Kinetics and Mechanism Study of Mercury Adsorption by Activated

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Kinetics and Mechanism Study of Mercury Adsorption by Activated Carbon in Wet Oxy-fuel Conditions Hui Wang, Haotian Shen, Chang Shen, Ya-ning Li, Zhanfeng Ying, and Yufeng Duan Energy Fuels, Just Accepted Manuscript • DOI: 10.1021/acs.energyfuels.8b03610 • Publication Date (Web): 07 Jan 2019 Downloaded from http://pubs.acs.org on January 17, 2019

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Kinetics and Mechanism Study of Mercury Adsorption by Activated Carbon in Wet Oxy-fuel Conditions Hui Wang*, a, b, Haotian Shen a, Chang Shen c, Ya-ning Li b, Zhanfeng Ying a, Yufeng Duan*, b a

School of Energy and Power Engineering, Nanjing University of Science and

Technology, Nanjing, 210094, China. b

Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education,

Southeast University, Nanjing, 210096, China. c Tsien

Hsue-Shen College, Nanjing University of Science and Technology, Nanjing,

210094, China. KEYWORDS: Activated carbon; Wet oxy-fuel gas; Mercury; Kinetic model; Adsorption mechanism ABSTRACT: In this paper, four kinetic models including intraparticle diffusion, pseudofirst-order, pseudo-second-order, and Elovich kinetic model were applied to explore the internal mechanism of mercury adsorption by activated carbon in wet oxy-fuel conditions. Results indicated that pseudo-second-order model and Elovich kinetic model could accurately describe the adsorption process, which meant that chemical adsorption played an important role in the adsorption of mercury by activated carbon. Intraparticle diffusion S1 ACS Paragon Plus Environment

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model indicated that internal diffusion was not the only step to control the entire adsorption process and did not have an inhibition on mercury removal. Meantime, the external mass transfer process is more effective in controlling the mercury adsorption process of activated carbon according to the fitting result of pseudo-first-order model. The intra particle diffusion rate was improved with bed height as the results of kinetic parameters. In addition, the higher temperature inhibited the external mass transfer, which was not conducive to the adsorption of mercury by activated carbon in wet oxy-fuel conditions. 1. INTRODUCTION At present, the trend of global warming is further strengthened. Global warming is mainly related to the greenhouse effect while CO2 emissions are the main culprit of the greenhouse effect1. With the continuous development of global warming, the climatic environment is experiencing the great changes2. Considering the harm of global warming, it is urgent to take necessary measures to control CO2 emissions. In order to solve the problem of CO2 emissions from coal combustion, some researchers from the institutions in China had made outstanding contributions3-5. They developed many advanced combustion technologies to control CO2 emissions. Among them, oxy-fuel combustion technology has been considered as a technology with good application prospects6, 7. However, a study indicated that in an oxy-fuel combustion system, the high mercury content in flue gas may destroy CO2 processing unit, causing serious security problem8. Therefore, it is of necessity to pay attention to the harm of mercury to oxy-fuel combustion system and the pollution it brought. Moreover, it has been found that the mercury could also destroy the environment, doing serious harm to the human body through the biological chain9-12. Coal-fired plants is S2 ACS Paragon Plus Environment

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the largest source of release of mercury in the world13. The mercury migration and emission characteristics of coal combustion process were studied because of the serious mercury pollution14-16. As a result, mercury should be removed not only the safety issues of the oxy-fuel combustion system, but also the environmental issues. There are three forms of mercury in the combustion flue gas. Divalent mercury (Hg2+) and particle mercury (HgP) can be removed easily, while elemental mercury (Hg0) is hard to remove due to its insolubility and volatility17-19. Conversion of Hg0 into easily removed Hg2+ is the key to remove Hg0 from coal-fired flue gas20-24. At present, many researchers studied the control methods to remove the mercury in coal-fired flue gas and these methods include pollutant control devices25 and activated carbon injection technology26-28, and so on. It has been realized that activated carbon has good adsorption properties, which can effectively remove SOx, NOx and Hg29, 30 from flue gas. However, the mercury removal efficiency was not very good and lacked the guidance by internal mechanism. To handle the problem mentioned above, scientists turned their attention to adsorption kinetics and found it can describe adsorption process and predict adsorption rate and mechanism well31. There are many kinetic models for adsorption process, such as intraparticle diffusion model32 and pseudo-first-order model33 which are used to describe intraparticle diffusion and external mass transfer processes respectively. The pseudosecond-order model34 based on Langmuir adsorption isotherm equation, and the Elovich model based on the Temkin adsorption isotherm equation35 can both be used to describe chemical adsorption process. These four kinetic models were based on the kinetic theory, S3 ACS Paragon Plus Environment

