Kinetic-Oriented Construction of MoS2 Synergistic Interface to Boost pH-Universal Hydrogen Evolution
Kinetic-Oriented Construction of MoS2 Synergistic Interface to Boost pH-Universal Hydrogen Evolution
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动力学导向构建 MoS2 协同界面以促进 pH 通用析氢
DOI：
10.1002/adfm.201908520
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发表时间：
2019-12-09
影响因子：
19
通讯作者：
Yang, Shihe
中科院分区：
文献类型：
--
作者：
Hu, Jue;Zhang, Chengxu;Yang, Shihe
作为未来可持续能源经济的先决条件，设计在酸性和碱性环境下具有相当的析氢催化性能的地球丰富的MoS2催化剂仍然是一个紧迫的挑战。降低能量壁垒可以增强催化剂的活性，但这通常不是一种策略。在这里，通过基于界面附近 Ni、Co 和 Mo 3d 能带偏移的同步调制来优化电子结构，提出了第一个基于 MoS2 的动力学导向设计，用于 pH 通用析氢催化。得益于这种理想的电子结构，所获得的MoS2/CoNi2S4催化剂在10 mA cm(-2)下实现了78和81 mV的超低过电势，在碱性和酸性介质中在200 mV过电势下分别实现了高达2.7和1.7 s(-1)的转换频率。 MoS2/CoNi2S4催化剂是迄今为止在碱性和酸性环境下报道的MoS2基催化剂中析氢反应表现最好的催化剂之一，同样重要的是在酸和碱中在10 mA cm(-2)下保持48 h后具有显着的长期稳定性，活性损失可以忽略不计。这项工作凸显了深入理解和合理设计用于未来能量存储和输送的高效 pH 通用电催化剂的潜力。
As a prerequisite for a sustainable energy economy in the future, designing earth-abundant MoS2 catalysts with a comparable hydrogen evolution catalytic performance in both acidic and alkaline environments is still an urgent challenge. Decreasing the energy barriers could enhance the catalysts' activity but is not often a strategy for doing so. Here, the first kinetic-oriented design of the MoS2-based heterostructure is presented for pH-universal hydrogen evolution catalysis by optimizing the electronic structure based on the simultaneous modulation of the 3d-band-offsets of Ni, Co, and Mo near the interface. Benefiting from this desirable electronic structure, the obtained MoS2/CoNi2S4 catalyst achieves an ultralow overpotential of 78 and 81 mV at 10 mA cm(-2), and turnover frequency as high as 2.7 and 1.7 s(-1) at the overpotential of 200 mV in alkaline and acidic media, respectively. The MoS2/CoNi2S4 catalyst represents one of the best hydrogen evolution reaction performing ones among MoS2-based catalysts reported to date in both alkaline and acidic environments, and equally important is the remarkable long-term stability with negligible activity loss after maintaining at 10 mA cm(-2) for 48 h in both acid and base. This work highlights the potential to deeply understand and rationally design highly efficient pH-universal electrocatalysts for future energy storage and delivery.