Rapid hydrogen adsorption-desorption at sulfur sites via an interstitial carbon strategy for efficient HER on MoS2

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-09-05 DOI:10.1016/j.apcatb.2023.122750

Qingqing Zhou , Zhongyuan Wang , Huadong Yuan , Jiade Wang , Hao Hu

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引用次数: 4

Abstract

Molybdenum disulfide (MoS₂), a noble-free material with plentiful unsaturated active edge sites, is expected to replace platinum catalysts for commercial electrocatalytic hydrogen production. However, efficient hydrogen adsorption-desorption processes on sulfur sites with full electron configuration still remain a challenge. Here, vertically oriented self-assembled metallic MoS₂ nanospheres anchored by interstitial atomic carbon (C_ia-MoS₂) are proposed to achieve a rapid hydrogen adsorption-desorption process. In 0.5 M H₂SO₄ solution, C_ia-MoS₂ exhibits fast kinetics (Tafel slope of 45 mV dec⁻¹ and overpotential of 87 mV at 10 mA cm⁻²), as well as a long-term durability over 72 h. As confirmed from X-ray absorption fine spectroscopy and density functional calculations, C_ia significantly optimizes the overall HER performance by reconfiguring the charge landscape and re-splitting the energy level of surface S moiety, which provides a universal strategy for fabricating stable unsaturated 2D catalysts toward HER.

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硫化钼上高效HER的间隙碳策略在硫位点的快速氢吸附-解吸

二硫化钼(MoS2)是一种具有丰富不饱和活性边位的无贵金属材料，有望取代铂催化剂用于商业电催化制氢。然而，高效的氢吸附-解吸过程仍然是一个挑战。本文提出了由间隙原子碳(Cia-MoS2)锚定的垂直取向自组装金属MoS2纳米球，以实现快速的氢吸附-解吸过程。在0.5 M H2SO4溶液中，Cia- mos2表现出快速的动力学(Tafel斜率为45 mV dec−1，过电位为87 mV, 10 mA cm−2)，以及超过72小时的长期耐久性。x射线吸收精细光谱和密度泛函数计算证实，Cia通过重新配置电荷景观和重新分裂表面S部分的能级，显着优化了整体HER性能。这为制备稳定的不饱和二维HER催化剂提供了一种通用策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.