論文

査読有り
2019年6月

SO2-Tolerant Selective Catalytic Reduction of NOx over Meso-TiO2@Fe2O3@Al2O3 Metal-Based Monolith Catalysts

ENVIRONMENTAL SCIENCE & TECHNOLOGY
  • Lupeng Han
  • ,
  • Min Gao
  • ,
  • Jun-ya Hasegawa
  • ,
  • Shuangxi Li
  • ,
  • Yongjie Shen
  • ,
  • Hongrui Li
  • ,
  • Liyi Shi
  • ,
  • Dengsong Zhang

53
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
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
  • 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

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