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<p>The apparent OER activity on S-incorporated catalyst outputs an over-estimated current, which is actually contributed not only from the oxygen evolution reaction (OER), but also from the inevitable surface reconstruction-involved electrochemical oxidation reactions. The mechanism of such catalysts still remains complex and controversial. Here, we applied a set of <i>operando</i> electrochemical-spectrometric methodologies to investigate the precise interfacial activation process on the bimetallic sulfide heterogeneous catalyst, which delivers an extraordinary OER activity of 100 mA cm<sup>−2</sup> at 190 mV overpotential. Differential electrochemical mass spectrometry (DEMS) suggested the electrochemical oxidations of the lattice S to SO, SO<sub>2</sub> and SO<sub>4</sub><sup>2−</sup> species and the coordinately unsaturated metal sites. <i>Operando</i> Raman and attenuated total reflectance surface-enhanced infrared absorption spectra confirmed the phase transformation of sulfide to oxide, and then to oxyhydroxide, which acted as an active site for OER. The density functional theory also simulated this process by showing that the (CoNi)<sub><i>x</i></sub>S<sub><i>y</i></sub> transition phase exhibited the optimal activity, and elucidated the attenuation kinetics of the apparent activity during OER. This study demonstrates the structure evolution of a certain S-incorporated catalyst and establishes the protocol for the real activity identification under the real-time reaction.</p>

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Disclosing the intrinsic electrocatalytic activity of transition-metal sulfides for enhanced water oxidation

  • 期刊论文

  • 发表日期：

    2025年4月15日

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  • Dan Zhu,
  • Lingxing Zan,
  • Yunchuan Tu,
  • Wenlin Zhang,
  • Hongling Zhang,
  • Yuxin Luo,
  • Lu Liu,
  • Jiawen Zheng,
  • Qiang Weng,
  • Qingbo Wei,
  • Di Li,
  • Xin Bo,
  • Chuan Zhao,
  • Feng Fu

摘要

The apparent OER activity on S-incorporated catalyst outputs an over-estimated current, which is actually contributed not only from the oxygen evolution reaction (OER), but also from the inevitable surface reconstruction-involved electrochemical oxidation reactions. The mechanism of such catalysts still remains complex and controversial. Here, we applied a set of operando electrochemical-spectrometric methodologies to investigate the precise interfacial activation process on the bimetallic sulfide heterogeneous catalyst, which delivers an extraordinary OER activity of 100 mA cm−2 at 190 mV overpotential. Differential electrochemical mass spectrometry (DEMS) suggested the electrochemical oxidations of the lattice S to SO, SO2 and SO42− species and the coordinately unsaturated metal sites. Operando Raman and attenuated total reflectance surface-enhanced infrared absorption spectra confirmed the phase transformation of sulfide to oxide, and then to oxyhydroxide, which acted as an active site for OER. The density functional theory also simulated this process by showing that the (CoNi)xSy transition phase exhibited the optimal activity, and elucidated the attenuation kinetics of the apparent activity during OER. This study demonstrates the structure evolution of a certain S-incorporated catalyst and establishes the protocol for the real activity identification under the real-time reaction.