Asymmetrically Steering Excited-State Reaction Channels for Ambient N<sub><b>2</b></sub> Catalytic Oxidation

Precise control of catalytic reactions in the excited state is challenging, as the highly reactive chemical environment strengthens both forward and reverse reactions simultaneously. Here, we propose a strategy to asymmetrically regulate the reaction channels via the physical mixing of the model catalyst Co<sub>3</sub>O<sub>4</sub>/Al<sub>2</sub>O<sub>3</sub> with 13X zeolite, enabling efficient plasma-driven N<sub>2</sub> oxidation with minimized reverse reaction kinetics. <i>In situ</i> characterization combined with molecular dynamics simulations reveals that the diffusion of the product NO is selectively accelerated through Na<sup>+</sup>-mediated transport channels. This promotes NO turnover on octahedral Co<sup>3+</sup> active sites, thereby unidirectionally shifting the reaction equilibrium. Thus, we demonstrate N<sub>2</sub> oxidation performance under ambient conditions that surpasses the efficiency of thermochemical conversion at 1,800 K, achieving more than a 3-fold improvement in the N<sub>2</sub> conversion rate compared to the conventional plasma-catalysis system. This work provides an approach to orderly modulate heterogeneous catalytic reactions in the excited state.

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Publication Details

Journal
JACS Au
Published
2025-08-20
DOI
https://doi.org/10.1021/jacsau.5c00767
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
0.00

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article

Asymmetrically Steering Excited-State Reaction Channels for Ambient N2 Catalytic Oxidation

Jianping Xiao, Jiabao Lv, Zhifu Qi, Yaqi Peng et al.
JACS Au
Catalytic Processes in Materials Science
article

Asymmetrically Steering Excited-State Reaction Channels for Ambient N2 Catalytic Oxidation

Jianping Xiao, Jiabao Lv, Zhifu Qi, Yaqi Peng, Songqiang Zhu, J. Wu, Shanzhi Liu, Lujie Liu, Angjian Wu, Xiaodong Li, Jianhua Yan, Liang Wang, Pu Guo
article en

Abstract

Precise control of catalytic reactions in the excited state is challenging, as the highly reactive chemical environment strengthens both forward and reverse reactions simultaneously. Here, we propose a strategy to asymmetrically regulate the reaction channels via the physical mixing of the model catalyst Co<sub>3</sub>O<sub>4</sub>/Al<sub>2</sub>O<sub>3</sub> with 13X zeolite, enabling efficient plasma-driven N<sub>2</sub> oxidation with minimized reverse reaction kinetics. <i>In situ</i> characterization combined with molecular dynamics simulations reveals that the diffusion of the product NO is selectively accelerated through Na<sup>+</sup>-mediated transport channels. This promotes NO turnover on octahedral Co<sup>3+</sup> active sites, thereby unidirectionally shifting the reaction equilibrium. Thus, we demonstrate N<sub>2</sub> oxidation performance under ambient conditions that surpasses the efficiency of thermochemical conversion at 1,800 K, achieving more than a 3-fold improvement in the N<sub>2</sub> conversion rate compared to the conventional plasma-catalysis system. This work provides an approach to orderly modulate heterogeneous catalytic reactions in the excited state.

JACS AuVol. 5(9)
Ministry of Education (NZ), Dalian Institute of Chemical Physics (CN), Inner Mongolia University (CN), Inner Mongolia Electric Power (China) (CN), Huaneng Clean Energy Research Institute (CN), Inner Mongolia Electric Power Survey & Design Institute (China) (CN), Zhejiang Energy Research Institute (CN), Zhejiang Lab (CN), Zhejiang Energy Group (China) (CN), University of Chinese Academy of Sciences (CN), State Key Laboratory of Clean Energy Utilization, Zhejiang University (CN)
National Natural Science Foundation of China, Government of Inner Mongolia Autonomous Region, Zhejiang University, Department of Science and Technology of Inner Mongolia, National Key Research and Development Program of China
Openalex Percentile: Top 84%
Catalytic Processes in Materials Science
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