An Efficient, Visible-Light-Driven, Hydrogen Evolution Catalyst NiS/Znx Cd1-x S Nanocrystal Derived from a Metal-Organic Framework.
An Efficient, Visible-Light-Driven, Hydrogen Evolution Catalyst NiS/Znx Cd1-x S Nanocrystal Derived from a Metal-Organic Framework.
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DOI：
10.1002/anie.201805425
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发表时间：
2018-07
影响因子：
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通讯作者：
Xiuxia Zhao;Jianrui Feng;Jing Liu;Wei Shi;Guang-ming Yang;Gui-Chang Wang;P. Cheng
中科院分区：
文献类型：
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作者：
Xiuxia Zhao;Jianrui Feng;Jing Liu;Wei Shi;Guang-ming Yang;Gui-Chang Wang;P. Cheng
光催化水分解制氢利用可持续的阳光是一个有前途的替代工业制氢。然而，高活性、可回收、廉价的光催化剂的缺乏阻碍了光催化析氢反应（HER）方案的发展。本文采用金属-有机框架(MOF)-模板策略制备了具有优异光催化HER活性的非贵金属助催化剂/固溶体异质结NiS/Znx Cd1-x S。通过调节mof中掺杂金属的浓度，可以微调异质结的化学成分和带隙，进一步优化其光吸收能力和光催化活性。NiS/Zn0.5 Cd0.5 S在可见光（λ>420 nm）照射下的最佳HER率为16.78 mmol g-1 h-1，具有较高的稳定性和可回收性。详细的表征和深入的DFT计算揭示了异质结和光催化活性之间的关系，并证实了NiS在加速水解离动力学方面的重要性，这是光催化HER的关键因素。
Photocatalytic water splitting for hydrogen production using sustainable sunlight is a promising alternative to industrial hydrogen production. However, the scarcity of highly active, recyclable, inexpensive photocatalysts impedes the development of photocatalytic hydrogen evolution reaction (HER) schemes. Herein, a metal-organic framework (MOF)-template strategy was developed to prepare non-noble metal co-catalyst/solid solution heterojunction NiS/Znx Cd1-x S with superior photocatalytic HER activity. By adjusting the doping metal concentration in MOFs, the chemical compositions and band gaps of the heterojunctions can be fine-tuned, and the light absorption capacity and photocatalytic activity were further optimized. NiS/Zn0.5 Cd0.5 S exhibits an optimal HER rate of 16.78 mmol g-1 h-1 and high stability and recyclability under visible-light irradiation (λ>420 nm). Detailed characterizations and in-depth DFT calculations reveal the relationship between the heterojunction and photocatalytic activity and confirm the importance of NiS in accelerating the water dissociation kinetics, which is a crucial factor for photocatalytic HER.