期刊
ACS NANO
卷 16, 期 8, 页码 12569-12579出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c04113
关键词
WSe2-VSe2 alloy; phase transition; atomic immiscibility; spin-polarized density functional theory; hydrogen evolution reaction
类别
资金
- Korean Ministry of Science and ICT [C140440, 2014R1A6A1030732, 2018R1A2B2006474, 2020R1A6A3A01095689, 2020R1A2C2004392]
- National Research Foundation of Korea [2020R1A6A3A01095689, 2020R1A2C2004392, 2018R1A2B2006474] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
Tuning the electronic structures of transition metal dichalcogenides (TMD) is crucial for their application in energy technologies. The study found that alloying WSe2 and VSe2 can convert the semiconductor material into a metal, accompanied by a phase transition. Additionally, the alloy phase also exhibits improved electrocatalytic activity.
Tuning the electronic structures of transition metal dichalcogenides (TMD) is essential for their implementation in next-generation energy technologies. In this study, we synthesized composition-tuned WSe2-VSe2 (W1-xVxSe2, x = 0-1) alloyed nanosheets using a colloidal reaction. Alloying the semiconducting WSe2 with VSe2 converts the material into a metallic one, followed by a 2H-to-1T phase transition at x = 0.7. Over a wide composition range, WSe2 and VSe2 are atomically immiscible and form separate ordered domains. The miscible alloy at x = 0.1 displayed enhanced electrocatalytic activity toward the hydrogen evolution reaction (HER) in an acidic electrolyte. This trend was correlated with the d-band center via a volcano-type relationship. Spin-polarized density functional theory calculations consistently predicted the atomic immiscibility, which became more significant at the 2H-1T phase transition composition. The Gibbs free energy of H adsorption on the basal planes (Se or hole sites) and the activation barriers along the Volmer-Heyrovsky reaction pathway supported the enhanced HER performance of the alloy phase, suggesting that the dispersed V-doped structures were responsible for the best HER catalytic activity. Our study demonstrates how the atomic structure of TMD alloy nanosheets plays a crucial role in enhancing catalytic activity.
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