Effects of O2 and SO2 on As2O3 adsorption over W-Cu/γ-Al2O3 surface: An experimental combined theoretical analysis

XING Jia-ying; WANG Chun-bo; LI Shun; HUANG Yu-lin; YUE Shuang

doi:10.19906/j.cnki.JFCT.2022033

Volume 50 Issue 10

Oct. 2022

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XING Jia-ying, WANG Chun-bo, LI Shun, HUANG Yu-lin, YUE Shuang. Effects of O2 and SO2 on As2O3 adsorption over W-Cu/γ-Al2O3 surface: An experimental combined theoretical analysis[J]. Journal of Fuel Chemistry and Technology, 2022, 50(10): 1324-1330. doi: 10.19906/j.cnki.JFCT.2022033

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XING Jia-ying, WANG Chun-bo, LI Shun, HUANG Yu-lin, YUE Shuang. Effects of O₂ and SO₂ on As₂O₃ adsorption over W-Cu/γ-Al₂O₃ surface: An experimental combined theoretical analysis[J]. Journal of Fuel Chemistry and Technology, 2022, 50(10): 1324-1330. doi: 10.19906/j.cnki.JFCT.2022033

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Effects of O₂ and SO₂ on As₂O₃ adsorption over W-Cu/γ-Al₂O₃ surface: An experimental combined theoretical analysis

doi: 10.19906/j.cnki.JFCT.2022033

Department of Energy Power & Mechanical Engineering, North China Electric Power University, Hebei Key Laboratory of Low Carbon and High Efficiency Power Generation Technology, Baoding 071003, China

Funds: The project was supported by National Key R&D Program of China (2020YFB0606301) and National Natural Science Foundation of China (51976059)

More Information

Corresponding author: E-mail: 120192102130@ncepu.edu.cn
Received Date: 2022-03-05
Rev Recd Date: 2022-04-01

Available Online: 2022-04-22

Publish Date: 2022-10-31

Abstract

Abstract

In this work, the effects of O₂ and SO₂ on gaseous As₂O₃ adsorption over W-Cu/γ-Al₂O₃ catalyst were investigated through adsorption experiment and density functional theory (DFT) method. Experimental results show that the As₂O₃ adsorption is facilitated by O₂, and intensified with the increasing concentrations of SO₂. However, it is slightly weakened with the SO₂ concentration of 2.0×10⁻³. The As₂O₃ adsorption on W-Cu/γ-Al₂O₃ surface with adsorbed gas constituents was calculated by DFT simulation to reveal the effect mechanism. The promoting effect of O₂ on arsenic adsorption is attributed to the formation of adsorbed oxygen. The pre-adsorbed O atom significantly enhances the adsorption activities of adjacent atoms, and the pre-adsorbed O₂ molecule provides the active sites for As₂O₃ adsorption. When SO₂ is introduced, the ${{\rm{SO}}^{{2}-} _{4}}$ and ${\rm{HSO}}^-_{4} $ are formed, which change the potential field of substrate surface, and further enhance the As₂O₃ adsorption. However, the competitive adsorption between SO₂ with As₂O₃ is strengthened with increasing SO₂ concentration, and it is the reason for the decreasing trend of As₂O₃ adsorption with high concentrations of SO₂.
- O₂,
- SO₂,
- As₂O₃,
- W-Cu/γ-Al₂O₃,
- adsorption,
- surface,
- DFT

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References(31)

