Enhancing electrochemical nitrogen fixation by mimicking π back-donation on laser-tuned Lewis acid sites in noble-metal-molybdenum carbide
Applied Catalysis B: Environmental(2023)
摘要
Conventional electrocatalysts underperform with reaction kinetics, nitrogen dissociation, and activated hydrogen recombination, demanding effective strategies for improving electrochemical nitrogen fixation. The challenge lies in the rational design of electron back-donating centers for nitrogen activation and hydrogen migration path optimization. This study proposes an effective laser-tuning strategy to construct noble-metal Lewis acid sites on molybdenum carbide (M-Mo2C, M = Ru, Rh, Pd, Ir), yielding a more active material system by mimicking π back-donation behavior. Laser-tuned Lewis acid sites can effectively break N≡N bonds, lower thermodynamic energy barrier of the rate-determining hydrogenation step (*NN → *N-NH), and optimize hydrogen migration pathway. The Rh-Mo2C shows superior NRR activity with NH3 yield of ∼26.3 µg h−1 cm−2cat. and Faradaic efficiency of ∼15.4%, which are 5.1- and 3.6-fold higher than those of Mo2C, respectively. This work demonstrates a unique and universal strategy for designing high-performance electrocatalysts by accurately manipulating electronic structure of active sites.
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关键词
Laser synthesis,Lewis acid sites,π back-donation,Molybdenum carbides,Electrochemical nitrogen fixation
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