<p>Although MoS<sub>2</sub> exhibits promising potential as an electrocatalyst for the hydrogen evolution reaction (HER) due to its phase stability, abundant edge sites, and large specific surface area, its inherently low electrical conductivity results in significant limitations in electron transfer and surface activity. Furthermore, aggregation/stacking and self-curling phenomena further impair its performance. To address these challenges, this study developed a coordination-driven self-assembly strategy to vertically anchor defect-rich MoS<sub>2</sub> nanoflowers onto a graphitic carbon framework exhibiting excellent conductivity. The resulting MoS<sub>2</sub>@C hybrids possess covalent interfacial bonding and three-dimensional nanoarchitecture that synergistically enhance acidic hydrogen evolution performance. <i>In situ</i> coordination of Mo precursors with carbonyl-functionalized carbon enables uniform dispersion of ultrathin petals, exposing abundant edge sites while creating atomically coupled Mo–C heterojunctions to accelerate charge transfer. Structural/spectroscopic analyses confirm a 60&#xa0;wt.% carbon framework that suppresses nanosheet aggregation and stabilizes metallic phases. Consequently, the MoS<sub>2</sub>@60C electrode achieves benchmark performance: 144.6&#xa0;mV overpotential at 10&#xa0;mA·cm<sup>−2</sup>, 50.7&#xa0;mV·dec<sup>−1</sup> Tafel slope, and 87.1% current retention after 100&#xa0;h in 0.5&#xa0;mol·L<sup>−1</sup> H<sub>2</sub>SO<sub>4</sub>, surpassing most MoS<sub>2</sub>-based catalysts. Carbon’s spatial confinement simultaneously mitigates restacking and sulfur leaching while establishing efficient charge-transfer pathways, collectively guaranteeing exceptional electrocatalytic activity and long-term operational stability in proton-exchange-membrane electrolyzers.</p> Graphical abstract <p></p>

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In situ growth of MoS2 nanoflowers on graphitic carbon for efficient hydrogen evolution reaction

  • Fei Zhu,
  • Fan Yang,
  • Li-Li Gao,
  • Lu Dong,
  • Wen-Ting Ye,
  • Jia-Ming Bian,
  • Hua Wang,
  • Ping Hu

摘要

Although MoS2 exhibits promising potential as an electrocatalyst for the hydrogen evolution reaction (HER) due to its phase stability, abundant edge sites, and large specific surface area, its inherently low electrical conductivity results in significant limitations in electron transfer and surface activity. Furthermore, aggregation/stacking and self-curling phenomena further impair its performance. To address these challenges, this study developed a coordination-driven self-assembly strategy to vertically anchor defect-rich MoS2 nanoflowers onto a graphitic carbon framework exhibiting excellent conductivity. The resulting MoS2@C hybrids possess covalent interfacial bonding and three-dimensional nanoarchitecture that synergistically enhance acidic hydrogen evolution performance. In situ coordination of Mo precursors with carbonyl-functionalized carbon enables uniform dispersion of ultrathin petals, exposing abundant edge sites while creating atomically coupled Mo–C heterojunctions to accelerate charge transfer. Structural/spectroscopic analyses confirm a 60 wt.% carbon framework that suppresses nanosheet aggregation and stabilizes metallic phases. Consequently, the MoS2@60C electrode achieves benchmark performance: 144.6 mV overpotential at 10 mA·cm−2, 50.7 mV·dec−1 Tafel slope, and 87.1% current retention after 100 h in 0.5 mol·L−1 H2SO4, surpassing most MoS2-based catalysts. Carbon’s spatial confinement simultaneously mitigates restacking and sulfur leaching while establishing efficient charge-transfer pathways, collectively guaranteeing exceptional electrocatalytic activity and long-term operational stability in proton-exchange-membrane electrolyzers.

Graphical abstract