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

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...

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Published inACS applied materials & interfaces Vol. 11; no. 5; pp. 4900 - 4907
Main Authors Guo, Kai, Fan, Gaofeng, Gu, Di, Yu, Shuohan, Ma, Kaili, Liu, Annai, Tan, Wei, Wang, Jiaming, Du, Xiangze, Zou, Weixin, Tang, Changjin, Dong, Lin
Format Journal Article
LanguageEnglish
Published American Chemical Society 06.02.2019
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ISSN1944-8244
1944-8252
1944-8252
DOI10.1021/acsami.8b15688

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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.
AbstractList 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.
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.
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.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.
Author Liu, Annai
Zou, Weixin
Wang, Jiaming
Dong, Lin
Tan, Wei
Fan, Gaofeng
Tang, Changjin
Gu, Di
Yu, Shuohan
Ma, Kaili
Du, Xiangze
Guo, Kai
AuthorAffiliation Jiangsu Key Laboratory of Vehicle Emissions Control
Sichuan University
School of Environment
School of Chemistry and Chemical Engineering
School of Chemistry
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pore size effect
sulfur poisoning
ammonium bisulfate decomposition
low temperature
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Snippet Sulfur poisoning has long been recognized as a bottleneck for the development of long-lived NH3-selective catalytic reduction (SCR) catalysts. Ammonium...
Sulfur poisoning has long been recognized as a bottleneck for the development of long-lived NH₃-selective catalytic reduction (SCR) catalysts. Ammonium...
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SubjectTerms active sites
ammonium bisulfate
catalysts
chromatography
engineering
Fourier transform infrared spectroscopy
poisoning
porosity
porous media
quantitative analysis
silica
sulfates
sulfur
temperature
Title Pore Size Expansion Accelerates Ammonium Bisulfate Decomposition for Improved Sulfur Resistance in Low-Temperature NH3‑SCR
URI http://dx.doi.org/10.1021/acsami.8b15688
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