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高边缘选择性原位电化学 Pt 沉积在富边缘层状 WS 纳米片上。

High Edge Selectivity of In Situ Electrochemical Pt Deposition on Edge-Rich Layered WS Nanosheets.

机构信息

Soochow Institute for Energy and Materials InnovationS, College of Physics, Optoelectronics and Energy, Soochow University, Suzhou, 215006, China.

Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Soochow University, Suzhou, 215006, China.

出版信息

Adv Mater. 2018 Feb;30(7). doi: 10.1002/adma.201704779. Epub 2017 Dec 22.

Abstract

Recent studies show that the Pt electrode can be slowly dissolved into the acidic media and regenerate on the working electrode along with the long-time hydrogen evolution reaction (HER) test. However, to date, the relationship between the Pt deposition and the intrinsic properties of the working electrode remains elusive. Herein, for the first time, the edge selectivity of in situ electrochemical Pt deposition on layered 2H-WS nanosheets, whose edge surface with rich dangling bonds is chemically active to regulate their properties, especially the interfacial reaction occurring between the electrode surface and the adjacent thin layer of the solution, is theoretically elucidated and experimentally verified by controlling the cathode polarization test using Pt wire as the counter electrode in H SO solution. It is revealed that the layered WS nanosheets with rich exposed edges show much stronger interaction with Pt atoms because the terminated S or S ligands on the edge exhibit much lower binding energy for Pt atoms compared with the apical S ligands on the terrace surface. The in situ electrochemical Pt-deposited WS nanosheets with rich exposed edges can act as a highly active hybrid electrocatalyst to accelerate HER kinetics and exhibit commercial Pt-like HER performance, especially in the alkaline media.

摘要

最近的研究表明,Pt 电极可以在酸性介质中缓慢溶解,并在长时间的析氢反应(HER)测试中在工作电极上重新生成。然而,迄今为止,Pt 沉积与工作电极的固有性质之间的关系仍然难以捉摸。在此,首次通过控制使用 Pt 丝作为对电极在 H2SO4溶液中的阴极极化测试,从理论上阐明并通过实验验证了层状 2H-WS 纳米片上原位电化学 Pt 沉积的边缘选择性,其边缘表面具有丰富的悬空键,具有化学活性,可以调节其性质,特别是在电极表面和相邻溶液薄层之间发生的界面反应。结果表明,具有丰富暴露边缘的层状 WS 纳米片与 Pt 原子具有更强的相互作用,因为边缘上终止的 S 或 S 配体与 Pt 原子的结合能比平台表面上的顶 S 配体低得多。具有丰富暴露边缘的原位电化学 Pt 沉积 WS 纳米片可以作为一种高活性的混合电催化剂来加速 HER 动力学,并表现出类似于商业 Pt 的 HER 性能,特别是在碱性介质中。

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