<p>Alkaline water electrolysis poses significant potential for large-scale industrial hydrogen generation, but is impeded by the absence of an efficient electrocatalyst capable of operating at high current densities while maintaining with minimal overpotential. Herein, we construct a mechanically stable and highly active RuSe<sub>2</sub>/MXene heterojunction electrocatalyst. A typical SC-Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> MXene substrate was successfully prepared by supercritical CO<sub>2</sub> (SC-CO<sub>2</sub>) etching, combined by subsequent DMSO intercalation treatment. Further, the RuSe<sub>2</sub> nanoparticles were uniformly deposited on the surface of SC-Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub>. Theoretical calculations and experimental results demonstrate that fluorine-rich MXene exhibits stable binding with the active 1T phase RuSe<sub>2</sub>. The as-prepared representative RuSe<sub>2</sub>@SC-Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub>-3 heterostructure showed exceptional alkaline hydrogen evolution performance, demonstrating an overpotential of 15&#xa0;mV at 10&#xa0;mA&#xa0;cm<sup>−2</sup> and a Tafel slope of 21.84&#xa0;mV&#xa0;dec<sup>−1</sup>, which presents excellent HER performance and stability at high-current-density conditions. Moreover, the overpotential under the current density of 500&#xa0;mA&#xa0;cm<sup>−2</sup> is merely 182&#xa0;mV, and the HER efficiency remains unaffected even after 5000 cycles and 120&#xa0;h of continuous testing.</p> Graphical abstract <p>A novel protocol is proposed for etching Ti3AlC2 MAX phase depending on the supercritical CO2 and ZnF2·4H<sub>2</sub>O as an effective etchant to fabricate MXene with enriched F delamination. The F-rich MXene exhibits stronger interactions with the active 1T phase RuSe2, thereby significantly enhancing the electrocatalytic activity and stability under high current density.</p>

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Supercritical CO2 etching MXene for RuSe2 coating as high-efficiency alkaline hydrogen evolution reaction catalyst

  • Shi-Long Han,
  • Qing-Yong Tian,
  • Bo Gao,
  • Xiao-Qing Sui,
  • Hong-Po Liu,
  • Wei-Jing Yao,
  • Wen-Zhuo Wu,
  • Qun Xu

摘要

Alkaline water electrolysis poses significant potential for large-scale industrial hydrogen generation, but is impeded by the absence of an efficient electrocatalyst capable of operating at high current densities while maintaining with minimal overpotential. Herein, we construct a mechanically stable and highly active RuSe2/MXene heterojunction electrocatalyst. A typical SC-Ti3C2Tx MXene substrate was successfully prepared by supercritical CO2 (SC-CO2) etching, combined by subsequent DMSO intercalation treatment. Further, the RuSe2 nanoparticles were uniformly deposited on the surface of SC-Ti3C2Tx. Theoretical calculations and experimental results demonstrate that fluorine-rich MXene exhibits stable binding with the active 1T phase RuSe2. The as-prepared representative RuSe2@SC-Ti3C2Tx-3 heterostructure showed exceptional alkaline hydrogen evolution performance, demonstrating an overpotential of 15 mV at 10 mA cm−2 and a Tafel slope of 21.84 mV dec−1, which presents excellent HER performance and stability at high-current-density conditions. Moreover, the overpotential under the current density of 500 mA cm−2 is merely 182 mV, and the HER efficiency remains unaffected even after 5000 cycles and 120 h of continuous testing.

Graphical abstract

A novel protocol is proposed for etching Ti3AlC2 MAX phase depending on the supercritical CO2 and ZnF2·4H2O as an effective etchant to fabricate MXene with enriched F delamination. The F-rich MXene exhibits stronger interactions with the active 1T phase RuSe2, thereby significantly enhancing the electrocatalytic activity and stability under high current density.