Replacing the traditional oxygen evolution reaction with the alcohol oxidation reaction (AOR) can significantly reduce anodic overpotential and offer high-value chemicals simultaneously. However, its progress is severely hampered by the intricate catalyst synthesis and inadequate control over the electronic structure of active sites. Here, we propose a strategy for nonequilibrium regulation of catalyst electronic structures via laser irradiation. By precisely modulating the number of laser pulses, the Ni2+/Ni3+ ratio can be effectively tailored. The NiL-100 electrode demonstrates excellent performance for the electrooxidation of multiple alcohols. Specifically, the current density of ethanol oxidation exceeds most of the Ni-based catalysts reported so far, with 92.66% FE for acetic acid. Combining the first-principles calculations, we establish the structure–activity relationship of catalysts: the laser-tuned electronic structure optimizes the adsorption energy of reaction intermediates, then improves the catalytic activity. This work introduces an efficient, simple, green, and low-cost method for the efficient manufacturing of self-supporting electrodes that enables precise regulation of electronic structures, which will provide new insights for the large-scale manufacturing of high-performance catalysts.
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2026 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.
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