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and could reflect the physical and chemical adsorption processes, and therefore widely used in kinetic analysis of adsorbent adsorption process. Many researchers have successfully explained the adsorption mechanism by using the kinetic models36, 37. Skodras G et al.38 used pseudo-first-order model, pseudo-second-order model and Elovich kinetic model to study the adsorption kinetics of mercury on activated carbon surface and found that the pseudo-second-order model fitted the results more accurately. Q Zhou et al.39 used four simplified adsorption kinetic models to study the influence of mercury removal performance of activated carbon under different flue gas components and adsorption temperature. L Zhong40 did some experiments under different experiment conditions and results indicated that the pseudo-second-model was the best model which fitted to the actual mercury adsorption behavior on AC-I 2 sorbent. Our recent paper41 studied the mercury adsorption by activated carbon in wet oxy-fuel conditions in a fixed-bed reactor which was shown in Figure 1. The related experimental results showed that the high bed height had a more positive effect on the mercury removal and low temperature (around 150 oC-200 oC) could largely enhance the chemical adsorption and the adsorption species and mechanism of different temperatures varied. Besides, Figure S1 and Figure S2 in Supporting Information showed the related experimental results. Moreover, the experimental parameters and sorbent characteristic (Table S1) were also shown in Supporting Information. However, the study of mechanism under different operating parameters was still lacking such as bed height, temperature and so on. In this paper, the kinetic process of mercury adsorption by activated carbon in oxy-fuel conditions was analyzed by using four kinetic models mentioned above from two perspectives, which were bed height and S4 ACS Paragon Plus Environment

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reaction temperature. The internal mechanism would be revealed, which can provide a theoretical reference and internal mechanism for the study of the transformation of mercury in the environment and the application of activated carbon in the treatment of coal-fired fuel gas. 2. COMPUTATIONAL MODELS AND PARAMETERS 2.1. Intraparticle Diffusion Model. Intraparticle diffusion model is commonly used to describe the internal diffusion process of pores during solid adsorption. The model considers the diffusion effect by using a partial differential equation describing the diffusion of spherical particles. The equation is expressed as followed:

qt  k p t

1

2

C

(1)

Where qt is the cumulative mercury adsorption per unit mass adsorbent, g/g; k p is the intraparticle diffusion rate constant, g/(gmin1/2); t is the reaction time, min; C is a constant related to the thickness of the boundary layer which represents the extent of the boundary layer effect, g/g. 2.2. Pseudo-first-order Kinetic Model. The pseudo-first-order model uses the concentration difference as the driving force to describe the mass transfer process. If the experimental data and the calculated data could agree well, then, we could reach the conclusion that the external mass transfer had an obvious control effect on adsorption process38. Pseudo-first-order kinetic equation is shown in Eq. (2) 39:

dqt  k1 ( qe  qt ) dt

(2)

Integrated by the boundary condition t=0, qt =0; t=t, qt=qt, the Eq. (4) is transformed to:

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qt  qe (1  e  k1t )

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(3)

Where qe is equilibrium adsorption capacity, g/g; k1 is the pseudo-first-order adsorption rate constant, min-1. 2.3. Pseudo-second-order Kinetic Model. The pseudo-second-order model, which is based on Langmuir adsorption isotherm equation, contains all processes of adsorption including external mass transfer, intraparticle diffusion, and surface adsorption. Among them, the formation of chemical bonds is the main factor affecting the pseudo-second-order kinetic adsorption. So it is used as the control step of the adsorption rate43. The equation is shown in Eq.(4):

dqt  k2 ( qe  qt ) 2 dt

(4)

While boundary conditions are t = 0, qt = 0; t=t, qt= qt,

q  qe 

qe  k2  t 1  qe  k2  t

(5)

