Ultrafine Ruthenium Nanoparticles Anchored on S,N-Codoped Carbon Nanofibers for H2 and Electricity Coproduction

IF 7.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yaxin Lai, Lvlv Ji*, Jianying Wang*, Jiangnan Shen, Junbin Liao, Xiaoyang He, Tao Wang, Zuofeng Chen and Sheng Wang*, 
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Abstract

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.

Abstract Image

锚定在 S、N-掺杂碳纳米纤维上的超细钌纳米粒子用于生产 H2 和电能
开发节能型氢气(H2)生产系统和高效电催化剂非常重要,但也极具挑战性。在此,我们报告了通过电纺丝辅助方法原位锚定在 S,N-掺杂碳纳米纤维(Ru@SNCNFs)上的超细钌(Ru)纳米粒子的合理设计与合成。在氢气进化反应(HER)和肼氧化反应(HzOR)中,Ru@SNCNFs 的催化性能优于 20% Pt/C 催化剂和大多数文献中的 Ru 基催化剂。将 Ru@SNCNFs 用作双功能电催化剂时,通过将 HER 和 HzOR 分别整合到 0.5 M H2SO4 和 1 M KOH 和 0.5 M N2H4 中,构建了一种不对称燃料电池。值得注意的是,它通过进一步收集电化学中和能量,同时实现了 H2 和电力的共生。密度泛函理论计算合理地解释了金属与支持物之间的相互作用,电子从 Ru 纳米粒子转移到 S、N-掺杂碳基质,从而改变了中间产物的结合特性,提高了内在活性。
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来源期刊
ACS Sustainable Chemistry & Engineering
ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.80
自引率
4.80%
发文量
1470
审稿时长
1.7 months
期刊介绍: ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.
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