Scholarlink

<p>Exploring earth-abundant, highly active bifunctional electrocatalysts for efficient hydrogen and oxygen evolution is crucial for water splitting. However, due to their distinct free energies and conducting behaviors (electron/hole), balancing the catalytic efficiency between hydrogen and oxygen evolution remains challenging for achieving bifunctional electrocatalysts. Here, we report a locally-doped MoS<sub>2</sub> monolayer with an in-plane heterostructure acting as a bifunctional electrocatalyst and apply it to the overall water splitting. In this heterostructure, the core region contains Mo/S vacancies, while the ring region was doped by Fe atoms (in two substitution configurations: 1Fe<sub>Mo</sub> and 3Fe<sub>Mo</sub>-V<sub>S</sub> clusters) with a p-type conductive characteristic. Our micro-cell measurements, combined with density functional theory (DFT) calculations, reveal that the vacancies-rich core region presents remarkable hydrogen evolution reaction (HER) activity while the Fe-doped ring gives an excellent oxygen evolution reaction (OER) activity, thus forming an in-plane bifunctional electrocatalyst. Finally, as a proof-of-concept for overall water splitting, we constructed a full-cell configuration based on a locally-doped MoS<sub>2</sub> monolayer, which achieved a cell voltage of 1.87&#xa0;V at 10&#xa0;mA·cm<sup>−2</sup>, demonstrating outstanding performance in strong acid electrolytes. Our work provides insight into the hetero-integration of bifunctional electrocatalysts at the atomic level, paving the way for designing transition metal dichalcogenide catalysts with activity-manipulated regions capable of multiple reactions.</p> Graphical abstract <p></p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Locally-doped MoS2 monolayer with in-plane bifunctional heterostructure toward overall water splitting

  • 期刊论文

  • 发表日期：

    2025年2月18日

查看全文
  • Zhuo-Jun Duan,
  • Hang Xia,
  • Han-Ze Li,
  • Gong-Lei Shao,
  • Yi-Zhang Ren,
  • Xuan Tang,
  • Qiu-Nan Liu,
  • Jin-Hua Hong,
  • Sheng Dai,
  • Yung-Chang Lin,
  • Kazu Suenaga,
  • Yong-Min He,
  • Song Liu

摘要

Exploring earth-abundant, highly active bifunctional electrocatalysts for efficient hydrogen and oxygen evolution is crucial for water splitting. However, due to their distinct free energies and conducting behaviors (electron/hole), balancing the catalytic efficiency between hydrogen and oxygen evolution remains challenging for achieving bifunctional electrocatalysts. Here, we report a locally-doped MoS2 monolayer with an in-plane heterostructure acting as a bifunctional electrocatalyst and apply it to the overall water splitting. In this heterostructure, the core region contains Mo/S vacancies, while the ring region was doped by Fe atoms (in two substitution configurations: 1FeMo and 3FeMo-VS clusters) with a p-type conductive characteristic. Our micro-cell measurements, combined with density functional theory (DFT) calculations, reveal that the vacancies-rich core region presents remarkable hydrogen evolution reaction (HER) activity while the Fe-doped ring gives an excellent oxygen evolution reaction (OER) activity, thus forming an in-plane bifunctional electrocatalyst. Finally, as a proof-of-concept for overall water splitting, we constructed a full-cell configuration based on a locally-doped MoS2 monolayer, which achieved a cell voltage of 1.87 V at 10 mA·cm−2, demonstrating outstanding performance in strong acid electrolytes. Our work provides insight into the hetero-integration of bifunctional electrocatalysts at the atomic level, paving the way for designing transition metal dichalcogenide catalysts with activity-manipulated regions capable of multiple reactions.

Graphical abstract