用于高效碱性析氢的 1T0.63-MoSe2@MoP 多相界面催化剂的定向构建,ACS Applied Materials & Interfaces

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用于高效碱性析氢的 1T0.63-MoSe2@MoP 多相界面催化剂的定向构建
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-06-28 , DOI: 10.1021/acsami.2c04093
Chen Li _{1,

2} , Wenting Hong ₁ , Qian Cai ₁ , Chuanyong Jian _{1,

3}

Affiliation

碱性水电解是工业制氢中应用最广泛的技术。然而，作为惰性碱性析氢电催化剂的过渡金属二硫属化物由于不合适的固有电子结构而具有缓慢的水吸附和解离动力学。为了解决这个问题，我们报告了一种多相界面催化剂 (MPIC) 的合成，即 1T _0.63 -MoSe ₂ @MoP (1T = 八面体相；MoSe ₂ = 硒化钼；MoP = 磷化钼)通过多相协同作用的界面电子结构，促进碱性析氢反应（HER）。因此，自立式 1T _0.63 -MoSe ₂@MoP MPIC 需要 358 mV 的小过电势才能在碱性淡水电解质中达到 1000 mA cm ^{–2的大电流密度，同时在人工碱性海水电解质中的大电流密度下具有令人印象深刻的 HER 活性和稳定性。}由于合成过程简单而成熟，这项工作揭示了钼基电催化剂在高电流密度下用于析氢的潜力，这为通过海水电解实现大规模商业制氢提供了愿景。同时，密度泛函理论研究一致证实，MoSe ₂中金属相和本征 HER 活性 MoP 的结合可以成功地调整其电子结构，从而提高 HER 催化活性。

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Directional Construction of a 1T0.63-MoSe2@MoP Multiphase-Interface Catalyst for Highly Efficient Alkaline Hydrogen Evolution

Alkaline water electrolysis is the most widely used technology for industrial hydrogen production. However, transition-metal dichalcogenides as inert alkaline hydrogen evolution electrocatalysts suffer from sluggish water adsorption and dissociation dynamics originating from the inappropriate intrinsic electronic structure. To address this issue, we report the synthesis of a type of multiphase-interface catalyst (MPIC), 1T_0.63-MoSe₂@MoP (1T = octahedral phase; MoSe₂ = molybdenum selenide; MoP = molybdenum phosphide), that tunes the intrinsic interfacial electronic structure by multiphase synergy, promoting the alkaline hydrogen evolution reaction (HER). Consequently, the self-standing 1T_0.63-MoSe₂@MoP MPIC requires a small overpotential of 358 mV to reach a large current density of 1000 mA cm^–2 in an alkaline freshwater electrolyte, along with impressive HER activity and stability at large current densities in an artificial alkaline seawater electrolyte. This work unravels the potential of Mo-based electrocatalysts for hydrogen evolution at high current densities, owing to the simple and mature synthesis process, which offers a vision to enable large-scale commercial hydrogen generation by seawater electrolysis. Meanwhile, density functional theory studies consistently confirm that the combination of metallic phase and intrinsic HER-active MoP in MoSe₂ could successfully tune its electronic structure to improve the HER catalytic activity.

更新日期：2022-06-28

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