Manipulating the heterostructure and architecture of Cu/CuO catalyst towards pH-universal hydrogen evolution reaction

JY Wang and Y Guo and HS Li and CP He and LL Wang and YZ Cao and J He and HW Jing and XM Wang and L Zhao, SURFACES AND INTERFACES, 73, 107568 (2025).

DOI: 10.1016/j.surfin.2025.107568

Producing hydrogen via electrocatalytic water splitting will benefit from the realization of more efficient and less expensive catalysts and scalable synthetic strategies. Herein, we present a facile thermal treatment method to synthesize well-distributed nanorod arrays of Cu/CuO schottky junctions as effective pH-universal hydrogen evolution reaction (HER) catalysts. By tuning the copper valence state with thermal treatment, an optimal Cu/CuO ratio (similar to 1:1) was achieved, enabling synergistic enhancement of HER activity. The resulting CuOx-300/CF electrocatalyst exhibits low cathodic overpotentials (247, 107, and 80 mV at 10 mA cm(-2)) and good stability across acidic, alkaline, and neutral media. Molecular dynamics and in situ infrared spectroscopy revealed that this synergy originates from distinct adsorption sites: CuO strongly adsorbs and dissociates interfacial water molecules (H2Oads), while the resultant H* intermediates preferentially adsorb on Cu sites. Both Tafel and Heyrovsky pathways contribute to H-2 generation, mediated by H2Oads, H*, and OH- through the Cu-CuO interface. This work demonstrates valence-state tuning as an effective strategy for enhancing H2O dissociation and optimizing key intermediates, offering valuable insights for designing superior electrocatalysts.

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