Oxidation mechanisms of H2S by oxygen and oxygen-containing functional groups on activated carbon

被引:67
作者
Li, Yuran [1 ]
Lin, Yuting [1 ,2 ]
Xu, Zhicheng [1 ,2 ]
Wang, Bin [1 ]
Zhu, Tingyu [1 ,3 ]
机构
[1] Chinese Acad Sci, Beijing Engn Res Ctr Proc Pollut Control, Natl Engn Lab Hydromet Cleaner Prod Technol, Inst Proc Engn, Beijing 100190, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
Activated carbon; Hydrogen sulfide; Elemental sulfur; Sulfate; Sulfite; SELECTIVE CATALYTIC-REDUCTION; HYDROGEN-SULFIDE; NO; ADSORPTION; SULFUR; SO2; NH3; REACTIVITY; NH3-SCR; MERCURY;
D O I
10.1016/j.fuproc.2019.03.006
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Activated carbon (AC) has the advantage of multi-pollutant control with a high removal efficiency for flue gas purification. It is necessary to determine the oxidation mechanism and oxidation products of hydrogen sulfide (H2S) on AC to simultaneously capture H2S and SO2. A fixed-bed reactor was coupled with a mass spectrometer (MS) to detect the gaseous components and X-ray photoelectron spectroscopy (XPS) was used to distinguish the sulfur-containing species in the oxidation products on AC and thermally treated AC to investigate the actions of the oxygen-containing functional groups. The results revealed that H2S was adsorbed on the AC surface and combined with oxygen-containing functional groups to form sulfate (SO42-) in the absence of O-2. In the presence of O-2, H2S and O-2 in the atmosphere were adsorbed on the AC active sites, and the catalytic reaction produced elemental sulfur. Elemental sulfur further reacted with O-2 to produce gaseous SO2. According to the detection results of XPS and the in situ diffuse reflectance infrared Fourier transform (in situ DRIFT) spectra, an oxidation mechanism of H2S by O-2 and oxygen-containing functional groups was described. The C=C and C = O bonds were broken by H2S, and then, C-S and S-O bonds of the intermediate products were generated. The C-S bond tended to form elemental sulfur, while the S-O bond likely formed a sulfate or gaseous SO2. Porosity analysis showed that the AC specific surface area decreased after H2S adsorption and that sulfate reduced the specific surface area much more than elemental sulfur.
引用
收藏
页码:110 / 119
页数:10
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