Boosting Ag/Al2O3 Catalytic Activity for NOx Removal via C3H6-SCR through Functional TiO2 Support Engineering

催化作用 化学 Boosting(机器学习) 材料科学 计算机科学 人工智能 有机化学
作者
Yun Zhong,Yingsheng An,Zidi Yan,Zhi Liu,Tao Shen,Hang Xiao,Yanshuang Zhang,Min Xiao,Yong De Yan,Yunbo Yu,Hong He
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:59 (35): 18771-18782 被引量:1
标识
DOI:10.1021/acs.est.5c07583
摘要

Alumina supported silver (Ag/Al2O3) is considered as a promising catalyst for the selective catalytic reduction of nitrogen oxides with hydrocarbons (HC-SCR). However, its practical implementation remains limited by insufficient catalytic performance. Herein, we present a novel strategy to fabricate a highly efficient Ag/TiO2/Al2O3 catalyst utilizing a functional TiO2-modified AlOOH precursor. The obtained catalyst demonstrates significantly enhanced catalytic activity, durability, and stability for C3H6-SCR across a broad temperature range compared to conventional Ag/Al2O3. The incorporation of TiO2 strengthens the Ag-support interaction through facilitating electron transfer from Ag to the TiO2/Al2O3 support, leading to the formation of highly dispersed Agnδ+ clusters as the dominant active species. Mechanistic studies reveal that Agnδ+ clusters effectively accelerate the partial oxidation of C3H6 to reactive enolic species, which in turn trigger a new pathway for NOx reduction via the formation of -CN intermediates. This change in reaction mechanism induced by TiO2 modification was also confirmed by a lower activation energy barrier for NOx reduction compared to that of Ag/Al2O3. By simultaneously optimizing both the density of active sites and their intrinsic reactivity, this approach delivers a substantial enhancement in C3H6-SCR performance, offering new insights into catalyst design for hydrocarbon-SCR applications.
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