Where, qe is the equilibrium absorbed amount, μg/g; q is the equilibrium absorbed amount at time t, μg/g; t is the absorbed time t, min; k2 is the kinetic constant of pseudo-secondorder kinetic equation, g/ (μg·min). 2.4. Elovich Kinetic Model. The Elovich kinetic model, which is based on the Temkin adsorption isotherm equation, is mainly used to describe the chemical adsorption process of gas on solid surface. The equation of the model can be expressed as Eq. (6):

dqt  ae  bqt dt

(6)

While boundary conditions were t = 0, qt = 0; t=t, qt= qt,

qt 

ln(t  t0 ) ln t0  b b

(7) S6

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Where a is the initial adsorption rate, g/ (gmin); b is a constant related to surface coverage and activation energy, g/g; t0=1/ (ab). 3. RESULTS AND DISCUSSION Four kinetic models were adopted to analyze the mechanism of mercury adsorption by activated carbon in wet oxy-fuel conditions. The error between the fitting result and the experiment data was evaluated by a correlation coefficient R2. The larger the R2 was, the closer the model was fitted to the description of the adsorption process. When the bed height was studied, the temperature kept invariable and was set at 150oC, and when the temperature was studied, the bed height kept invariable and was set at 3.5mm. 3.1. Kinetic Analysis of Mercury Adsorption by Activated Carbon with Intraparticle Diffusion Model. Figure 2 and Figure 3 showed the fitting results of the intraparticle diffusion model for different bed heights and different adsorption temperatures. Table 1 showed the parameters and correlation coefficient obtained by fitting the intraparticle diffusion equation. In Figure 2, it could be seen that no matter the bed height was 2 mm or 3.5 mm even 5 mm, the fitting curve were not consistent with experimental data well. Meanwhile, the curves did not pass through the origin, which indicated that internal diffusion was not the only step to control the entire adsorption process. In Table 1, the kp of different bed heights ranged from 25.4976 to 26.3889, which meant the adsorption rate, remained the similar level, indicating that internal diffusion did not have an inhibition on mercury removal. In addition, R2 were almost below 0.95 did not show a significant correlation with bed height. It summarized that the internal diffusion was not the only step to control the entire adsorption process.


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In Figure 3, the fitting curves of 150 oC and 250 oC were all not consistent well with the experimental results. As to the temperature of 350 oC and 450 oC, it can be seen in Table 1 that the kp showed a downward trend with the increase of temperature due to the function of intraparticle diffusion of mercury in sorbent was decreased with temperature increased. Moreover, according to the research from Rumayor M44,

45,

the following

reactions might affect the kinetic parameters due to the different reaction temperature, as shown in the following reactions R1-R3. Hg 2SO4 (s)  HgSO4 (s)  Hg(s)

R1

3HgSO 4 (s)  HgSO 4  2HgO(s)+2SO 2 (g)+O 2 (g)

R2

HgSO 4  2HgO(s)  3Hg(g)+SO 2 (g)+2O 2 (g)

R3

Therefore, it can be summarized that the adsorption rate was very fast in the initial stage of adsorption, which indicated that surface adsorption occurred in the initial stage of adsorption. With the reaction proceeding, kp increased continuously, and the adsorption rate remained high, indicating that internal diffusion has no restrictive effect. The adsorption of mercury was mainly divided into two stages, which were surface adsorption and internal diffusion adsorption. The initial adsorption stage was surface adsorption and active center of the activated carbon surface made the adsorption rate fast46. When surface active sites were occupied, the adsorption entered the second stage that was the diffusion adsorption in the pore. 3.2. Kinetic Analysis of Mercury Adsorption by Activated Carbon with Pseudo-firstorder Kinetic Model. Figure 4 and Figure 5 showed the fitting curves of different bed heights and adsorption temperatures by pseudo-first-model. Table 2 showed the parameters and correlation coefficient obtained by pseudo-first-model. It could be seen from Figure 4 that no matter what height of the bed was, the fitting results were consistent well with the S8 ACS Paragon Plus Environment

