Enhancing effects of edge-N in Pt-based carbon support on hydrogen evolution reaction

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces Pub Date : 2024-11-24 DOI:10.1016/j.surfin.2024.105499

Xianyou Luo , Bokai Cao , Muhammad Fayaz , Wende Lai , Baodong Du , Heng Zheng , Xunhui Xiong , Yong Chen

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Abstract

N-doped carbons have been widely employed as support materials for metal-based catalysts. However, the specific impact of edge-N in Pt-based carbon supports for hydrogen evolution reaction (HER) has rarely been systematically studied. In this study, activated carbon (AC) from coconut shells was used as a model support. Edge-N-dominated carbon supports (NAC) were obtained by calcining a mixture of melamine and AC. Furthermore, the NAC was annealed at 1200 °C to generate N-deficient NAC-1200. Structural analyses revealed that the incorporation of edge-N not only reduces the Pt particle size but also enhances Pt dispersion and anchoring. Consequently, the optimized Pt/NAC catalyst demonstrated a smaller overpotential of 44 mV in contrast to Pt/AC (81 mV) and Pt/NAC-1200 (69 mV). Moreover, the Pt/NAC catalyst exhibited a lower activation energy of 27.11 kJ mol^-1 compared to Pt/AC (30.43 kJ mol^-1) during the HER process, along with significantly enhanced HER stability. Theoretical calculations further confirmed the critical role of edge-N species, particularly pyridinic-N, in tuning the electronic structure and reducing the reaction barrier of the Pt/C catalyst, thus greatly enhancing HER performance. This study provides valuable insights for the development of advanced edge-N-dominated carbon supports.

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铂基碳支持物中的边缘-N 对氢气进化反应的促进作用

掺杂 N 的碳已被广泛用作金属催化剂的支撑材料。然而，人们很少系统地研究铂基碳载体中的边缘 N 对氢进化反应（HER）的具体影响。本研究以椰壳活性炭（AC）为模型支撑。通过煅烧三聚氰胺和 AC 的混合物，获得了边缘 N 主导的碳支撑（NAC）。此外，将 NAC 在 1200 °C 下退火，生成缺 N 的 NAC-1200。结构分析表明，边缘 N 的加入不仅减小了铂的粒径，还增强了铂的分散性和锚定性。因此，与 Pt/AC（81 mV）和 Pt/NAC-1200 （69 mV）相比，优化后的 Pt/NAC 催化剂过电位更低，仅为 44 mV。此外，与 Pt/AC（30.43 kJ mol-1）相比，Pt/NAC 催化剂在 HER 过程中的活化能更低，仅为 27.11 kJ mol-1，同时 HER 的稳定性也显著增强。理论计算进一步证实了边缘-N 物种（尤其是吡啶-N）在调整 Pt/C 催化剂的电子结构和降低反应势垒方面的关键作用，从而大大提高了 HER 性能。这项研究为开发先进的边缘-N为主的碳支持物提供了宝贵的启示。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Surfaces and Interfaces Chemistry-General Chemistry

CiteScore

8.50

自引率

6.50%

发文量

753

审稿时长

35 days

期刊介绍： The aim of the journal is to provide a respectful outlet for ''sound science'' papers in all research areas on surfaces and interfaces. We define sound science papers as papers that describe new and well-executed research, but that do not necessarily provide brand new insights or are merely a description of research results. Surfaces and Interfaces publishes research papers in all fields of surface science which may not always find the right home on first submission to our Elsevier sister journals (Applied Surface, Surface and Coatings Technology, Thin Solid Films)