Tunning active oxygen species for boosting Hg0 removal and SO2-resistance of Mn-Fe oxides supported on (NH4)2S2O8 doping activated coke

被引:23
作者
Du, Xueyu [1 ,2 ]
Li, Caiting [1 ,2 ]
Zhang, Jie [1 ,2 ]
Zhu, Youcai [1 ,2 ]
Liang, Caixia [1 ,2 ]
Huang, Le [1 ,2 ]
Yang, Kuang [1 ,2 ]
Yao, Chaoliang [3 ]
Ma, Ying [3 ]
机构
[1] Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Peoples R China
[2] Hunan Univ, Key Lab Environm Biol & Pollut Control, Minist Educ, Changsha 410082, Peoples R China
[3] Yonker Environm Protect Co Ltd, Changsha 410330, Peoples R China
关键词
MnFe/NAC; oxygen functional groups; Hg-0; control; SO2-resistance; Hg-TPD; ELEMENTAL MERCURY REMOVAL; SIMULATED FLUE-GAS; REACTION-MECHANISM; CATALYTIC-REDUCTION; ADSORPTION; TEMPERATURE; OXIDATION; CARBON; CAPTURE; SO2;
D O I
10.1016/j.jhazmat.2022.129882
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Active oxygen species (AOS) play an essential role in modulating the activity of activated coke (AC) based samples. In this paper, AC was endowed with abundant AOS by modifying with (NH4)(2)S2O8 and MnOx-FeOx for Hg-0 removal. (NH4)(2)S2O8 treatment induced abundant micropores and oxygen-containing functional groups, and thus provided more anchoring sites for the dispersion of MnOx-FeOx. The synergy of MnOx-FeOx and interaction between MnOx-FeOx and NAC support contributed to a larger surface area, highly-dispersed active components, stronger reducibility, and more metal ions with high valence of MnFe/NAC. The optimal MnFe/NAC exhibited superior Hg-0 removal efficiency above 90% at 120 similar to 180 degrees C, as well as excellent performance for simultaneous removal of Hg-0 and NO, and 600 ppm SO2 and 8 vol.% H2O addition led to a slight deterioration. XPS and Hg-TPD revealed that mercury adsorbed on MnFe/NAC included phy-Hg, C=O-Hg, COO-Hg, and O-L-HgO. Besides, the priority of AOS for Hg-0 chemisorption was C=O > COO- > O-L, and Hg2+ was also detected in the outlet. Moreover, the SO2-poisoning effect was ascribed to the sulfation of MnOx and the occupation of COO- and C=O, and FeOx incorporation enhanced the SO2-resistance through weakening SO2 adsorption on C=O and COO-. The motivation of O-2 mainly contributed to the regeneration of AOS, especially O-L. The excellent regeneration performance and stability further affirmed the application potential of MnFe/NAC for Hg-0 capture from coal-fired flue gas.
引用
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页数:14
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共 74 条
[1]  
[Anonymous], 2011, GB132232011
[2]   CHEMISTRY IN NONINTEGER DIMENSIONS BETWEEN 2 AND 3 .2. FRACTAL SURFACES OF ADSORBENTS [J].
AVNIR, D ;
FARIN, D ;
PFEIFER, P .
JOURNAL OF CHEMICAL PHYSICS, 1983, 79 (07) :3566-3571
[3]   Simultaneous removal of HCHO and elemental mercury from flue gas over Co-Ce oxides supported on activated coke impregnated by sulfuric acid [J].
Chen, Jiaqiang ;
Li, Caiting ;
Li, Shanhong ;
Lu, Pei ;
Gao, Lei ;
Du, Xueyu ;
Yi, Yaoyao .
CHEMICAL ENGINEERING JOURNAL, 2018, 338 :358-368
[4]   Novel Effective Catalyst for Elemental Mercury Removal from Coal-Fired Flue Gas and the Mechanism Investigation [J].
Chen, Wanmiao ;
Pei, Yang ;
Huang, Wenjun ;
Qu, Zan ;
Hu, Xiaofang ;
Yan, Naiqiang .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2016, 50 (05) :2564-2572
[5]   Synthesis of covalently bonded graphene oxide-iron magnetic nanoparticles and the kinetics of mercury removal [J].
Diagboya, Paul N. ;
Olu-Owolabi, Bamidele I. ;
Adebowale, Kayode O. .
RSC ADVANCES, 2015, 5 (04) :2536-2542
[6]   Investigation of Elemental Mercury Removal from Coal-Fired Boiler Flue Gas over MIL101-Cr [J].
Dong, Lu ;
Huang, Yaji ;
Liu, Lingqin ;
Liu, Changqi ;
Xu, Ligang ;
Zha, Jianrui ;
Chen, Hao ;
Liu, Hao .
ENERGY & FUELS, 2019, 33 (09) :8864-8875
[7]   Highly efficient simultaneous removal of HCHO and elemental mercury over Mn-Co oxides promoted Zr-AC samples [J].
Du, Xueyu ;
Li, Caiting ;
Zhang, Jie ;
Zhao, Lingkui ;
Li, Shanhong ;
Lyu, Yue ;
Zhang, Yindi ;
Zhu, Youcai ;
Huang, Le .
JOURNAL OF HAZARDOUS MATERIALS, 2021, 408
[8]   Promotional removal of HCHO from simulated flue gas over Mn-Fe oxides modified activated coke [J].
Du, Xueyu ;
Li, Caiting ;
Zhao, Lingkui ;
Zhang, Jie ;
Gao, Lei ;
Sheng, Jingjing ;
Yi, Yaoyao ;
Chen, Jiaqiang ;
Zeng, Guangming .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 232 :37-48
[9]   Removal of Gas-Phase Element Mercury by Activated Carbon Fiber Impregnated with CeO2 [J].
Fan, Xiaopeng ;
Li, Caiting ;
Zeng, Guangming ;
Gao, Zhao ;
Chen, Ling ;
Zhang, Wei ;
Gao, Hongliang .
ENERGY & FUELS, 2010, 24 (08) :4250-4254
[10]   Influence of textures, oxygen-containing functional groups and metal species on SO2 and NO removal over Ce-Mn/NAC [J].
Fang Ning-Jie ;
Guo Jia-Xiu ;
Shu Song ;
Li Jian-Jun ;
Chu Ying-Hao .
FUEL, 2017, 202 :328-337