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experiment results. That meant that the pseudo-first-model could describe the adsorption process well, and indicating the external mass transfer process is more effective in controlling the mercury adsorption process of activated carbon. In Table 2, it can be seen that the parameter value of R2 were all above 0.99 which agreed with the experimental results. With the bed height increasing, the k1 ranged from 2.70E-05 to 2.76E-05 and the R2 ranged from 0.99789 to 0.99807. The changes of k1 and R2 in bed height were not obviously which meant that the change of bed height had little effect on external mass transfer. As shown in Figure 5, it could be seen that the fitting curves were also fitted well with the experiment results, which meant that the pseudo-first-model could describe the adsorption process well. The parameter value of mercury uptake increased with the adsorption certain time except that the temperature of 350 oC and 450 oC due to higher temperature. Different with the change of bed height, the change of temperature had an obvious effect on adsorption process. From Table 2, it can be seen that the k1 ranged from 3.46E-05 to 1.49E-03 while R2 ranged from 0.99881 to 0.98899, which meant a good prediction of the pseudo-first-model to the experimental data. Moreover, with the increase of temperature, the correlation coefficient R2 kept decreasing, which indicated that the external mass transfer process had a weakening effect on the adsorption process. Moreover, the fluctuation of k1 was quite large, indicating the temperature change had a great influence on the external mass transfer process, which was consistent with the experimental results mentioned above. 3.3. Kinetic Analysis of Mercury Adsorption by Activated Carbon with Pseudosecond-order Kinetic Model. Figure 6 and Figure 7 showed the fitting curve of different S9 ACS Paragon Plus Environment

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bed heights and temperatures by pseudo-second-model. Table 3 showed the parameters and correlation coefficient obtained by pseudo-second-model. In Figure 6, according to bed height, the fitting cures were all fitted well with the experiment data, which indicated that the pseudo-second-model could be used to describe adsorption process, indicating that chemisorption was dominant in the adsorption. In Table 3, it could be seen that R2 was higher than 0.989, which revealed that the pseudo-second-order model could predicted the experimental results well in these conditions. Moreover, qe and k2 increased with the bed height increased as shown in Table 3. In Fugue 7, the fitting curves of different temperatures by pseudo-second-model were all fitted well with the experiment data, which meant that the pseudo-second-model could be used to describe the adsorption process. In Table 3, when the temperature was 150 oC, the qe and k2 were the largest. Besides, the correlation coefficient of each working condition was relatively high which above 0.99 except for that at 450 oC (0.98903). The correlation coefficient was very similar to that of external mass transfer, which was fitted by pseudofirst-model, and it could be summarized that the process of mass transfer could not be ignored while considering chemical adsorption. 3.4. Kinetic Analysis of Mercury Adsorption by Activated Carbon with Elovich Model. Figure 8 and Figure 9 showed the fitting curves of different bed heights and temperatures by Elovich model. Table 4 showed the parameters and correlation coefficient obtained by Elovich model. In Figure 8, it could be seen that the fitting curves were consistent well with the experiment results. It meant that the Elovich model could be used to describe the adsorption process, confirming the conclusion that chemisorption rate and external mass transfer could control mercury adsorption process. From Table 4, the R2 were S10 ACS Paragon Plus Environment

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all very high which were both above 0.99 which agreed with the experimental results, and among them, when the bed height was 3.5 mm, the value of b were the largest, which meant the bed height could influenced the activation energy of mercury on the surface of activated carbon. In Figure 9, the fitting curves of different temperatures by Elovich model were still consistent well with experiment data. With time passed by, the mercury uptake maintained increased while the growth rate of that at 350 oC and 450 oC were not obvious due to higher temperatures destroyed the activity of activated carbon. The above phenomenon could be attributed to the higher temperature lower some thermodynamic parameters such as activation energy and free energy47,

48.

In Table 4, the higher R2 in the factors of

temperature represented a good prediction by the Elovich model with experimental results. b was the lowest at 450 oC, which meant that at that temperature, the surface adsorption ability was weak due to the higher temperature. Therefore, it could be summarized that the activation energy of mercury on the surface of activated carbon had a close relation with adsorption temperature. 4. CONCLUSION In this paper, four kinetic models including intraparticle diffusion model, pseudo-firstorder model, pseudo-second-order model, and Elovich model were adopted to analyze the mechanism of mercury adsorption by activated carbon in wet oxy-fuel conditions. Results showed that internal diffusion was not the only step. The fitting results of pseudo-secondorder model and the Elovich kinetic model indicated that chemical adsorption dominated the mercury adsorption by activated carbon while external mass transfer could not be ignored obtained by pseudo-first-order model. S11 ACS Paragon Plus Environment

