A DFT study on the adsorption of various mercury species in the coal combustion flue gases on the Mo-doped Fe<sub>3</sub>O<sub>4</sub>(111) surface

CHEN Jia-min; ZHOU Chang-song; YANG Hong-min; WU Hao

Volume 48 Issue 5

May 2020

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2020 > 48(5): 525-532

CHEN Jia-min, ZHOU Chang-song, YANG Hong-min, WU Hao. A DFT study on the adsorption of various mercury species in the coal combustion flue gases on the Mo-doped Fe3O4(111) surface[J]. Journal of Fuel Chemistry and Technology, 2020, 48(5): 525-532.

Citation:

CHEN Jia-min, ZHOU Chang-song, YANG Hong-min, WU Hao. A DFT study on the adsorption of various mercury species in the coal combustion flue gases on the Mo-doped Fe₃O₄(111) surface[J]. Journal of Fuel Chemistry and Technology, 2020, 48(5): 525-532.

Citation:

PDF( 6078 KB)

A DFT study on the adsorption of various mercury species in the coal combustion flue gases on the Mo-doped Fe₃O₄(111) surface

School of Energy&Mechanical Engineering, Nanjing Normal University, Nanjing 210042, China

Funds:

the National Natural Science Foundation of China 51676101

the National Natural Science Foundation of China 51806107

the Natural Science Foundation of Jiangsu Province BK20161558

the Natural Science Foundation of Jiangsu Province BK20180731

More Information

Corresponding author: ZHOU Chang-song, E-mail:cszhou@njnu.edu.cn
Received Date: 2020-01-19
Rev Recd Date: 2020-03-16

Available Online: 2021-01-23

Publish Date: 2020-05-10

Abstract

Abstract

The adsorption characteristics of Hg⁰, HgCl and HgCl₂ on the Mo-doped Fe₃O₄ (111) Fe_tet surface were investigated by density functional theory (DFT) calculation with the CASTEP software package. The results indicate that both HgCl and HgCl₂ are chemically adsorbed on the Mo-doped Fe₃O₄ (111) Fe_tet surface, whereas Hg⁰ is bound to the surface by physisorption. The binding energies of HgCl on the Mo-doped Fe₃O₄ (111) Fe_tet surface is about 40%-66% higher than that on the pure Fe₃O₄ (111) Fe_tet surface. For the adsorption of HgCl₂ molecule on the pure Fe₃O₄ (111) Fe_tet surface, two Cl atoms interact with one Mo atom and one Fe atom, forming the "M" structure; in contrast, on the Mo-doped Fe₃O₄ (111) Fe_tet surface, the stronger interaction between Cl atom and Mo atom allows a complete dissociation of HgCl₂ and release of Hg. The adsorption mechanism of mercury species on the Mo-doped Fe₃O₄ (111) Fe_tet surface revealed in this work may be helpful for the practical removal of mercury from coal-fired flue gases.
- mercury,
- density functional theory,
- Mo doped,
- Fe₃O₄(111) surface,
- adsorption

FullText(HTML)

References(36)

