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Frontiers in Energy

ISSN 2095-1701

ISSN 2095-1698(Online)

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Front. Energy    2021, Vol. 15 Issue (1) : 159-169    https://doi.org/10.1007/s11708-020-0719-7
RESEARCH ARTICLE
Optimization of process parameters for preparation of powdered activated coke to achieve maximum SO2 adsorption using response surface methodology
Binxuan ZHOU1, Tao WANG1(), Tianming XU1, Cheng LI1, Yuan ZHAO1, Jiapeng FU1, Zhen ZHANG2, Zhanlong SONG1, Chunyuan MA1()
1. National Engineering Laboratory for Reducing Emissions from Coal Combustion, Engineering Research Center of Environmental Thermal Technology of the Ministry of Education, Shandong Key Laboratory of Energy Carbon Reduction and Resource Utilization, School of Energy and Power Engineering, Shandong University, Jinan 250061, China
2. School of Electric Power, North China University of Water Resources and Electric Power, Zhengzhou 450045, China
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Abstract

Powdered activated coke (PAC) is a good adsorbent of SO2, but its adsorption capacity is affected by many factors in the preparation process. To prepare the PAC with a high SO2 adsorption capacity using JJ-coal under flue gas atmosphere, six parameters (oxygen-coal equivalent ratio, reaction temperature, reaction time, O2 concentration, CO2 concentration, and H2O concentration) were screened and optimized using the response surface methodology (RSM). The results of factor screening experiment show that reaction temperature, O2 concentration, and H2O (g) concentration are the significant factors. Then, a quadratic polynomial regression model between the significant factors and SO2 adsorption capacity was established using the central composite design (CCD). The model optimization results indicate that when reaction temperature is 904.74°C, O2 concentration is 4.67%, H2O concentration is 27.98%, the PAC (PAC-OP) prepared had a higher SO2 adsorption capacity of 68.15 mg/g while its SO2 adsorption capacity from a validation experiment is 68.82 mg/g, and the error with the optimal value is 0.98%. Compared to two typical commercial activated cokes (ACs), PAC-OP has relatively more developed pore structures, and its SBET and Vtot are 349 m2/g and 0.1475 cm3/g, significantly higher than the 186 m2/g and 0.1041 cm3/g of AC1, and the 132 m2/g and 0.0768 cm3/g of AC2. Besides, it also has abundant oxygen-containing functional groups, its surface O content being 12.09%, higher than the 10.42% of AC1 and 10.49% of AC2. Inevitably, the SO2 adsorption capacity of PAC-OP is also significantly higher than that of both AC1 and AC2, which is 68.82 mg/g versus 32.53 mg/g and 24.79 mg/g, respectively.
Keywords powdered activated coke (PAC)      SO2 adsorption capacity      parameters optimization      response surface methodology     
Corresponding Author(s): Tao WANG,Chunyuan MA   
Online First Date: 04 January 2021    Issue Date: 19 March 2021
 Cite this article:   
Binxuan ZHOU,Tao WANG,Tianming XU, et al. Optimization of process parameters for preparation of powdered activated coke to achieve maximum SO2 adsorption using response surface methodology[J]. Front. Energy, 2021, 15(1): 159-169.
 URL:  
https://academic.hep.com.cn/fie/EN/10.1007/s11708-020-0719-7
https://academic.hep.com.cn/fie/EN/Y2021/V15/I1/159
