Effect of bias in Argon Plasma on Electronic Structure of Electrocatalyst Pt/CNT for Hydrogen Evolution Reaction

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2025-02-04 DOI:10.1007/s10562-025-04944-7

Chang Liu, Yanlei Liu, Hongmei Sun, Nan Yu, Guohua Ni

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Abstract

Electronic structure engineering provides an effective route to enhance the mass activity and stability of Pt-based catalysts. In this paper, platinum nanoparticles supported on carbon nanotubes (Pt/CNTs) are prepared by treating the H₂PtCl₆/CNT precursor with argon plasma at different bias. Extensive structural characterization indicates that, compared with positive and zero bias of the substrate, negative bias causes the most defects in CNTs (I_D/I_G = 1.11), results in the lowest valence state of Pt, and achieves the highest Pt loading (4.9 wt%). Meanwhile, the synthesized Pt/CNTs at negative bias (Pt/CNT-V₋) demonstrate significant catalytic activity and exceptional stability in the hydrogen evolution reaction (HER). The Pt/CNT-V₋ catalyst exhibits an overpotential of 45 mV at a current density of 10 mA cm^− 2 and a mass activity of 3.28 A mg^− 1 for the HER in 0.5 M H₂SO₄, surpassing the performance of commercial JM-Pt/C. The overpotential of the Pt/CNT-V₋ catalyst only negatively shifts by 3 mV after 3000 cycles, compared to the 9 mV shift observed for JM-Pt/C. This simple method provides a new strategy for tuning the electronic properties of metals on carbon carriers.

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氩等离子体中偏压对析氢Pt/CNT电催化剂电子结构的影响

电子结构工程为提高pt基催化剂的质量活性和稳定性提供了有效途径。本文采用不同偏压的氩等离子体处理H2PtCl6/CNT前驱体，制备了负载在碳纳米管上的铂纳米颗粒。广泛的结构表征表明，与衬底的正偏压和零偏压相比，负偏压导致CNTs中缺陷最多（ID/IG = 1.11），导致Pt的最低价态，并获得最高的Pt负载（4.9 wt%）。同时，在负偏压下合成的Pt/CNTs （Pt/CNT-V−）在析氢反应（HER）中表现出显著的催化活性和优异的稳定性。Pt/CNT-V -催化剂在电流密度为10 mA cm - 2时的过电位为45 mV，在0.5 M H2SO4中，HER的质量活度为3.28 a mg - 1，超过了商业JM-Pt/C的性能。在3000次循环后，Pt/CNT-V -催化剂的过电位仅负移3mv，而JM-Pt/C催化剂的过电位负移9mv。这种简单的方法为调整碳载体上金属的电子特性提供了一种新的策略。图形抽象

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.