<p>The integration of urea oxidation reaction (UOR) and hydrogen evolution reaction (HER) into urea electrolysis can concurrently accomplish energy-conserving hydrogen (H<sub>2</sub>) production and the treatment of urea-contaminated wastewater. Central to achieving this goal is the development of efficient and cost-effective bifunctional electrocatalysts. In this study, a novel one-pot green strategy was developed for the in-situ synthesis of molybdenum-doped Ni<sub>3</sub>S<sub>2</sub> nanorods on nickel foam (Mo-Ni<sub>3</sub>S<sub>2</sub>/NF), serving as an efficient bifunctional electrocatalyst for the UOR and HER. The incorporation of Mo effectively modulates both the morphological and electronic structure of Ni<sub>3</sub>S<sub>2</sub>, bringing a substantial increase in accessible active sites and a marked improvement in charge transfer efficiency. Notably, to deliver a current density of 10&#xa0;mA cm<sup>-2</sup>, the Mo-Ni<sub>3</sub>S<sub>2</sub>/NF three-dimensional electrode requires merely 1.339&#xa0;V (UOR) and 0.138&#xa0;V (HER) when tested in 1.0&#xa0;M KOH containing 0.5&#xa0;M urea, underscoring its remarkable catalytic activity. Moreover, the Mo-Ni<sub>3</sub>S<sub>2</sub>/NF based urea electrolyzer attains 10&#xa0;mA cm<sup>-2</sup> at merely 1.477&#xa0;V and shows excellent durability over 48&#xa0;h. Density functional theory (DFT) calculations indicate enhanced electron cloud density near the Fermi level relative to undoped Ni<sub>3</sub>S<sub>2</sub>, demonstrating that Mo doping improves both conductivity and carrier density. Our finding provides a new way to design efficient bifunctional catalysts for urea-assisted energy-efficiency H<sub>2</sub> production.</p>

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Mo doping with morphology regulation of Ni3S2 as efficient bifunctional electrocatalysts for urea-assisted hydrogen generation

  • Feng Jing,
  • Zhen Liu,
  • Bo Cheng,
  • Sihan Fu,
  • Zhiyi Wang,
  • Hongying Mei,
  • Kangwen Qiu

摘要

The integration of urea oxidation reaction (UOR) and hydrogen evolution reaction (HER) into urea electrolysis can concurrently accomplish energy-conserving hydrogen (H2) production and the treatment of urea-contaminated wastewater. Central to achieving this goal is the development of efficient and cost-effective bifunctional electrocatalysts. In this study, a novel one-pot green strategy was developed for the in-situ synthesis of molybdenum-doped Ni3S2 nanorods on nickel foam (Mo-Ni3S2/NF), serving as an efficient bifunctional electrocatalyst for the UOR and HER. The incorporation of Mo effectively modulates both the morphological and electronic structure of Ni3S2, bringing a substantial increase in accessible active sites and a marked improvement in charge transfer efficiency. Notably, to deliver a current density of 10 mA cm-2, the Mo-Ni3S2/NF three-dimensional electrode requires merely 1.339 V (UOR) and 0.138 V (HER) when tested in 1.0 M KOH containing 0.5 M urea, underscoring its remarkable catalytic activity. Moreover, the Mo-Ni3S2/NF based urea electrolyzer attains 10 mA cm-2 at merely 1.477 V and shows excellent durability over 48 h. Density functional theory (DFT) calculations indicate enhanced electron cloud density near the Fermi level relative to undoped Ni3S2, demonstrating that Mo doping improves both conductivity and carrier density. Our finding provides a new way to design efficient bifunctional catalysts for urea-assisted energy-efficiency H2 production.