Activity Self-Optimization Steered by Dynamically Evolved Fe3+@Fe2+ Double-Center on Fe2O3 Catalyst for NH3-SCR

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Yuan, Hai Yang
Sun, Ningning
Chen, Jianfu
Yang, Hua Gui
Hu, P
Wang, Haifeng
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2022
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Abstract

Identification of the active centers dynamically stable under the reaction condition is of paramount importance but challenging because of the limited knowledge of steady-state chemistry on catalysts at the atomic level. Herein, focusing on the Fe2O3 catalyst for the selective catalytic reduction of NO with NH3 (NH3-SCR) as a model system, we reveal quantitatively the self-evolving Fe3+@Fe2+ (∼1:1) double-centers under the in-situ condition by the first-principles microkinetic simulations, which enables the accurate prediction of the optimal industry operating temperature (590 K). The cooperation of this double-center achieves the self-optimization of catalytic activity and rationalizes the intrinsic origin of Fe2O3 catalyzing NH3-SCR at middle-high temperatures instead of high temperatures. Our findings demonstrate the atomic-level self-evolution of active sites and the dynamically adjusted activity variation of the catalyst under the in-situ condition during the reaction process and provide insights into the reaction mechanism and catalyst optimization.

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JACS Au

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2

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10

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© 2022 The Authors. Published by American Chemical Society. This publication is licensed under CC-BY-NC-ND 4.0.

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Chemical sciences

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Physical Sciences

Chemistry, Multidisciplinary

Chemistry

dynamically active center

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Yuan, HY; Sun, N; Chen, J; Yang, HG; Hu, P; Wang, H, Activity Self-Optimization Steered by Dynamically Evolved Fe3+@Fe2+ Double-Center on Fe2O3 Catalyst for NH3-SCR, JACS Au, 2022, 2 (10), pp. 2352-2358

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