相、硫空位和边缘对多孔二硫化钼纳米片析氢反应催化活性的贡献,Journal of the American Chemical Society

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相、硫空位和边缘对多孔二硫化钼纳米片析氢反应催化活性的贡献
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2016-06-21 , DOI: 10.1021/jacs.6b03714
Ying Yin , Jiecai Han , Yumin Zhang , Xinghong Zhang , Ping Xu , Quan Yuan , Leith Samad ₁ , Xianjie Wang , Yi Wang , Zhihua Zhang ₂ , Peng Zhang ₃ , Xingzhong Cao ₃ , Bo Song , Song Jin ₁

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二硫化钼（MoS2）是一种很有前途的析氢反应（HER）非贵金属催化剂，由于其优异的性能而被广泛研究，但对其催化活性的影响因素缺乏了解阻碍了 MoS2-的进一步设计和增强。基于电催化剂。在这里，通过使用由液体氨辅助锂化途径合成的新型多孔（多孔）金属 1T 相 MoS2 纳米片，我们系统地研究了晶体结构（相）、边缘和硫空位（S 空位）对催化的贡献。五种代表性 MoS2 纳米片样品对 HER 的活性，包括 2H 和 1T 相、多孔 2H 和 1T 相以及硫补偿的多孔 2H 相。在多孔 1T 相 MoS2 纳米片中实现了卓越的 HER 催化活性，该纳米片比传统的 1T 相 MoS2 具有更多的边缘和 S 空位。一项比较研究表明，该相在决定 HER 性能方面起着关键作用，因为 1T 相 MoS2 总是优于相应的 2H 相 MoS2 样品，并且边缘和 S 空位也对多孔 MoS2 样品的催化活性有显着贡献. 然后，使用电子自旋共振光谱和正电子湮没寿命光谱的组合缺陷表征技术来量化 S 空位，分别阐明每个因素的贡献。这项研究为设计基于 MoS2 或其他具有增强 HER 性能的层状材料的电催化剂提供了新的见解并开辟了新的途径。

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Contributions of Phase, Sulfur Vacancies, and Edges to the Hydrogen Evolution Reaction Catalytic Activity of Porous Molybdenum Disulfide Nanosheets

Molybdenum disulfide (MoS2) is a promising nonprecious catalyst for the hydrogen evolution reaction (HER) that has been extensively studied due to its excellent performance, but the lack of understanding of the factors that impact its catalytic activity hinders further design and enhancement of MoS2-based electrocatalysts. Here, by using novel porous (holey) metallic 1T phase MoS2 nanosheets synthesized by a liquid-ammonia-assisted lithiation route, we systematically investigated the contributions of crystal structure (phase), edges, and sulfur vacancies (S-vacancies) to the catalytic activity toward HER from five representative MoS2 nanosheet samples, including 2H and 1T phase, porous 2H and 1T phase, and sulfur-compensated porous 2H phase. Superior HER catalytic activity was achieved in the porous 1T phase MoS2 nanosheets that have even more edges and S-vacancies than conventional 1T phase MoS2. A comparative study revealed that the phase serves as the key role in determining the HER performance, as 1T phase MoS2 always outperforms the corresponding 2H phase MoS2 samples, and that both edges and S-vacancies also contribute significantly to the catalytic activity in porous MoS2 samples. Then, using combined defect characterization techniques of electron spin resonance spectroscopy and positron annihilation lifetime spectroscopy to quantify the S-vacancies, the contributions of each factor were individually elucidated. This study presents new insights and opens up new avenues for designing electrocatalysts based on MoS2 or other layered materials with enhanced HER performance.

更新日期：2016-06-21

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