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According to the obtained kinetic parameters, the intra particle diffusion rate, and the pseudo-first-order adsorption rate were improved with the bed height increased, which promoted the internal diffusion, the external mass transfer, and the chemisorption process. Moreover, the intra particle diffusion rate, the pseudo-first-order adsorption rate, and the pseudo-second-order adsorption rate were significantly reduced with increasing temperature, inhibiting the intra particle diffusion and the external mass transfer, which was not conducive to the adsorption. AUTHOR INFORMATION Corresponding Author *E-mail: [email protected]. Tel/Fax: +86-25-84314965. *E-mail: [email protected]. Tel/Fax: +86-25-83795652. NOTES The authors declare no competing financial interest. ACKNOWLEDGMENT This work was supported by the National Natural Science Foundation of China (51706104, 51876039); the Natural Science Foundation of Jiangsu Province (Grant No. BK20170849); the Peak of the Six Talents Program of Jiangsu Province (XNY-026) and the Fundamental Research Funds for the Central Universities (No.30916011334). REFERENCES (1). Birat, J. P.; Vizioz, J. P., CO2 Emissions and the Steel Industry's available Responses to the Greenhouse Effect. Revue De Metallurgie 2017. (2). Cook, J.; Oreskes, N.; Doran, P. T.; Anderegg, W. R. L.; Verheggen, B.; Maibach, E. W.; Carlton, J. S.; Lewandowsky, S.; Skuce, A. G.; Green, S. A., Consensus on consensus: S12 ACS Paragon Plus Environment

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Lagergren, S. In About the theory of so-called adsorption of solution substances,

1998; 1998. (34).

Yuhshan, H., Citation review of Lagergren kinetic rate equation on adsorption

reactions. Scientometrics 2004, 59, (1), 171-177. (35).

Zuorro, A.; Maffei, G.; Lavecchia, R., Kinetic modeling of azo dye adsorption on

non-living cells of Nannochloropsis oceanica. Journal of Environmental Chemical Engineering 2017, 5, (4). (36).

Wang, H.; Wang, S.; Duan, Y.; Li, Y.-n.; Xue, Y.; Ying, Z., Activated Carbon for S16 ACS Paragon Plus Environment

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Energy & Fuels

Capturing Hg in Flue Gas under O2/CO2 Combustion Conditions. Part 1: Experimental and Kinetic Study. Energ Fuel 2018, 32, (2), 1900-1906. (37).

Wang, H.; Wang, S.; Duan, Y.; Li, Y.-n.; Ying, Z., Activated Carbon for

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Skodras, G.; Diamantopoulou, I.; Pantoleontos, G.; Sakellaropoulos, G. P.,

Kinetic studies of elemental mercury adsorption in activated carbon fixed bed reactor. Journal of Hazardous Materials 2008, 158, (1), 1-13. (39).

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Carbon Adsorption for Mercury Removal. Proceedings of the Csee 2013, 33, (29), 10-17. (40).

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mercury adsorption in activated carbon modified by iodine steam vapor deposition method. Fuel 2017, 188, 343-351. (41).

Wang, H.; Shen, C.; Duan, Y.; Ying, Z.; Li, Y.-n., Synergistic Effect between H2O

and SO2 on Mercury Removal by Activated Carbon in O2/CO2 Conditions. Journal of Chemical Technology & Biotechnology 2018, DOI:10.1002/jctb.5866. (42).

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Page 19 of 31 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Energy & Fuels

T

Heater Heater Control

Gas Mixer Hg Sorbent

Hg

Gas Analyzer

Valve MFC Water Btah

Activated Carbon

Hg Analyzer

Figure 1. Schematic diagram of a fixed-bed reactor system.


Energy & Fuels

(a) 250

2.0 mm 3.5 mm 5.0 mm Calculated

200

Mercury Uptake (g/g)


250

150 100 50 0

0

2

4

1/2

6

1/2

8

10

B B C C D D

100 50

0

(a) 250

(a) 250


3.5 mm Calculated

200 150 100 50 0

Model Equation Reduced Chi-Sqr Adj. R-Square

150

0

12

2.0 mm Calculated

200

t (min )


1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 20 of 31

0

20

40

60

80

Time (min)

100

120

20

40

60

80

Time (min)

100

120

5.0 mm Calculated

200

Model Equation Reduced Chi-Sqr 150 Adj. R-Square


B 100 B C C 50 D D

B B C C D D

0

0

20

40

60

80

Time (min)

100

120

Figure 2. Kinetic analysis of mercury adsorption on activated carbon surface by intraparticle diffusion mode at different bed heights.


