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Abstract The electrocatalytic hydrogen evolution reaction (HER) is one of the most studied and promising processes for hydrogen fuel generation. Single-atom catalysts have been shown to exhibit ultra-high HER catalytic activity, but the harsh preparation conditions and the low single-atom loading hinder their practical applications. Furthermore, promoting hydrogen evolution reaction kinetics, especially in alkaline electrolytes, remains as an important challenge. Herein, Pt/C60catalysts with high-loading, high-dispersion single-atomic platinum anchored on C60are achieved through a room-temperature synthetic strategy. Pt/C60-2 exhibits high HER catalytic performance with a low overpotential (η10) of 25 mV at 10 mA cm−2. Density functional theory calculations reveal that the Pt-C60polymeric structures in Pt/C60-2 favors water adsorption, and the shell-like charge redistribution around the Pt-bonding region induced by the curved surfaces of two adjacent C60facilitates the desorption of hydrogen, thus favoring fast reaction kinetics for hydrogen evolution.
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This content will become publicly available on August 1, 2025
Ultrasmall and Highly Dispersed Pt Entities Deposited on Mesoporous N‐doped Carbon Nanospheres by Pulsed CVD for Improved HER
Abstract Vapor‐based deposition techniques are emerging approaches for the design of carbon‐supported metal powder electrocatalysts with tailored catalyst entities, sizes, and dispersions. Herein, a pulsed CVD (Pt‐pCVD) approach is employed to deposit different Pt entities on mesoporous N‐doped carbon (MPNC) nanospheres to design high‐performance hydrogen evolution reaction (HER) electrocatalysts. The influence of consecutive precursor pulse number (50‐250) and deposition temperature (225–300 °C) are investigated. The Pt‐pCVD process results in highly dispersed ultrasmall Pt clusters (≈1 nm in size) and Pt single atoms, while under certain conditions few larger Pt nanoparticles are formed. The best MPNC‐Pt‐pCVD electrocatalyst prepared in this work (250 pulses, 250 °C) reveals a Pt HER mass activity of 22.2 ± 1.2 A mg−1Ptat ‐50 mV versus the reversible hydrogen electrode (RHE), thereby outperforming a commercially available Pt/C electrocatalyst by 40% as a result of the increased Pt utilization. Remarkably, after optimization of the Pt electrode loading, an ultrahigh Pt mass activity of 56 ± 2 A mg−1Ptat ‐50 mV versus RHE is found, which is among the highest Pt mass activities of Pt single atom and cluster‐based electrocatalysts reported so far.
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- PAR ID:
- 10584848
- Publisher / Repository:
- Wiley-VCH GmbH
- Date Published:
- Journal Name:
- Small
- Volume:
- 20
- Issue:
- 34
- ISSN:
- 1613-6810
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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