Samples Proximate (wt.%, dry basis) Ultimate (wt.%, dry ash-free basis)
V A FC C H O N S
JJ-coal 36.40 9.86 53.74 81.83 5.04 11.56 1.10 0.48
Tab.1  Analysis of experimental materials
Fig.1  Experimental system for PAC preparation.
Fig.2  Flowchart of DOE.
Factors Symbol Ranges and levels
−1 +1
Oxygen to coal equivalent ratio (–) X1 0.1 0.3
Reaction temperature/°C X2 700 900
Reaction time/s X3 2 4
Oxygen concentration/% X4 2 6
Carbon dioxide concentration/% X5 4 12
Vapor concentration/% X6 5 20
Tab.2  Values and levels of factors in two-level factorial design
Run X1 (–) X2/°C X3/s X4/% X5/% X6/% S/(mg·g–1)
1 0.1 900 4 2 4 5 59.10
2 0.3 900 4 6 12 20 65.66
3 0.3 900 2 6 4 5 64.51
4 0.1 900 2 6 12 5 62.84
5 0.3 900 4 2 12 5 62.91
6 0.3 700 4 6 4 5 41.39
7 0.1 700 2 2 4 5 37.89
8 0.1 700 4 2 12 20 40.34
9 0.1 900 2 2 12 20 64.49
10 0.3 700 4 2 4 20 40.01
11 0.1 700 4 6 12 5 41.11
12 0.3 700 2 6 12 20 43.04
13 0.3 700 2 2 12 5 38.31
14 0.1 900 4 6 4 20 61.88
15 0.3 900 2 2 4 20 63.76
16 0.1 700 2 6 4 20 42.00
Tab.3  Experimental matrix and results for two-level factorial design
Fig.3  Pareto chart and main effect plots for response of SO2 adsorption capacity.
Fig.4  Central composite design (CCD) for three factors.
Significant factors Symbol Ranges and levels
–a (–1.68) –1 0 +1 +a ( +1.68)
Reaction temperature/°C Y1 732 800 900 1000 1068
Oxygen concentration/% Y2 2.64 4 6 8 9.36
Vapor concentration/% Y3 3.18 10 20 30 36.82
Tab.4  Values and levels of the significant factors used in CCD
Run Y1/°C Y2/% Y3/% S/(mg·g–1)
1 900 6 20 67.77
2 800 8 10 60.95
3 800 4 30 60.05
4 1000 8 10 48.80
5 800 8 30 54.10
6 900 6 36.82 63.49
7 1000 4 10 52.96
8 900 6 20 66.68
9 900 6 3.18 61.77
10 900 9.36 20 56.89
11 732 6 20 48.45
12 900 6 20 66.59
13 1068 6 20 42.69
14 800 4 10 52.72
15 900 2.64 20 62.07
16 1000 4 30 61.72
17 1000 8 30 50.38
Tab.5  Experimental matrix and results for CCD in RSM
Source P-value
Model <0.0001, significant
Y1 0.0009
Y2 0.0014
Y3 0.0149
Y1*Y2 0.001
Y1*Y3 0.0194
Y2*Y3 0.0003
Y1*Y1 <0.0001
Y2*Y2 0.0001
Y3*Y3 0.0028
Lack of fit 0.2165, not significant
R2 0.9892
Adequate precision 27.451
Tab.6  ANOVA for the model
Fig.5  Comparison of values predicted by S model and actual values.
Fig.6  Central composite design (CCD) for three factors.
Parameter or response Lower limit Upper limit Weight Importance Criteria Desirability
Reaction temperature/°C 800 1000 1 3 In range 1
Oxygen concentration/% 4 8 1 3 In range 1
Vapor concentration/% 10 30 1 3 In range 1
SO2 adsorption capacity/(mg·g–1) 50 70 1 3 Maximize 0.749
Tab.7  Optimization criteria and desirability for responses
Factors Experimental value Predicted value Error/%
Y1/°C 905 904.74 0.03
Y2/% 4.7 4.67 0.64
Y3/% 28 27.98 0.07
S/(mg·g–1) 68.82 68.15 0.98
Tab.8  Model optimization results versus experimental verification results
Fig.7  Pore structure analysis for three samples.
Sample SBET/(m2·g–1) Vtot/(cm3·g–1) Vmic/(cm3·g–1) Vmic<1 nm/(cm3·g–1) Vmic/Vtot Vmic<1 nm/Vmic
PAC-OP 349 0.1475 0.1124 0.0804 76.2% 71.5%
AC1 186 0.1041 0.0525 0.0369 50.4% 70.3%
AC2 132 0.0768 0.0356 0.0147 46.4% 41.3%
Tab.9  Pore structure parameters of three samples
Fig.8  Characterization of surface functional groups for three samples.
Fig.9  SO2 adsorption performance test of PAC-OP, AC1 and AC2.
Fig.10  SO2 adsorption capacities of PAC-OP, AC1, and AC2 versus regeneration number.
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