缺陷单层二硒化钒析氧还原电催化性能的密度泛函理论研究

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL
Rabia Hassan , Rehan Hassan , Fei Ma
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引用次数: 0

摘要

在电驱动的水裂解过程中,缓慢的析氧反应(OER)严重阻碍了析氢反应(HER)。本文利用带D3校正的密度泛函理论(DFT-D3)探讨了缺陷单层VSe2在析氧反应(OER)和氧还原反应(ORR)中的电催化电位。在2D-VSe2中引入了固有点缺陷,如硒(D1)和钒(D2)空位。研究了OER和ORR中间体(O, OH和OOH)的可能位点,如Se Top, V Top,空位和桥位。具有V空位(D2)的VSe2单层膜OER/ORR过电位显著降低(η= 0.19 V/0.46 V),表明其催化活性增强。具有V空位(D2) (η= 0.19 V)的VSe2单层膜的OER性能优于IrO2和RuO2 (η= 0.37 V和0.56 V), ORR性能(η= 0.46 V)与贵重Pt (η=0.4 V)相当。Pourbaix图进一步证实了VSe2在各种pH环境下的水稳定性,确立了其作为OER和ORR催化剂的潜力。这些发现表明,缺陷工程,特别是钒空位,可以显著提高VSe2单层电催化活性,有助于高性能电催化剂的开发。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Density functional theory study on the electrocatalytic performance of defected monolayer vanadium diselenide for oxygen evolution and reduction reactions

Density functional theory study on the electrocatalytic performance of defected monolayer vanadium diselenide for oxygen evolution and reduction reactions
The slow oxygen evolution reaction (OER) in the water-splitting driven by electricity, significantly impedes the hydrogen evolution reaction (HER). In this paper, density functional theory with D3 correction (DFT-D3) is utilized to explore the electrocatalytic potential of defected mono-layered VSe2 for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Intrinsic point defects, such as, selenium (D1) and vanadium (D2) vacancies, are introduced into 2D-VSe2. Possible sites, like, Se Top, V Top, vacancies and bridge positions are investigated for OER and ORR intermediates (O, OH and OOH). VSe2 monolayer with V vacancy (D2) shows significantly reduced overpotential for OER/ORR (η= 0.19 V/0.46 V), indicating enhanced catalytic activity. The OER performances of VSe2 monolayer with V vacancy (D2) (η= 0.19 V) surpasses those of IrO2 and RuO2 (η= 0.37 V and 0.56 V), and the ORR performances (η= 0.46 V) are comparable to those of precious Pt (η=0.4 V). The Pourbaix diagram further confirms the aqueous stability of VSe2 in various pH environments, establishing its potential as a robust catalyst for OER and ORR. These findings suggest that defect engineering, particularly vanadium vacancies, could significantly improve the electrocatalytic activity of VSe2 monolayers, contributing to the development of high-performance electrocatalysts.
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来源期刊
Surface Science
Surface Science 化学-物理:凝聚态物理
CiteScore
3.30
自引率
5.30%
发文量
137
审稿时长
25 days
期刊介绍: Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.
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