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 in | ACS applied materials & interfaces Vol. 11; no. 5; pp. 4900 - 4907 |
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Main Authors | , , , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
American Chemical Society
06.02.2019
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Subjects | |
Online Access | Get full text |
ISSN | 1944-8244 1944-8252 1944-8252 |
DOI | 10.1021/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. |
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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 |
AuthorAffiliation_xml | – name: School of Environment – name: Jiangsu Key Laboratory of Vehicle Emissions Control – name: School of Chemistry and Chemical Engineering – name: Sichuan University – name: School of Chemistry |
Author_xml | – sequence: 1 givenname: Kai surname: Guo fullname: Guo, Kai – sequence: 2 givenname: Gaofeng surname: Fan fullname: Fan, Gaofeng – sequence: 3 givenname: Di surname: Gu fullname: Gu, Di – sequence: 4 givenname: Shuohan surname: Yu fullname: Yu, Shuohan – sequence: 5 givenname: Kaili surname: Ma fullname: Ma, Kaili – sequence: 6 givenname: Annai surname: Liu fullname: Liu, Annai – sequence: 7 givenname: Wei surname: Tan fullname: Tan, Wei – sequence: 8 givenname: Jiaming surname: Wang fullname: Wang, Jiaming – sequence: 9 givenname: Xiangze surname: Du fullname: Du, Xiangze organization: Sichuan University – sequence: 10 givenname: Weixin surname: Zou fullname: Zou, Weixin – sequence: 11 givenname: Changjin surname: Tang fullname: Tang, Changjin email: tangcj@nju.edu.cn organization: Jiangsu Key Laboratory of Vehicle Emissions Control – sequence: 12 givenname: Lin orcidid: 0000-0002-8393-6669 surname: Dong fullname: Dong, Lin email: donglin@nju.edu.cn organization: Jiangsu Key Laboratory of Vehicle Emissions Control |
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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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Title | Pore Size Expansion Accelerates Ammonium Bisulfate Decomposition for Improved Sulfur Resistance in Low-Temperature NH3‑SCR |
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