2019年6月
SO2-Tolerant Selective Catalytic Reduction of NOx over Meso-TiO2@Fe2O3@Al2O3 Metal-Based Monolith Catalysts
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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- 巻
- 53
- 号
- 11
- 開始ページ
- 6462
- 終了ページ
- 6473
- 記述言語
- 英語
- 掲載種別
- 研究論文(学術雑誌)
- DOI
- 10.1021/acs.est.9b00435
- 出版者・発行元
- AMER CHEMICAL SOC
It is an intractable issue to improve the low-temperature SO2-tolerant selective catalytic reduction (SCR) of NOx with NH3 because deposited sulfates are difficult to decompose below 300 degrees C. Herein, we established a low-temperature self-prevention mechanism of mesoporous-TiO2@Fe2O3 core-shell composites against sulfate deposition using experiments and density functional theory. The mesoporous TiO2-shell effectively restrained the deposition of FeSO4 and NH4HSO4 because of weak SO2 adsorption and promoted NH4HSO4 decomposition on the mesoporous-TiO2. The electron transfer at the Fe2O3 (core)-TiO2 (shell) interface accelerated the redox cycle, launching the "Fast SCR" reaction, which broadened the low-temperature window. Engineered from the nano- to macro-scale, we achieved one-pot self-installation of mesoporous-TiO2@Fe2O3 composites on the self-tailored AlOOH@Al-mesh monoliths. After the thermal treatment, the mesoporous-TiO2@Fe2O3@Al2O3 monolith catalyst delivered a broad window of 220-420 degrees C with NO conversion above 90% and had superior SO2 tolerance at 260 degrees C. The effective heat removal of Al-mesh monolithcatalysts restrained NH3 oxidation to NO and N2O while suppressing the decomposition of NH4NO3 to N2O, and this led to much better high-temperature activity and N-2 selectivity. This work supplies a new point for the development of low-temperature SO2-tolerant monolithic SCR catalysts with high N-2 selectivity, which is of great significance for both academic interests and practical applications.
- リンク情報
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- DOI
- https://doi.org/10.1021/acs.est.9b00435
- PubMed
- https://www.ncbi.nlm.nih.gov/pubmed/31063367
- Web of Science
- https://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcAuth=JSTA_CEL&SrcApp=J_Gate_JST&DestLinkType=FullRecord&KeyUT=WOS:000470793900037&DestApp=WOS_CPL
- URL
- http://orcid.org/0000-0002-7263-1157
- ID情報
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- DOI : 10.1021/acs.est.9b00435
- ISSN : 0013-936X
- eISSN : 1520-5851
- ORCIDのPut Code : 57682987
- PubMed ID : 31063367
- Web of Science ID : WOS:000470793900037