Beneficial surface defect engineering of MoS2 electrocatalyst for efficient hydrogen evolution reaction

IF 4.1 3区 化学 Q1 CHEMISTRY, ANALYTICAL Journal of Electroanalytical Chemistry Pub Date : 2024-11-19 DOI:10.1016/j.jelechem.2024.118814
Jyoti Ganapati Badiger , Maheswari Arunachalam , Rohini Subhash Kanase , Suzan Abdelfattah Sayed , Kwang-Soon Ahn , Soon Hyung Kang
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Abstract

Hydrogen evolution reaction (HER) is considered the most efficient method for hydrogen production using an effective electrocatalyst. Molybdenum disulfide (MoS2), with its unique 2D layered structure, is the most promising electrocatalyst. This is attributed to its flexibility, which facilitates the exploration of various MoS2 phases and properties, closely mirroring those of platinum, particularly its Gibbs energy (ΔGH* ̃ 0.08 eV), which makes MoS2 an excellent electrocatalyst. However, its low electrical conductivity and inert basal planes limit its effectiveness for HER. This study utilized a facile hot-gun approach to successfully introduce sulfur vacancies, simultaneously incorporating oxygen from the air, which partially occupied these vacancies. This process resulted in the formation of an intermediate MoOxSy interlayer, yielding a highly effective electrocatalyst. Exposure to the hot gun for a short duration led to several changes, notably expanding the interlayer spacing and altering the atomic S:O ratio from approximately 75 % to 57 %, primarily affecting the MoS2 structure. The optimal duration for hot-gun treatment was determined to be 30 s, enhancing electrochemical activity for HER, with an overpotential of 486 mV vs. RHE (briefly marked as VRHE) at a current density of 10 mA·cm−2 and Tafel slope of 224 mV·dec-1. The improvement in basal active sites, attributable to the formation of defects from sulfur vacancies and partial passivation by oxygen at these sites, was identified as the key factor for this enhanced performance.
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有利于高效氢进化反应的 MoS2 电催化剂表面缺陷工程
氢进化反应(HER)被认为是使用有效电催化剂制氢的最有效方法。二硫化钼(MoS2)具有独特的二维层状结构,是最有前途的电催化剂。这要归功于它的灵活性,这种灵活性有助于探索 MoS2 的各种相态和特性,这些相态和特性与铂的相态和特性密切相关,特别是它的吉布斯能(ΔGH* ̃ 0.08 eV),这使得 MoS2 成为一种极佳的电催化剂。然而,MoS2 的低导电性和惰性基底面限制了其在 HER 方面的有效性。本研究利用简便的热枪方法成功引入了硫空位,同时从空气中引入了氧,部分占据了这些空位。这一过程形成了中间的 MoOxSy 夹层,产生了一种高效的电催化剂。短时间暴露在热风枪下会导致几种变化,特别是扩大层间间距和改变原子 S:O 比率,从大约 75% 降至 57%,主要影响 MoS2 结构。热枪处理的最佳持续时间为 30 秒,可提高 HER 的电化学活性,在电流密度为 10 mA-cm-2、塔菲尔斜率为 224 mV-dec-1 时,相对于 RHE 的过电位为 486 mV(简要标记为 VRHE)。基底活性位点的改善被认为是性能提高的关键因素,这归因于硫空位形成的缺陷以及这些位点上氧的部分钝化。
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来源期刊
CiteScore
7.80
自引率
6.70%
发文量
912
审稿时长
2.4 months
期刊介绍: The Journal of Electroanalytical Chemistry is the foremost international journal devoted to the interdisciplinary subject of electrochemistry in all its aspects, theoretical as well as applied. Electrochemistry is a wide ranging area that is in a state of continuous evolution. Rather than compiling a long list of topics covered by the Journal, the editors would like to draw particular attention to the key issues of novelty, topicality and quality. Papers should present new and interesting electrochemical science in a way that is accessible to the reader. The presentation and discussion should be at a level that is consistent with the international status of the Journal. Reports describing the application of well-established techniques to problems that are essentially technical will not be accepted. Similarly, papers that report observations but fail to provide adequate interpretation will be rejected by the Editors. Papers dealing with technical electrochemistry should be submitted to other specialist journals unless the authors can show that their work provides substantially new insights into electrochemical processes.
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