References

[1]	杨婷婷, 白杨, 吕游, 张文广. SCR脱硝系统多目标优化控制研究[J]. 中国电机工程学报,2021,41(14):4905−4911. YANG Ting-ting, BAI Yang, LV You, ZHANG Wen-guang. Study on multi-objective optimal control of SCR denitrification system[J]. Proc CSEE,2021,41(14):4905−4911.
[2]	ZHOU J, GUO R T, ZHANG X F, LIU Y Z, DUAN C P, WU G L, PAN W G. Cerium oxide-based catalysts for low-temperature selective catalytic reduction of NO_x with NH₃: A Review[J]. Energy Fuels,2021,35(4):2981−2998.
[3]	王钧伟, 徐灿, 秦伟, 张建利, 张先龙, 董彦杰, 崔晓峰. 凹凸棒石(PG)负载MnO_x催化剂脱除气态Hg⁰的研究[J]. 燃料化学学报,2020,48(12):1442−1451. doi: 10.3969/j.issn.0253-2409.2020.12.005 WANG Jun-wei, QIN Wei, ZHANG Jian-li, ZHANG Xian-long, DONG Yan-jie. CUI Xiao-feng. Hg⁰ removal by palygorskite ( PG) supported MnO_x catalyst[J]. J Fuel Chem Technol,2020,48(12):1442−1451. doi: 10.3969/j.issn.0253-2409.2020.12.005
[4]	张霄玲, 鲍佳宁, 李运甲, 皇甫林, 李文松, 高士秋, 许光文, 李长明, 余剑. 工业MnOx颗粒催化剂的制备及其低温脱硝应用研究[J]. 化工学报,2020,71(11):5169−5177. ZHANG Xiao-ling, BAO Jia-ning, LI Yun-jia, HUANG Pu-lin, LI Wen-song, GAO Shi-qiu, XU Guang-wen, LI Chang-ming, YU Jian. Preparation and industrial application for MnO_x particle catalyst for low temperature denitration[J]. J Chem Ind Eng,2020,71(11):5169−5177.
[5]	黄海凤, 王庐云, 漆仲华, 卢晗锋. 柴油尾气DOC催化剂Pt-Pd/CeO₂的活性和抗硫性[J]. 燃料化学学报,2013,41(11):1401−1408. HUANG Hai-feng, WANG Lu-yun, QI Zhong-hua, LU Han-feng. Activity and Sulfur resistance of Pt-Pd/CeO₂ as DOC catalyst for diesel exhaust[J]. J Fuel Chem Technol,2013,41(11):1401−1408.
[6]	李萍, 李长明, 段正康, 高士秋, 许光文, 余剑. 低温烟气脱硝催化剂适用条件与动力学[J]. 化工学报,2019,70(8):29681−2990. LI Ping, LI Chang-ming, DUAN Zheng-kang, GAO Shi-qiu, XU Guang-wen, YU Jian. Application conditions and kinetics simulation over SCR catalyst for flue gas denitrification under low temperature[J]. J Chem Ind Eng,2019,70(8):29681−2990.
[7]	UPAKUL D, AMÉLIE J, EINAR A, EILERTSEN, HERMANN E, MARK A, SATU T, BERT M, ANDREW M. Confirmation of isolated Cu²⁺ ions in SSZ-13 zeolite as active sites in NH₃-selective catalytic reduction[J]. J Phys Chem C,2012,116(7):4809−4818. doi: 10.1021/jp212450d
[8]	FICKEL D, D’ADDIO E, LAUTERBACH J, LOBO R. The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites[J]. Appl Catal B: Environ,2011,102(3/4):441−448. doi: 10.1016/j.apcatb.2010.12.022
[9]	WANG H Y, WANG B D, ZHOU J L, LI G, ZHANG D J, MA Z R, XIONG R H, SUN Q, XU W Q. CuO modified vanadium-based SCR catalysts for Hg⁰ oxidation and NO reduction[J]. J Environ Manage,2019,239(1):17−22.
[10]	赵清森. CuO/γ-Al₂O₃及其改性催化剂脱硫脱硝性能研究[D]. 武汉: 华中科技大学, 2009. ZHAO Qing-sen. The experimental study on desulfurization and denitrification by CuO/γ-Al₂O₃ and modified catalysts[D]. Wuhan: Huazhong University of Science and Technology, 2009.
[11]	HU J Y, LUO G Q, LI Z H, LIU, M Y, ZOU R J, LI X, YAO H. Deactivation mechanism of KCl and K₂SO₄ poisoned V₂O₅/WO₃-TiO₂ catalyst on gaseous elemental mercury oxidation[J]. Fuel,2020,278(9):118245.
[12]	ZHANG Y, ZHAO L, KANG M D, CHEN Z, GAO S J, HAO H G. Insights into high CO-SCR performance of CuCoAlO catalysts derived from LDH/MOFs composites and study of H₂O/SO₂ and alkali metal resistance[J]. Chem Eng J,2021,426:131873. doi: 10.1016/j.cej.2021.131873
[13]	SHEN F H, LIU J, ZHANG Z, DAI J X. On-Line analysis and kinetic behavior of arsenic release during coal combustion and pyrolysis[J]. Environ Sci Technol,2015,49(22):13716−13723. doi: 10.1021/acs.est.5b03626
[14]	LIU H M, PAN W P, WANG C B, SHEN F H. Volatilization of arsenic during coal combustion based on isothermal thermogravimetric analysis at 600−1500 ℃[J]. Energy Fuels,2016,30(8):6790−6798. doi: 10.1021/acs.energyfuels.6b00816
