氮空位增强Ru-VN金属-载体相互作用促进酸性和碱性电催化析氢性能

Nitrogen vacancies enhance the Ru-VN metal-support interaction, promoting acidic and basic electrocatalytic hydrogen evolution performance

  • 摘要: 开发高性能、高稳定性和高适用性的钌(Ru)基电催化剂是全解水制氢的关键。采用浸渍–氢气还原法在钒化氮(VN)载体上构建了具有不同氮空位浓度的Ru@VN1−x系列催化剂。结构表征表明,氮空位的引入促进了Ru纳米颗粒的均匀分散,并增强了Ru与VN载体之间的金属–载体电子耦合。电化学测试结果显示,Ru@VN1−x-m在1 mol·L−1 KOH和0.5 mol·L−1 H2SO4中分别仅需46 mV和45 mV的过电位即可达到10 mA·cm−2,并可稳定运行60 h。以该催化剂组装的碱性和酸性整体水分解器件在10 mA·cm−2下所需电压分别为1.54 V和1.58 V,驱动电压显著优于商用RuO2电解池。结果表明,氮空位通过增强Ru与缺陷VN载体之间的相互作用并调控界面电子结构,优化了H*吸附/脱附行为,从而显著提升了宽pH条件下的HER性能。

     

    Abstract: Developing active and stable ruthenium (Ru)-based electrocatalysts with broad applicability is essential for hydrogen production via overall water splitting. We prepared a series of Ru@VN1−x catalysts with varying nitrogen vacancy concentrations on vanadium nitride (VN) supports using an impregnation and hydrogen reduction method. Structural characterization indicates that nitrogen vacancies promote the uniform dispersion of Ru nanoparticles and strengthen the metal-support electronic coupling between Ru and VN. Electrochemical tests show that Ru@VN1−x-m requires overpotentials of only 46 mV and 45 mV to reach 10 mA·cm−2 in 1 mol·L−1 KOH and 0.5 mol·L−1 H2SO4, respectively, operating stably for 60 hours. Alkaline and acidic overall water splitting devices assembled with this catalyst require voltages of 1.54 V and 1.58 V at 10 mA·cm−2, respectively. These driving voltages are lower than those of commercial RuO2 electrolyzers. Nitrogen vacancies enhance the interaction between Ru and the defective VN support and regulate the interfacial electronic structure. This optimizes the H* adsorption and desorption behavior, improving the hydrogen evolution reaction (HER) performance across a wide pH range.

     

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