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<p>Water electrolysis has emerged as the preferred solution for “green energy” production, and the current key bottleneck lies in inadequate bifunctional activity and stability. In this work, heterostructured MoN@Mo<sub>2</sub>N was synthesized by a rapid CO<sub>2</sub> laser-induced strategy, which exhibits excellent bifunctional electrochemical activity for alkaline overall water splitting. The MoN@Mo<sub>2</sub>N catalyst delivers the overpotential of 35 and 280 mV to achieve 10 mA cm<sup>−2</sup> under alkaline condition, respectively, and only 1.52 V of cell voltage is needed for overall water splitting. The anion exchange membrane water electrolysis (AEMWE) system was also assembled, operating for 350 h under the current density at 1 A cm<sup>−2</sup> (industrial level) without obvious degradation at a cell voltage of 1.96 V. The interfacial work function difference drives the construction of a built-in electric field (BIEF), rendering directional electron transfer from MoN to Mo<sub>2</sub>N. <i>In-situ</i> Raman spectroscopy and theoretical calculations indicate that *H adsorption on the heterostructured interface could be regulated, which follows a hydrogen spillover mechanism for hydrogen evolution reaction (HER), in which Mo<sub>2</sub>N contributes to promoting H<sub>2</sub>O activation and serves as a *H reservoir, and MoN could be responsible for the favorable H<sub>2</sub> formation. Additionally, the BIEF leads to optimized intermediate adsorption and reaction energy barrier on the hetero-MoN by modulating d-p orbital coupling, which breaks the intrinsic limitation of the linear scaling relationship and enables promoted OER catalytic activity. This research may provide vital foundations for the large-scale application of hydrogen production and shed new light on the rational design and fabrication of bifunctional electrocatalysts for water electrolysis.</p>

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Hydrogen spillover and d-p orbital coupling regulation: interfacial built-in electric fields on heterostructured MoN@Mo2N trigger efficient overall water splitting

  • 期刊论文

  • 发表日期：

    2026年7月24日

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  • Jiawei Wang,
  • Tingxue Fang,
  • Yuhao Wang,
  • Chuanfu Su,
  • Honghai Sun,
  • Nan Wang,
  • Dong Xiang,
  • Kedi Cai

摘要

Water electrolysis has emerged as the preferred solution for “green energy” production, and the current key bottleneck lies in inadequate bifunctional activity and stability. In this work, heterostructured MoN@Mo2N was synthesized by a rapid CO2 laser-induced strategy, which exhibits excellent bifunctional electrochemical activity for alkaline overall water splitting. The MoN@Mo2N catalyst delivers the overpotential of 35 and 280 mV to achieve 10 mA cm−2 under alkaline condition, respectively, and only 1.52 V of cell voltage is needed for overall water splitting. The anion exchange membrane water electrolysis (AEMWE) system was also assembled, operating for 350 h under the current density at 1 A cm−2 (industrial level) without obvious degradation at a cell voltage of 1.96 V. The interfacial work function difference drives the construction of a built-in electric field (BIEF), rendering directional electron transfer from MoN to Mo2N. In-situ Raman spectroscopy and theoretical calculations indicate that *H adsorption on the heterostructured interface could be regulated, which follows a hydrogen spillover mechanism for hydrogen evolution reaction (HER), in which Mo2N contributes to promoting H2O activation and serves as a *H reservoir, and MoN could be responsible for the favorable H2 formation. Additionally, the BIEF leads to optimized intermediate adsorption and reaction energy barrier on the hetero-MoN by modulating d-p orbital coupling, which breaks the intrinsic limitation of the linear scaling relationship and enables promoted OER catalytic activity. This research may provide vital foundations for the large-scale application of hydrogen production and shed new light on the rational design and fabrication of bifunctional electrocatalysts for water electrolysis.