Removing mercury from flue gas by sulfur-doped zeolite-templated carbon: Synthesize and adsorption mechanism

被引:31
作者
Liu, Ying [1 ]
Wang, Jiaxin [1 ]
Wang, Tao [1 ]
Pan, Wei-Ping [1 ,2 ]
机构
[1] North China Elect Power Univ, Key Lab Power Stn Energy Transfer Convers & Syst, Minist Educ, Beijing 102206, Peoples R China
[2] ICSET Solut, Bowling Green, KY 42104 USA
关键词
Elemental mercury; Sulfur; Chemical vapor deposition; Zeolite-templated carbon; Density functional theory; GASEOUS ELEMENTAL MERCURY; ACTIVATED CARBON; FUNCTIONAL-GROUPS; OXIDATION; BIOCHAR; TEMPERATURE; FRAMEWORK; CATALYSTS; SURFACE; FIBERS;
D O I
10.1016/j.seppur.2022.121228
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Elemental mercury is harmful to humanity and the ecological environment. It is a simple and feasible method to capture elemental mercury by carbon-based adsorbents. The purpose of this work is to develop zeolite-templated carbon with and without sulfur (ZTC and S-doped ZTC) and to explore their mercury adsorption performance. ZTC and S-doped ZTC were synthesized by chemical vapor deposition (CVD) method and their mercury adsorption performance were tested at 30 and 150 degrees C. Among all ZTC samples, BEA-ZTC-HS exhibited highest mercury removal efficiency (MRE) whose initial value was 99.99% (150 degrees C) and 97.39% (30 degrees C) and decreased to 96.63% and 89.15% after one hour mercury adsorption. The physical and chemical properties of the ZTC samples were characterized by various methods to explain the high MRE of BEA-ZTC-HS. The experimental results shown that BEA-ZTC-HS replicated the crystal structure of BEA zeolite faithfully and exhibited regular microporous structure and doesn't have obvious elemental sulfur whose existence could block the micropores in ZTC. This was helpful to the mass transfer of Hg-0 in ZTC. Moreover, the chemical properties of BEA-ZTC-HS shown that the introduced sulfur were mainly bonded to the carbon framework of ZTC in the form of thiophene, sulfone, sulfoxide and sulfonic acid. Those sulfur-containing functional groups provided main active sites for mercury capture and exhibited higher activity at 150 degrees C. Finally, Density Functional Theory (DFT) was used to reveal the adsorption mechanism of ZTC and S-doped ZTC on Hg-0. Due to its good properties of regeneration, higher MRE, good thermal stability and low cost, BEA-ZTC-HS has a wide prospect for industrial application in the wide temperature ranges compared to the activated carbon injection technology.
引用
收藏
页数:15
相关论文
共 62 条
[11]   Unique thermal contraction of zeolite-templated carbons enabling micropore size tailoring and its effects on methane storage [J].
Choi, Seokin ;
Alkhabbaz, Mustafa A. ;
Wang, Yuguo ;
Othman, Rashid M. ;
Choi, Minkee .
CARBON, 2019, 141 :143-153
[12]   Large-scale synthesis of high-quality zeolite-templated carbons without depositing external carbon layers [J].
Choi, Seokin ;
Kim, Hyeonbin ;
Lee, Songhyun ;
Wang, Yuguo ;
Ercan, Cemal ;
Othman, Rashid ;
Choi, Minkee .
CHEMICAL ENGINEERING JOURNAL, 2015, 280 :597-605
[13]   On the adsorption of elemental mercury on single-atom TM (TM = V, Cr, Mn, Co) decorated graphene substrates [J].
Gao, Zhengyang ;
Xu, Shaopeng ;
Li, Linlin ;
Yan, Ge ;
Yang, Weijie ;
Wu, Chongchong ;
Gates, Ian D. .
APPLIED SURFACE SCIENCE, 2020, 516
[14]   Novel sorbents for mercury removal from flue gas [J].
Granite, EJ ;
Pennline, HW ;
Hargis, RA .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2000, 39 (04) :1020-1029
[15]   Mercury adsorption properties of sulfur-impregnated adsorbents [J].
Hsi, HC ;
Rood, MJ ;
Rostam-Abadi, M ;
Chen, SG ;
Chang, R .
JOURNAL OF ENVIRONMENTAL ENGINEERING-ASCE, 2002, 128 (11) :1080-1089
[16]   Effects of sulfur impregnation temperature on the properties and mercury adsorption capacities of activated carbon fibers (ACFs) [J].
Hsi, HC ;
Rood, MJ ;
Rostam-Abadi, M ;
Chen, SG ;
Chang, R .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2001, 35 (13) :2785-2791
[17]   Sulfurized biochar prepared by simplified technic with superior adsorption property towards aqueous Hg(II) and adsorption mechanisms [J].
Huang, Shengze ;
Liang, Qianwei ;
Geng, Junjie ;
Luo, Hanjin ;
Wei, Qiang .
MATERIALS CHEMISTRY AND PHYSICS, 2019, 238
[18]   Manganese oxide/titania materials for removal of NOx and elemental mercury from flue gas [J].
Ji, Lei ;
Sreekanth, Pavani M. ;
Smirniotis, Panagiotis G. ;
Thiel, Stephen W. ;
Pinto, Neville G. .
ENERGY & FUELS, 2008, 22 (04) :2299-2306
[19]   Acceleration of the reaction of H2S and SO2 by non-thermal plasma to improve the mercury adsorption performance of activated carbon [J].
Ji, Qingyu ;
Luo, Guangqian ;
Shi, Mengting ;
Zou, Renjie ;
Fang, Can ;
Xu, Yang ;
Li, Xian ;
Yao, Hong .
CHEMICAL ENGINEERING JOURNAL, 2021, 423
[20]   Adsorption mechanism of elemental mercury (Hg0)) on the surface of MnCl2 (110) studied by Density Functional Theory [J].
Ji, Wenchao ;
Shen, Zhemin ;
Fan, Maohong ;
Su, Pingru ;
Tang, Qingli ;
Zou, Congyang .
CHEMICAL ENGINEERING JOURNAL, 2016, 283 :58-64