References

[1]	中国统计年鉴[M].北京: 中国统计出版社, 2009. Statistical Yearbook of China[M]. Beijing: China Statistics Press, 2009
[2]	ZHENG Y, JENSEN A D, WINDELIN C, JENSEN F. Review of technologies for mercury removal from flue gas from cement production processes[J]. Prog Energy Combust, 2012, 38(5):599-629. doi: 10.1016/j.pecs.2012.05.001
[3]	CARPI A. Mercury from combustion sources:A review of the chemical species emitted and their transport in the atmosphere[J]. Water Air Soil Poll, 1997, 98(3/4):241-254. doi: 10.1023/A:1026429911010
[4]	YANG Y, LIU J, WANG Z, ZHANG Z. Homogeneous and heterogeneous reaction mechanisms and kinetics of mercury oxidation in coal-fired flue gas with bromine addition[J]. Proc Combust Inst, 2016, 36(3):4039-4049. doi: 10.1016/j.proci.2016.08.068
[5]	ZHANG B K, LIU J, ZHENG C G, CHANG M. Theoretical study of mercury species adsorption mechanism on MnO₂(110) surface[J]. Chem Eng J, 2014, 256:93-100. doi: 10.1016/j.cej.2014.07.008
[6]	GALBREATH K C, ZYGARLICKE C J. Mercury speciation in coal combustion andgasfication flue gases[J]. Environ Sci Technol, 1996, 30(8):2421-2426. doi: 10.1021/es950935t
[7]	WHO (World Health Organization). Preventing Disease through Healthy Environment: Exposure to Mercury: A Major Public Health Concern[R]. Geneva, Switzerland, WHO, 2007.https://www.who.int/ipcs/features/mercury.pdf
[8]	SJOSTROM S, DURHAM M, BUSTARD C J, MARTIN C. Activated carbon injection for mercury control:overview[J]. Fuel, 2010, 89(6):1320-1322. doi: 10.1016/j.fuel.2009.11.016
[9]	YANG H, XU Z, FAN M, BLAND A E, JUDKINS R R. Adsorbents for capturing mercury in coal-fired boiler flue gas[J]. J Hazard Mater, 2017, 146(1/2):1-11. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=f0cd45182e099bdc9fa4f37ea20e7604
[10]	WANG P, HU S, XIANG J, SU S, SUN L, CAO F, XIAO X, ZHANG A. Analysis of mercury species over CuO-MnO₂-Fe₂O₃/γ-Al₂O₃ catalysts by thermal desorption[J]. Proc Combust Inst, 2015, 35(3):2847-2853. doi: 10.1016/j.proci.2014.06.054
[11]	ZHANG A, ZHENG W, SONG J, HU S, LIU Z, XIANG J. Cobalt manganese oxides modified titania catalysts for oxidation of elemental mercury at low flue gas temperature[J]. Chem Eng J, 2014, 236:29-38. doi: 10.1016/j.cej.2013.09.060
[12]	ZHOU C S, SUN L S, XIANG J, HU S, SU S, ZHAO A C. The experimental and mechanism study of novel heterogeneous Fenton-like reactions using Fe_3-xTi_xO₄ catalysts for Hg⁰ absorption[J]. Proc Combust Inst, 2015, 35(3):2875-2882. doi: 10.1016/j.proci.2014.06.049
[13]	ZHOU C S, SUN L S, ZHANG A C, WU X F, MA C, SU S, HU S, XIANG J. Fe_3-xCu_xO₄ as highly active heterogeneous Fenton-like catalysts towards elemental mercury removal[J]. Chemosphere, 2015, 125:16-24. doi: 10.1016/j.chemosphere.2014.12.082
[14]	LI H L, FENG S H, YANG Z Q, YANG J P, LIU S J, HU Y C, ZHONG L, QU W Q. Density functional theory study of mercury adsorption on CuS surface:Effect of typical flue gas components[J]. Energy Fuels, 2019, 33(2):1540-1546. doi: 10.1021/acs.energyfuels.8b03585
[15]	ZHAO H T, MU X L, YANG G, GEORGE M. Graphene-like MoS₂ containing adsorbents for Hg⁰ capture at coal-fired power plants[J]. Appl Energy, 2017, 207:254-264. doi: 10.1016/j.apenergy.2017.05.172
[16]	WANG Z, LIU J, YANG Y J, LIU F, DING J Y. Heterogeneous reaction mechanism of elemental mercury oxidation by oxygen species over MnO₂ catalyst[J]. Proc Combust Inst, 2019, 37(3):2967-2975. doi: 10.1016/j.proci.2018.06.132
[17]	杨涛, 温晓东, 任君, 李永旺, 王建国, 霍春芳. Fe₃O₄(111), (110)和(001)表面结构的密度泛函理论研究[J].燃料化学学报, 2010, 38(1):121-128. doi: 10.3969/j.issn.0253-2409.2010.01.022 YANG Tao, WEN Xiao-dong, REN Jun, LI Yong-wang, WANG Jian-guo, HUO Chun-fang. Surface structures of Fe₃0₄(111), (110), and (001):A density functional theory study[J]. J Fuel Chem Technol, 2010, 38(1):121-128. doi: 10.3969/j.issn.0253-2409.2010.01.022
[18]	YANG T, WEN X D, HUO C F, LI Y W, WANG J G, JIAO H J. Structure and energetics of hydrogen adsorption on Fe₃O₄(111)[J]. J Mol Catal A Chem, 2009, 302(1):129-136. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=802ff593ce32abc1bbba8631d8eda968