[15]	LI X, LI J H, PENG Y, SI W Z, HE X, HAO J M. Regeneration of commercial SCR catalysts: Probing the existing forms of arsenic oxide[J]. Environ Sci Technol,2015,49(16):9971−9978. doi: 10.1021/acs.est.5b02257
[16]	陆强, 裴鑫琦, 徐明新, 王涵啸, 吴亚昌, 欧阳昊东. SCR脱硝催化剂抗砷中毒改性优化与再生研究进展[J]. 化工进展,2021,40(5):2365−2374. LU Qiang, PEI Xin-qi, XU Ming-xin, WANG Han-xiao, WU Ya-chang, OUYANG Hao-dong. Progress in the development and regeneration of SCR catalysts for anti-arsenic poisoning[J]. Chem Ind Eng Prog,2021,40(5):2365−2374.
[17]	LI X Y, J. CHEN J, XIAO Y, LU C M, YAO H. Insight into the homogenous and heterogeneous transformation behavior of arsenic on commercial V₂O₅-WO₃-TiO₂ and novel γ-Fe₂O₃ catalysts during selective catalytic reduction of NO_x[J]. Fuel,2021,301:121051. doi: 10.1016/j.fuel.2021.121051
[18]	DORIS V, HANNS H, JOSEF S, WOLFGANG G, FRANZ R. Deactivation processes on TiO₂ V₂O₅ based denox catalysts[J]. Chem Ing Tech,1988,60(9):714−715. doi: 10.1002/cite.330600918
[19]	XING J Y, WANG C B, HUANG Y L, YUE S, EDWARD J. The effect of W and Mo modification on arsenic adsorption over Cu/γ-Al₂O₃ catalyst: Experimental and theoretical analysis[J]. Chem Eng J,2022,432:134376. doi: 10.1016/j.cej.2021.134376
[20]	XING J Y, WANG C B, ZHANG Y, SI T, LIU X. A deep insight into the role of O₂ on As₂O₃ capture over γ-Al₂O₃ sorbent: Experimental and DFT study[J]. Chem Eng J,2020,410:128311.
[21]	ZHANG Y, WANG C B, LIU H M. Experiment and mechanism research on gas-phase As₂O₃ adsorption of Fe₂O₃/γ-Al₂O₃[J]. Fuel,2016,181:1034−1040. doi: 10.1016/j.fuel.2016.04.141
[22]	CHEN D K, HU H Y, XU Z, LIU H, CAO J X, SHEN J H, YAO H. Findings of proper temperatures for arsenic capture by CaO in the simulated flue gas with and without SO₂[J]. Chem Eng J,2015,267:201−206. doi: 10.1016/j.cej.2015.01.035
[23]	HU P B, WENG Q Y, LI D L, LV T, WANG S J, ZHOU Y Q. Effects of O₂, SO₂, H₂O and CO₂ on As₂O₃ adsorption by γ-Al₂O₃ based on DFT analysis[J]. J Hazard Mater,2020,403:123866.
[24]	刘翔, 张月, 邢佳颖, 郭雨生, 许桐, 王春波. Mn改性Fe₂O₃/γ-Al₂O₃脱除气相As₂O₃实验研究[J]. 中国电机工程学报,2021,41(15):5250−5258. LIU Xiang, ZHANG Yue, XING Jia-ying, GUO Yu-sheng, XU Tong, WANG Chun-bo. Experimental study on removal of gas-phase As₂O₃ by Mn modified Fe₂O₃/γ-Al₂O₃[J]. Proc CSEE,2021,41(15):5250−5258.
[25]	GAO Z Y, SUN Y, LI M H, YANG W J, DING X L. Adsorption sensitivity of Fe decorated different graphene supports toward toxic gas molecules (CO and NO)[J]. Appl Surf Sci,2018,456:351−359. doi: 10.1016/j.apsusc.2018.06.112
[26]	HALGREN T A, LIPSCOMB W N. The synchronous-transit method for determining reaction pathways and locating molecular transition states[J]. Chem Phys Lett,1977,49(2):225−232. doi: 10.1016/0009-2614(77)80574-5
[27]	CONTRERAS M L, AROSTEGUI J M, ARMESTO L. Arsenic interactions during co-combustion processes based on thermodynamic equilibrium calculations[J]. Fuel,2009,88(3):539−546. doi: 10.1016/j.fuel.2008.09.028
[28]	SONG B, SONG M, CHEN D D, MENG F Y, WEI Y X. Retention of arsenic in coal combustion flue gas at high temperature in the presence of CaO[J]. Fuel,2020,259:116249. doi: 10.1016/j.fuel.2019.116249
[29]	DENG X Y, MIN B K, GULOY A, CYNTHIA M. Enhancement of O₂ dissociation on Au(111) by adsorbed oxygen: implications for oxidation catalysis[J]. J Am Chem Soc,2005,127(25):9267. doi: 10.1021/ja050144j
[30]	WANG Z, LIU J, YANG Y, 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
[31]	GAO Z Y, LI M H, SUN Y, YANG W J. Effects of oxygen functional complexes on arsenic adsorption over carbonaceous surface[J]. J Hazard Mater,2018,360(15):436−444.