Pt Single Atoms and Clusters Supported on N-Doped Porous Carbon for Improved Hydrogen Evolution Reaction

IF 5.3 2区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Nano Materials Pub Date : 2024-10-18 DOI:10.1021/acsanm.4c0487910.1021/acsanm.4c04879

Jianfei Lei*, Ying Chen, Kaijie Liu, Shenao Liu, Yang Liu, Shanteng Zhang, Jinmei Wang, Fujing Dong and Yanfei Liu,

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Abstract

Platinum is renowned for its exceptional catalytic performance in the hydrogen evolution reaction (HER), but its high cost and rarity seriously hinder the large-scale application of platinum electrocatalysts. Constructing highly dispersed platinum active sites is an effective strategy to lower the loading of Pt while maintaining high activity. Herein, a highly dispersed Pt catalyst composed of a mixture of single atoms and clusters is synthesized on porous N-doped carbon (Pt/N-PC) derived from renewable peony. The existence of Pt single atoms and clusters was confirmed by combining methods such as aberration-corrected high-angle annular dark field-scanning transmission electron microscopy images (HAADF-STEM), X-ray absorption fine structure (XAFS), and X-ray photoelectron spectroscopy (XPS). The Pt/N-PC catalyst exhibits superior performance compared to the Pt-free catalyst (N-PC) as well as to the commercial 20 wt % Pt/C catalyst. It exhibits an overpotential of just 11 mV at a current density of 10 mA/cm², a Tafel slope of 24.1 mV/dec, and an exceptional long-term durability in acidic environments. Notably, upon optimizing the geometric loading amount of Pt, the optimal catalyst achieves an ultrahigh platinum mass activity of 3.44 A mg^–1_Pt at a potential of −50 mV. This value is approximately 9.5 times greater than that of the commercial 20 wt % Pt/C catalyst (0.36 A mg^–1_Pt).

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掺杂 N 的多孔碳上支持的铂单原子和铂簇可改善氢气进化反应

铂因其在氢进化反应（HER）中的卓越催化性能而闻名于世，但其高昂的成本和稀有性严重阻碍了铂电催化剂的大规模应用。构建高度分散的铂活性位点是在保持高活性的同时降低铂负载的有效策略。本文在可再生牡丹提取的多孔 N 掺杂碳（Pt/N-PC）上合成了一种由单个原子和团簇混合组成的高分散铂催化剂。通过结合像差校正高角度环形暗场扫描透射电子显微镜图像（HAADF-STEM）、X射线吸收精细结构（XAFS）和X射线光电子能谱（XPS）等方法，证实了铂单原子和铂团簇的存在。与无铂催化剂（N-PC）以及 20 wt % Pt/C 催化剂相比，Pt/N-PC 催化剂表现出更优越的性能。在电流密度为 10 mA/cm2 时，它的过电位仅为 11 mV，塔菲尔斜率为 24.1 mV/dec，并且在酸性环境中具有卓越的长期耐久性。值得注意的是，在优化铂的几何负载量后，最佳催化剂在 -50 mV 电位下达到了 3.44 A mg-1Pt 的超高铂质量活性。该值约为 20 wt % Pt/C 催化剂（0.36 A mg-1Pt）的 9.5 倍。

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来源期刊

ACS Applied Nano Materials Multiple-

CiteScore

8.30

自引率

3.40%

发文量

1601

期刊介绍： ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.