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<p>Glycerol electrooxidation emerges as an electrochemically cogent paradigm to supplant the sluggish oxygen evolution reaction in water electrolysis. However, most non-precious catalysts still suffer from large electrolytic voltage and poor stability when operating at industrially relevant current densities. Here, we develop a heterostructure catalyst by immobilizing abundant cobalt phosphide (CoP) nanoparticles on conductive cobalt nitride (Co<sub>2</sub>N<sub>0.67</sub>) support, which results in the construction of a strong built-in electric field at the heterointerface. The optimal catalyst demonstrates effective bifunctional catalytic performance, yielding an industrial-level current density of 500 mA cm<sup>−2</sup> at low potentials of −141 mV and 1.44 V for hydrogen evolution and glycerol oxidation, respectively. When integrated into a flow cell system, this catalyst maintains good stability for 260 hours at 1 A cm<sup>−2</sup> (1.67 V) while preserving &gt; 85% Faradaic efficiency for formate production. Both theoretical and experimental analyses substantiate that the built-in electric field drives directional electron transfer from CoP to Co<sub>2</sub>N<sub>0.67</sub>, forming an electron-deficient region at the CoP interface that enriches OH* species, and an electron-rich region at the Co<sub>2</sub>N<sub>0.67</sub> interface, facilitating hydrogen adsorption, thereby expediting the glycerol and H* co-adsorption process. Multiple in-situ spectroscopic characterizations verify the existence of a combined direct/indirect oxidation mechanism for glycerol electrooxidation. This discovery sets the stage for low-voltage hydrogen production by hybrid water splitting using the excess electrical power whenever and wherever available.</p>

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Built-in electric field engineering in Co2N0.67/CoP heterostructures for glycerol electrooxidation-assisted hydrogen production

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月17日

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  • Yong Zhang,
  • Ying Qi,
  • Haiqing Zhou,
  • Yan Zhang,
  • Jingying Sun,
  • Wenqi Ma,
  • Jiayi Hu,
  • Ligang Feng,
  • Fang Yu

摘要

Glycerol electrooxidation emerges as an electrochemically cogent paradigm to supplant the sluggish oxygen evolution reaction in water electrolysis. However, most non-precious catalysts still suffer from large electrolytic voltage and poor stability when operating at industrially relevant current densities. Here, we develop a heterostructure catalyst by immobilizing abundant cobalt phosphide (CoP) nanoparticles on conductive cobalt nitride (Co2N0.67) support, which results in the construction of a strong built-in electric field at the heterointerface. The optimal catalyst demonstrates effective bifunctional catalytic performance, yielding an industrial-level current density of 500 mA cm−2 at low potentials of −141 mV and 1.44 V for hydrogen evolution and glycerol oxidation, respectively. When integrated into a flow cell system, this catalyst maintains good stability for 260 hours at 1 A cm−2 (1.67 V) while preserving > 85% Faradaic efficiency for formate production. Both theoretical and experimental analyses substantiate that the built-in electric field drives directional electron transfer from CoP to Co2N0.67, forming an electron-deficient region at the CoP interface that enriches OH* species, and an electron-rich region at the Co2N0.67 interface, facilitating hydrogen adsorption, thereby expediting the glycerol and H* co-adsorption process. Multiple in-situ spectroscopic characterizations verify the existence of a combined direct/indirect oxidation mechanism for glycerol electrooxidation. This discovery sets the stage for low-voltage hydrogen production by hybrid water splitting using the excess electrical power whenever and wherever available.