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Ultrafine Ruthenium Nanoparticles Anchored on S,N-Codoped Carbon Nanofibers for H2 and Electricity Coproduction
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2024-11-13 , DOI: 10.1021/acssuschemeng.4c07973
Yaxin Lai, Lvlv Ji, Jianying Wang, Jiangnan Shen, Junbin Liao, Xiaoyang He, Tao Wang, Zuofeng Chen, Sheng Wang

The development of an energy-saving hydrogen (H2) production system and efficient electrocatalysts is of high importance but challenging. Herein, we report the rational design and synthesis of ultrafine ruthenium (Ru) nanoparticles in situ anchored on S,N-codoped carbon nanofibers (Ru@SNCNFs) by an electrospinning-assisted method. For both the hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR), Ru@SNCNFs demonstrate superior catalytic performances compared to a 20% Pt/C catalyst and most Ru-based catalysts in literatures. When Ru@SNCNFs are applied as bifunctional electrocatalysts, an asymmetric fuel cell is constructed by integrating HER in 0.5 M H2SO4 and HzOR in 1 M KOH and 0.5 M N2H4. Remarkably, it achieves simultaneously H2 and electricity coproduction by further harvesting the electrochemical neutralization energy. Density functional theory calculations rationalize the metal–support interaction with electron transfer from Ru nanoparticles to S,N-codoped carbon matrix, therefore modifying the binding characteristics of intermediates toward the intrinsic activity enhancement.

中文翻译:


锚定在 S,N 共掺杂碳纳米纤维上的超细钌纳米颗粒用于 H2 和电力共产



开发节能的氢气 (H2) 生产系统和高效的电催化剂非常重要,但也具有挑战性。在此,我们报道了通过静电纺丝辅助方法原锚定在 S,N 共掺杂碳纳米纤维 (Ru@SNCNFs) 上的超细钌 (Ru) 纳米颗粒的合理设计和合成。对于析氢反应 (HER) 和肼氧化反应 (HzOR),与 20% Pt/C 催化剂和文献中的大多数 Ru 基催化剂相比,Ru@SNCNFs表现出优异的催化性能。当Ru@SNCNFs用作双功能电催化剂时,通过将 HER 集成到 0.5 M H2SO4 和 HzOR 中,构建了 1 M KOH 和 0.5 M N2H4 中的 HzOR。值得注意的是,它通过进一步收集电化学中和能同时实现 H2 和电的共产。密度泛函理论计算使金属-载体相互作用合理化,电子从 Ru 纳米颗粒转移到 S,N 共掺碳基体,从而改变中间体的结合特性,以实现本征活性增强。
更新日期:2024-11-13
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