Page 21 of 31


250

(a) 250

o

150 C o 250 C o 350 C o 450 C Calculated

200 150 100 50 0

0

2

4

150 100 50 0

0

2

6

1/2

8

10

(b) 250

o

150 C o 250 C o 350 C Calculated

200

1/2

t (min )



1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Energy & Fuels

4

1/2

6

1/2

t (min )

8

10

12

12

o

450 C Calculated

200 150 100 50 0

0

2

4

1/2

6

1/2

t (min )

8

10

12

Figure 3. Kinetic analysis of mercury adsorption on activated carbon surface by intraparticle diffusion model at different adsorption temperatures.


Energy & Fuels

(a) 250

200



150 100 50 0

0

(a) 250

20

40

60

80

Time (min)

100

150 100 50

0

20

40

200


B 100 B C C 50 D D

B B C C D D

0

(a) 250

3.5 mm Calculated

200

0

2.0 mm Calculated


0

120



250


1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 22 of 31

60

80

Time (min)

100

120

20

40

60

80

Time (min)

100

120

5.0 mm Calculated

200



B 100 B C C 50 D D

B B C C D D

0

0

20

40

60

80

Time (min)

100

120

Figure 4. Kinetic analysis of mercury adsorption on activated carbon surface by pseudofirst-order kinetic model at different bed heights.


Page 23 of 31


250

(a) 250

o


200 150

B B C C D D E E

50

0

20

40

60

(b) 250


B B C C D D E E

100 50

20

40

60

80

Time (min)

100

120

100

120

o

Model Equation 200 Reduced ChiAdj. R-Square

150

0

80

Time (min)

o


200

0

Model Equation Reduced ChiAdj. R-Square

100

0


1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Energy & Fuels

450 C Calculated

Model Equation Reduced ChiAdj. R-Square

150

B B C C D D E E

100 50 0

0

20

40

60

80

Time (min)

100

120

Figure 5. Kinetic analysis of mercury adsorption on activated carbon surface by pseudofirst-order kinetic model at different adsorption temperatures.


Energy & Fuels

(a) 250

Model

Model

Equation


200

Adj. R-Square

150

200

Reduced Chi-Sqr Adj. R-Square

50mg AC+250 50mg AC+250mg SiO2


Model

Model

Equation

Reduced Chi-Sqr

100

Equation

2.0 mm Calculated

Reduced Chi-Sqr



250

150

Equation Reduced Chi-Sqr

Adj. R-Square

Adj. R-Square



Model

Model

100

Equation

Equation

50 0

50

Reduced Chi-Sqr

0

20

40

60

80

Time (min)

100

Reduced Chi-Sqr

Adj. R-Square

Adj. R-Square



120

(b) 250

0

0

20

40

60

80

Time (min)

100

120

(a) 250

Model

200

Model

Equation

3.5 mm Calculated

Adj. R-Square

150

200




Model

Model

Equation

Reduced Chi-Sqr

100

Equation

5.0 mm Calculated

Reduced Chi-Sqr



1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 24 of 31

150

Equation Reduced Chi-Sqr

Adj. R-Square

Adj. R-Square



Model

Model

100

Equation

Equation

50 0

Reduced Chi-Sqr

50


Adj. R-Square 50mg AC+750 50mg AC+750mg SiO2

0

20

40

60

80

Time (min)

100

120

0


0

20

40

60

80

Time (min)

100

120

Figure 6. Kinetic analysis of mercury adsorption on activated carbon surface by pseudo second order kinetic model at different bed heights.


Page 25 of 31

Model


250

Equation

o


200 150

Reduced Chi-Sqr Adj. R-Square 150 ℃ 150 ℃ Model Equation Reduced Chi-Sqr Adj. R-Square 250 ℃ 250 ℃

100


50

350℃ 350℃ Model

0

Equation

0

20

40

60

80

100

Reduced Chi-Sqr

120

Adj. R-Square

Time (min)

