Ru-Cd/碳纳米管双功能电催化剂用于氢氧化和析氢反应

Ru-Cd/Carbon nanotube Bifunctional Electrocatalysts for Hydrogen Oxidation and Hydrogen Evolution Reaction

  • 摘要: 实现高效催化析氢反应(Hydrogen Evolution Reaction,HER)和氢氧化反应(Hydrogen Oxidation Reaction,HOR)对于构建氢经济,推动社会可持续发展具有重要的意义。金属钌(Ru)凭借其固有的高亲氧特性,被认为是一种极具发展前景的碱性氢电催化剂。本文通过引入过渡金属镉(Cd)来调控Ru的表面电子结构,优化Ru对吸附态活性氢(H*)和羟基(OH*)结合能,并有效促进电子转移,成功开发出一种低Ru含量的碳纳米管负载Ru-Cd复合材料(Ru-Cd/CNT)。电化学性能测试表明,该材料在HOR和HER中均展现出高效且稳定的催化性能。在0.1 mol/L KOH电解液进行HOR性能测试,在50 mV的过电位下(vs. RHE),Ru-Cd/CNT的几何动力学电流密度(jk)可达16.31 mA·cm−2,分别为商业Pt/C和Ru/C催化剂的5倍和9倍,其几何交换电流密度(j0)达到2.05 mA·cm−2,亦优于商业Pt/C和Ru/C催化剂。在HER测试中,当电流密度为10 mA·cm−2时,Ru-Cd/CNT的析氢过电位仅为34 mV,远低于商业Pt/C(65 mV)和Ru/C催化剂(60 mV)。此外,Ru-Cd/CNT在碱性HOR/HER测试过程中均展示出优异的CO耐受性和稳定性:在0.1% CO存在下运行2000 s,电流密度衰减仅为8%;连续运行12000 s后,电流密度衰减仅10%,均优于商业Pt/C和Ru/C催化剂。该研究为开发高性能、可持续的氢氧燃料电池电极材料提供了新的思路和重要参考。

     

    Abstract: Achieving efficient electrocatalysis for the Hydrogen Evolution Reaction (HER) and Hydrogen Oxidation Reaction (HOR) is of great significance for establishing a hydrogen economy and promoting sustainable social development. Ruthenium (Ru), with its inherent high oxophilicity, is regarded as a highly promising electrocatalyst for alkaline hydrogen electrocatalysis. In this work, transition metal cadmium (Cd) was introduced to regulate the surface electronic structure of Ru, optimize the binding energies of adsorbed active hydrogen (H*) and hydroxyl (OH*) on Ru, and effectively promote electron transfer. A carbon-nanotube-supported Ru–Cd composite (Ru–Cd/CNT) with low Ru loading was successfully fabricated. Electrochemical measurements demonstrate that the as-prepared catalyst exhibits highly efficient and stable catalytic performance toward both HOR and HER. In 0.1 mol/L KOH electrolyte for HOR, the Ru–Cd/CNT catalyst achieves a geometric kinetic current density (jk) of 16.31 mA·cm−2 at an overpotential of 50 mV (vs. RHE), which is 5 and 9 times higher than those of commercial Pt/C and Ru/C catalysts, respectively. Its geometric exchange current density (j0) reaches 2.05 mA·cm−2, also superior to commercial Pt/C and Ru/C. For HER, Ru–Cd/CNT delivers an overpotential of only 34 mV at a current density of 10 mA·cm−2, much lower than commercial Pt/C (65 mV) and Ru/C (60 mV). Furthermore, Ru–Cd/CNT shows excellent CO tolerance and stability in alkaline HOR/HER measurements: the current density decreases by only 8% after 2000 s operation in the presence of 0.1% CO, and by merely 10% after 12000 s continuous operation, both outperforming commercial Pt/C and Ru/C. This study provides a new strategy and important reference for developing high-performance and sustainable electrode materials for hydrogen–oxygen fuel cells.

     

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