Plasma-assisted manipulation of vanadia nanoclusters for efficient selective catalytic reduction of NOx

被引:3
|
作者
Yin, Yong [1 ]
Luo, Bingcheng [2 ]
Li, Kezhi [3 ]
Moskowitz, Benjamin M. [4 ]
Mosevizky Lis, Bar [4 ]
Wachs, Israel E. [4 ]
Zhu, Minghui [5 ]
Sun, Ye [1 ]
Zhu, Tianle [1 ]
Li, Xiang [1 ]
机构
[1] Beihang Univ, Sch Space & Environm, Beijing 100191, Peoples R China
[2] China Agr Univ, Coll Sci, Beijing 100083, Peoples R China
[3] Sinopec Catalyst Co Ltd, Inst Engn Technol, Beijing 101111, Peoples R China
[4] Lehigh Univ, Dept Chem & Biomol Engn, Operando Mol Spect & Catalysis Lab, Bethlehem, PA 18015 USA
[5] East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China
基金
中国国家自然科学基金;
关键词
TOTAL-ENERGY CALCULATIONS; ELASTIC BAND METHOD; LOW-TEMPERATURE; NITRIC-OXIDE; ACTIVE-SITES; ELECTRONIC-PROPERTIES; SOLID CATALYSTS; NH3; SCR; ADSORPTION;
D O I
10.1038/s41467-024-47878-1
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Supported nanoclusters (SNCs) with distinct geometric and electronic structures have garnered significant attention in the field of heterogeneous catalysis. However, their directed synthesis remains a challenge due to limited efficient approaches. This study presents a plasma-assisted treatment strategy to achieve supported metal oxide nanoclusters from a rapid transformation of monomeric dispersed metal oxides. As a case study, oligomeric vanadia-dominated surface sites were derived from the classic supported V2O5-WO3/TiO2 (VWT) catalyst and showed nearly an order of magnitude increase in turnover frequency (TOF) value via an H-2-plasma treatment for selective catalytic reduction of NO with NH3. Such oligomeric surface VOx sites were not only successfully observed and firstly distinguished from WOx and TiO2 by advanced electron microscopy, but also facilitated the generation of surface amide and nitrates intermediates that enable barrier-less steps in the SCR reaction as observed by modulation excitation spectroscopy technologies and predicted DFT calculations.
引用
收藏
页数:12
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