[19]	YU X H, HUO C F, LI Y W, WANG J G, JIAO H J. Fe₃O₄ surface electronic structures and stability from GGA+U[J]. Surf Sci, 2012, 606(9/10):872-879. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=34643c0cf308a81e5cffecc3d2d84e43
[20]	赵中霞, 任韧, 任奕璟, 周志立.过渡元素掺杂Fe₃O₄(001)表面磁电性能的理论研究[J].无机化学学报, 2017, 33(6):923-931. http://d.old.wanfangdata.com.cn/Periodical/wjhxxb201706002 ZHAO Zhong-xia, REN Ren, REN Yi-jing, ZHOU Zhi-li. Theoretical study of the magnetic and electric properties of transition elements doped Fe₃O₄(001) surface[J]. Chin J Inorg Chem, 2017, 33(6):923-931. http://d.old.wanfangdata.com.cn/Periodical/wjhxxb201706002
[21]	FU Z M, YANG B W, ZHANG Y, ZHANG N, YANG Z X. Dopant segregation and CO adsorption on doped Fe₃O₄(111) surfaces:A first principle study[J]. J Catal, 2108, 364:291-296. doi: 10.1016/j.jcat.2018.05.027
[22]	FU Z M, WANG J Q, ZHANG N, AN Y P, YANG Z X. Effect of Cu doping on the catalytic activity of Fe₃O₄ in water-gas shift reactions[J]. Int J Hydrogen Energy, 2015, 40(5):2193-2198. doi: 10.1016/j.ijhydene.2014.12.063
[23]	XUE P Y, FU Z M, YANG Z X. The density functional theory studies on the promoting effect of the Cu-modified Fe₃O₄ catalysts[J]. Phys Lett A, 2015, 379(6):607-612. doi: 10.1016/j.physleta.2014.12.014
[24]	SONG Z J, WANG B, YU J, MA C, CHEN T, YANG W, LIU S, SUN L S. Effect of Ti doping on heterogeneous oxidation of NO over Fe₃O₄ (111) surface by H₂O₂:A density functional study[J]. Chem Eng J, 2018, 354:517-524. doi: 10.1016/j.cej.2018.08.042
[25]	孟静.基于Fe₃O₄半金属性质的第一性原理研究[D].河北: 燕山大学, 2011. http://cdmd.cnki.com.cn/Article/CDMD-10216-1011281564.htm MENG Jing. The first-principles study on the based Fe₃O₄ of half-metallic properties[D]. Heibei: Yanshan Universuty, 2011. http://cdmd.cnki.com.cn/Article/CDMD-10216-1011281564.htm
[26]	PERDEW J P, BURKE K, ERNZERHOF M. Generalized gradient approximation made simple[J]. Phys Rev Lett, 1996, 77:3865-3868. doi: 10.1103/PhysRevLett.77.3865
[27]	WHITE J A, BIRD D M. Implementation of gradient-corrected exchange-correlation potentials in Car-Parrinello total-energy calculations[J]. Phys Rev B, 1994, 50(7):4954-4957. doi: 10.1103/PhysRevB.50.4954
[28]	周长松, 杨宏旻, 孙佳兴, 祁东旭, 毛琳, 宋子健, 孙路石. Fe₃O₄协同H₂O₂气相高级氧化单质汞的机理[J].化工学报, 2018, 69(5):1840-1845. http://d.old.wanfangdata.com.cn/Periodical/hgxb201805004 ZHOU Chang-song, YANG Hong-min, SUN Jia-xing, QI Dong-xu, MAO Lin, SONG Zi-jian, SUN Lu-shi. Mechanism of Hg removal by gaseous advanced oxidation process with Fe₃O₄ and H₂O₂[J]. J Chem Ind Eng (China), 2018, 69(5):1840-1845. http://d.old.wanfangdata.com.cn/Periodical/hgxb201805004
[29]	XU Z M, LV X J, CHEN J A, JIANG L X, LAI Y Q, LI J. First principles study of adsorption and oxidation mechanism of elemental mercury by HCl over MoS₂(100) surface[J]. Chem Eng J, 2017, 308:1225-1232. doi: 10.1016/j.cej.2016.10.059
[30]	GUO P, GUO X, ZHENG C G. Computational insights into interactions between Hg species and α-Fe₂O₃ (001)[J]. Fuel, 2011, 90(5):1840-1846. doi: 10.1016/j.fuel.2010.11.007
[31]	HUANG D M, CAO D B, LI Y W, JIAO H J. Density function theory study of CO adsorption on Fe₃O₄(111) surface[J]. J Phys Chem B, 2006, 110(28):13920-13295. doi: 10.1021/jp0568273
[32]	KAUPP M, VON SCHNERING H G. Origin of the unique stability of condensed-phase Hg₂²⁺. An ab initio investigation of M^I and M^II species (M=Zn, Cd, Hg)[J]. Inorg Chem, 1994, 33(18):4179-4185. doi: 10.1021/ic00096a049
[33]	HU A, OTTO P, LADIK J. Relativistic all-electron molecular Hartree-Fock-Dirac-(Gaunt) calculations on HgO[J]. J Mol Struct, 1999, 468(3):163-169. doi: 10.1016/S0166-1280(98)00508-9
[34]	YANG Y, LIU J, ZHANG B, LIU F. Mechanistic studies of mercury adsorption and oxidation by oxygen over spinel-type MnFe₂O₄[J]. J Hazard Mater, 2017, 321:154-161. doi: 10.1016/j.jhazmat.2016.09.007
[35]	SU T, QIN Z, HUANG G, JI H, JIANG Y, CHEN J. Density functional theory study on the interaction of CO₂ with Fe₃O₄(111) surface[J]. Appl Surf Sci, 2016, 378(15):270-276. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=148eadf365b70ee00e34b503fc17feeb
[36]	ZHANG B, LIU J, YANG Y, CHANG M. Oxidation mechanism of elemental mercury by HCl over MnO₂ catalyst:Insights from first principles[J]. Chem Eng J, 2015, 280:354-362. doi: 10.1016/j.cej.2015.06.056