450 ℃ 450 ℃

Model

Model

(a) 250

(b) 250

Equation

o


200

Adj. R-Square 150 ℃ 150 ℃

Equation

o

450 C Calculated

Reduced Chi-Sqr



1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Energy & Fuels


200

150 ℃ 150 ℃

Model

Model

Equation

150

Reduced Chi-Sqr

Equation

150

Reduced Chi-Sqr

100

Model

Adj. R-Square

Adj. R-Square

250 ℃

250 ℃

250 ℃

100

Model

250 ℃

Equation

Equation

Reduced Chi-Sqr

50

Reduced Chi-Sqr

Adj. R-Square

Adj. R-Square

350℃

350℃

50

350℃

350℃

Model

0

Equation

0

20

40

60

80

Time (min)

100

120


Model

0

Equation

0

20

450 ℃ 450 ℃

40

60

80

Time (min)

100

120

Adj. R-Square 450 ℃ 450 ℃

Figure 7. Kinetic analysis of mercury adsorption on activated carbon surface by pseudo second order kinetic model at different adsorption temperatures.


Reduced Chi-Sqr

Energy & Fuels

(a) 250

200



150 100 50 0

0

(b) 250

20

40

60

80

Time (min)

100

150 100 50

0

20

40

150 100 50

0

(c) 250

3.5 mm Calculated

200

0

2.0 mm Calculated

200

0

120



250


1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 26 of 31

60

80

Time (min)

100

120

20

40

60

80

100

120

60

80

100

120

Time (min)

5.0 mm Calculated

200 150 100 50 0

0

20

40

Time (min)

Figure 8. Kinetic analysis of mercury adsorption on activated carbon surface by Elovich kinetic model at different bed heights.


Page 27 of 31


250

(a) 250

o


200 150 100 50 0

0

20

40

150 100 50 0

0

20

40

80

100

(b) 250

o


200

60

Time (min)



1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Energy & Fuels

60

80

Time (min)

100

120

120

o

450 C Calculated

200 150 100 50 0

0

20

40

60

80

Time (min)

100

120

Figure 9. Kinetic analysis of mercury adsorption on activated carbon surface by Elovich kinetic model at different adsorption temperatures.


Energy & Fuels 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 28 of 31

Table 1. The Parameters and Correlation Coefficient Obtained from Intraparticle Diffusion Model. Factors

Value

kp[g/(gmin1/2)]

C(g/g)

R2

2

25.4976

-71.2712

0.94129

3.5

25.7452

-70.6607

0.94377

5

26.3889

-73.2492

0.94047

150

25.7452

-70.6607

0.94377

250

11.3308

-33.1605

0.93754

350

1.2470

-2.2776

0.98285

450

0.9902

-2.2961

0.94948

Bed Height (mm)

Adsorption Temperature (oC)


Page 29 of 31 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Energy & Fuels

Table 2. The Parameters and Correlation Coefficient Obtained from Pseudo-firstorder Kinetic Model. Factors

Value

qe(g/g)

k1(min-1)

R2

2

7.13E04

2.70E-05

0.99789

3.5

5.67E04

3.46E-05

0.99881

5

7.25E04

2.76E-05

0.99807

150

5.67E04

3.46E-05

0.99881

250

4.34E04

1.93E-05

0.99458

350

19.3745

7.76 E-03

0.99530

450

57.7188

1.49 E-03

0.98899

Bed Height (mm)



Energy & Fuels 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 30 of 31

Table 3. The Parameters and Correlation Coefficient Obtained from Pseudo-secondorder Kinetic Model. qe Factors

k2 R2

Value (g/g)

g/(μg•min)

2

6.47E04

1.9256

0.99794

3.5

6.97E04

1.9598

0.99886

5

8.78E04

1.9995

0.99812

150

5.48E04

1.9598

0.99886

250

4.12E04

0.8376

0.99463

350

30.6751

0.1552

0.99595

450

107.6453

0.0863

0.98903

Bed Height (mm)



Page 31 of 31 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Energy & Fuels

Table 4. The Parameters and Correlation Coefficient Obtained from Elovich Model. Factors

Value

a(g/(gmin))

b(g/g)

R2

2

1.9280

1.46E-05

0.99788

3.5

1.9630

1.84E-05

0.99881

5

2.0021

1.44E-05

0.99807

150

1.9630

1.84E-05

0.99881

250

0.8383

2.19E-05

0.99458

350

0.1609

7.78E-02

0.99654

450

0.08666

2.02E-02

0.98908

Bed Height (mm)



Kinetics and Mechanism Study of Mercury Adsorption by Activated

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