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Pore Size Expansion Accelerates Ammonium Bisulfate Decomposition for Improved Sulfur Resistance in Low-Temperature NH₃-SCR

Author:
Guo, Kai, Fan, Gaofeng, Gu, Di, Yu, Shuohan, Ma, Kaili, Liu, Annai, Tan, Wei, Wang, Jiaming, Du, Xiangze, Zou, Weixin, Tang, Changjin, Dong, Lin
Source:
ACS applied materials & interfaces 2019 v.11 no.5 pp. 4900-4907
ISSN:
1944-8252
Subject:
Fourier transform infrared spectroscopy, active sites, ammonium bisulfate, catalysts, chromatography, engineering, poisoning, porosity, porous media, quantitative analysis, silica, sulfates, sulfur, temperature
Abstract:
Sulfur poisoning has long been recognized as a bottleneck for the development of long-lived NH₃-selective catalytic reduction (SCR) catalysts. Ammonium bisulfate (ABS) deposition on active sites is the major cause of sulfur poisoning at low temperatures, and activating ABS decomposition is regarded as the ultimate way to alleviate sulfur poisoning. In the present study, we reported an interesting finding that ABS decomposition can be simply tailored via adjusting the pore size of the material it deposited. We initiated this study from the preparation of mesoporous silica SBA-15 with uniform one-dimensional pore structure but different pore sizes, followed by ABS loading to investigate the effect. The results showed that ABS decomposition proceeded more easily on SBA-15 with larger pores, and the decomposition temperature declined as large as 40 °C with increasing pore size of SBA-15 from 4.8 to 11.8 nm. To further ascertain the real effect in NH₃-SCR reaction, the Fe₂O₃/SBA-15 probe catalyst was prepared. It was found that the catalyst with larger mesopores exhibited much improved sulfur resistance, and quantitative analysis results obtained from Fourier transform infrared and ion chromatograph further proved that the deposited sulfates were greatly alleviated. The result of the present study demonstrates for the first time the vital role of pore size engineering in ABS decomposition and may open up new opportunities for designing NH₃-SCR catalysts with excellent sulfur resistance.
Agid:
6302442