用表面离子修饰 1T-MoS2 以实现电催化氢进化反应

Lulu Chen, Yichao Huang, Limin Wang, Sixuan Huang, Zhuangjun Fan
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摘要

二硫化钼(MoS2)被认为是氢进化反应(HER)中一种蓬勃发展且具有成本效益的电催化剂。遗憾的是,2H-MoS2 半导体相本身具有保守的电子本征传输速率,且活性位点局限于边缘区域,导致氢进化反应的电催化性能不尽如人意。在此,我们采用水热法制备了高导电性金属相 1T-MoS2 纳米片,并通过原位还原策略在其表面引入了一系列过渡金属离子,实现了 MoS2 的表面改性。研究发现,金属 Ni 和 Co 不仅增强了 1T-MoS2 的本征电导率,还显著增加了催化剂中活性位点的数量,从而使催化剂表现出优异的 HER 活性。在 1.0 M KOH 介质中,Ni@1T-MoS2 表现出快速的反应动力学(86 mV-dec-1)、良好的机械稳定性(约 28 h)和低能耗,并且在 50 mA-cm-2 条件下过电位仅为 187 mV。
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Modification 1T-MoS2 with surface ions towards electrocatalytic hydrogen evolution reaction
Molybdenum disulfide (MoS2) is considered as a thriving and cost-efficient electrocatalyst for hydrogen evolution reaction (HER). Unfortunately, the semiconductor phase of 2H-MoS2 itself has a conservative electronic intrinsic transport rate and the restricted active sites to edge regions, leading to unsatisfactory electrocatalytic performance of HER. Here, we have fabricated highly conductive metal phase 1T-MoS2 nanosheets by a hydrothermal method and introduced a series of transition metal ions on their surfaces by an in-situ reduction strategy to achieve MoS2 surface modification. It was found that the metals Ni and Co not only enhanced the intrinsic conductivity of 1T-MoS2, but also significantly increased the number of active sites in the catalyst, which resulted in the catalyst exhibiting excellent HER activity. Ni@1T-MoS2 exhibits fast reaction kinetics (86 mV·dec-1), good mechanical stability (~28 h) and low energy consumption in 1.0 M KOH medium, as well as an over-potential of only 187 mV at 50 mA·cm-2.
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