Wonyoung Lee, Taeyoung Jeong, Kiwon Kim, Jeeyoung Yoo, Joonhee Kang, Byeongyong Lee, Myeongjin Kim
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引用次数: 0
摘要
铂（Pt）单原子催化剂（SAC）是商用铂/碳（C）催化剂的理想替代品，因为它们在氢进化反应（HER）中具有可调的催化活性和最高的原子效率。在此，我们报告了一种氮（N）掺杂的三维（3D）皱褶石墨烯支撑铂SAC（NCG/Pt），它能在酸性介质中高效催化氢进化反应。在电流密度为 10 mA cm-2 时，NCG/Pt 的过电位为 0.11 V，质量活度为 2852.9 A g-1Pt，与 Pt/C 相比，氢（H）生产能力高出 3.6 倍。系统控制的电化学表征以及同步辐射 X 射线吸收光谱（XAS）和 N2 吸附-脱附等温线实验成功地建立了结构-活性关系，而催化性能的增强主要归功于铂吡啶 N4 分子与皱褶石墨烯（CG）支撑之间的协同效应。我们的研究工作为设计一种高效、稳健、坚固的酸性 HER 电催化剂提供了一种合理的方法。
Atomically Dispersed Platinum Supported on Crumpled Graphene Supports for Highly Efficient Hydrogen Evolution Reaction
Platinum (Pt) single-atom catalysts (SACs) are a promising alternative to commercial Pt/carbon (C) catalysts because of their tunable catalytic activity with maximum atomic efficiency for the hydrogen evolution reaction (HER). Herein, we report a nitrogen (N)-doped three-dimensional (3D) crumpled graphene-supported Pt SAC (NCG/Pt) that efficiently catalyzes HER under acidic media. The NCG/Pt demonstrates an overpotential of 0.11 V at a current density of 10 mA cm−2 with a mass activity of 2852.9 A g−1Pt, highlighting its superior 3.6 times greater hydrogen (H) production capacity compared to Pt/C. Systematically controlled electrochemical characterization together with synchrotron-based X-ray absorption spectroscopy (XAS) and N2 adsorption–desorption isotherm experiment successfully established the structure–activity relationship, and the enhanced catalytic performance was mainly attributed to the synergistic effect between the Pt-pyridinic N4 moiety and the crumpled graphene (CG) support. Our work presents a rational approach to designing a highly effective, robust, and efficient electrocatalyst for acidic HER.
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