The Role of Nitrogen Doping in Modulating Ruthenium Nanocatalysts for Enhanced Electrochemical Hydrogen Evolution Reaction in Alkaline Medium

纳米材料基催化剂 电化学 X射线光电子能谱 过电位 材料科学 碳纤维 无机化学 X射线吸收光谱法 催化作用 碳纳米管 化学工程 化学 吸收光谱法 纳米技术 物理化学 纳米颗粒 电极 有机化学 工程类 物理 复合材料 量子力学 复合数
作者
Lavanya Korampattu,Sidharth Barik,Ajmal Pandikassala,Rajashri Urkude,Sreekumar Kurungot,Paresh L. Dhepe
出处
期刊:Chemistry of Materials [American Chemical Society]
卷期号:36 (9): 4262-4274 被引量:2
标识
DOI:10.1021/acs.chemmater.3c03169
摘要

Nitrogen doping has become a fundamental approach to enhance the catalytic performance of carbon materials across various applications. The introduction of nitrogen creates defects and active sites, promoting the formation of small metal particles and strengthening the metal–support interaction within carbon materials. However, the challenge lies in developing sustainable and cost-effective methods for synthesizing nitrogen-doped carbon materials. In this study, we present a sustainable approach for the synthesis of ruthenium on nitrogen-doped carbon catalysts (Ru-CCP) using chitosan as a nitrogen and carbon source. Unlike traditional methods, our process avoids the use of additional nitrogen precursors and templates, streamlining the synthesis while using a renewable resource. The synthesized material exhibits an exceptional performance in the electrochemical hydrogen evolution reaction (HER) in alkaline conditions by achieving a current density of 25 mA cm–2 at an impressively low overpotential of 46 mV, outperforming Pt/C under similar conditions. The detailed studies on structural and electronic properties of the materials using X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and transmission electron microscopy (TEM) revealed that the remarkable catalytic activity is upheld by the unique interplay between Ruδ+ and surface nitrogen moieties, notably pyridinic and pyrrolic nitrogen. Here, we demonstrate the control of particle size and electronic environment around the metal atom via the interaction of nitrogen and unravel the role of nitrogen doping in tuning the catalytic performance. In addition, this work offers insights into efficient HER catalyst design and emphasizes the potential of biomass-derived materials like chitosan in advancing clean hydrogen production for renewable energy applications.
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