structure was removed in the washing stage, resulting in the weight reduction and AC yield of activated carbon.
  1. 2.

    The influence of carbonization temperature on adsorption capacity of methylene blue.

     
As shown in Fig. 7, PAC prepared at 600 °C with impregnation ratio of 1:2 had the highest adsorption capacity, and the value was 311.39 mg/g; LAC prepared at 600 °C with impregnation ratio of 1:0.5 had the lowest adsorption capacity. The influence of carbonization temperature on the adsorption capacity of methylene blue showed different phenomena among the XAC samples. The adsorption capacity of RAC and PAC on methylene blue decreased with the increase of temperature, while the adsorption capacity of BAC increased first and then decreased with the increase of temperature, and the adsorption capacity of LAC on methylene blue increased with the increase of temperature.
Fig. 7

Influence of carbonization temperature on adsorption capacity of methylene blue

In general, the higher the activation temperature was, the more complete the volatilization of the residual volatiles, the more developed the microporous structure, and the greater the specific surface area and adsorption activity were. Some samples such as LAC followed the above rules, that the increase of activation temperature promoted the formation of porous structure of activated carbon and the increase in adsorption of methylene blue.

However, due to the raw material of carbon skeleton and characteristics, also the influence of activator dosage, when carbonization temperatures raised further, the reactions of dehydrogenation and deoxidization occurred more fully which reacted between activator and waste residues such as PR and RR. And then ignition loss occured, which led to the collapses of pore structure and the broken-down part of the biomass. As a result, the specific surface area of activated carbon and the adsorption capacity of methylene blue were both decreased.
  1. 3.

    Analyzed by SEM.

     

The morphological structures of XACs were observed using a field-emission scanning electron microscope (SEM) (Nanosem 430, FEI, USA).

Carbonization temperature was regarded as an independent variable, whose influence on AC preparation process was manifested by SEM pictures as below. Taking impregnation ratio at 1:1 as an example, the SEM of XACs prepared by different waste residues at different carbonization is shown in Fig. 8. The pictures show the impact of carbonization temperature for different raw materials. It can be found that activated carbon BAC, RAC and PAC formed under activation at different temperatures had developed pore structures, and the porosity would be further enhanced with the increase of activation temperature. At a higher temperature of 800 °C, some holes would fuse together or the hole wall would collapse to form a larger hole or gap. However, LAC activated carbon was not very developed compared with the above three porous structures, so this kind of waste may not be suitable for preparing activated carbon under this condition. The SEM of BACs prepared at different carbonization temperatures and impregnation ratios is shown in Fig. 5b. The influence of carbonization temperature is discussed under the condition of same material and different impregnation ratio. It can be found from the electron microscope figure that the increase of activation temperature is indeed conducive to the formation of pore structure, but the further increase of temperature will result in the full thermal decomposition of cellulose and hemicellulose in biomass, which will lead to the collapse of pore skeleton. Therefore, the activation temperature should be controlled within an appropriate range.
Fig. 8

SEM of XACs on different carbonization temperature

SEM of XACs with different carbonization temperature with impregnation ratio at 1:1.

Conclusions

The activated carbon samples prepared by the raw material BR, PR, RR and LR are characterized by TG analysis, BET and SEM. TG analysis predicted that the AC yield sequence of 4 waste residues was RR > LR > PR > BR, while the experimental data after activation of zinc chloride did not follow this rule. This suggests that the activator has different effects on each waste residue. Nitrogen adsorption–desorption data and pore size distribution measured by BET all indicate that BAC, RAC and PAC samples have microporous and mesoporous structures and may have good adsorption performance which have been confirmed by experimental data of the adsorption capacity of methylene blue and SEM pictures. Therefore, BR, PR and RR are suitable for preparing activated carbon.

According to the data of the yield of AC and adsorption capacity of methylene blue, the suitable preparation conditions of the four XACs were analyzed from the aspects of impregnation ratio and carbonization temperature.

Due to its different structure and composition, the optimal conditions for the preparation of activated carbon from these waste residues have different characteristics.

For bagasse, the optimum preparation condition was 700 °C and the impregnation ratio was 1:1, the adsorption capacity of methylene blue reached 246.83 mg/g, AC yield was 40.98% of the moment.

For reed root residue, the optimum preparation condition was 600 °C and the impregnation ratio was 1:2, the adsorption capacity of methylene blue reached 268.07 mg/g, AC yield was 34.3% of the moment.

For Pueraria residue, the optimum preparation condition was 700 °C and the impregnation ratio was 1:2. The adsorption capacity of methylene blue reached 297.33 mg/g, AC yield was 34.1% of the moment.

In general, with the increase of carbonization temperature, the carbon yield of BAC, PAC and RAC decrease. BAC, PAC and RAC can achieve better carbon yield when the impregnation ratio is 1:1, but the impregnation ratio needs to be further increased to 1:2 to reach the maximum adsorption capacity of methylene blue.

Notes

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Copyright information

© Zhejiang University Press 2020

Authors and Affiliations

  1. 1.Key Lab for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and TechnologyTianjin UniversityTianjinChina
  2. 2.Department of Chemical EngineeringTianjin University Renai CollegeJinghai District, TianjinChina
  3. 3.National Engineering Research Center for Distillation TechnologyTianjinChina
  4. 4.Collaborative Innovation Center of Chemical Science and EngineeringTianjinChina

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