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

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High Resolution Image Download MS PowerPoint Slide 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 3 O 4 /Al 2 O 3 with 13X zeolite, enabling efficient plasma-driven N 2 oxidation with minimized reverse reaction kinetics. In situ characterization combined with molecular dynamics simulations reveals that the diffusion of the product NO is selectively accelerated through Na + -mediated transport channels. This promotes NO turnover on octahedral Co 3+ active sites, thereby unidirectionally shifting the reaction equilibrium. Thus, we demonstrate N 2 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 2 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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