Zhao Xiuxia, Feng Jianrui, Liu Jing, Shi Wei, Yang Guangming, Wang Gui-Chang, Cheng Peng
Key Laboratory of Advanced Energy Material Chemistry (MOE), College of Chemistry, Nankai University, Tianjin, 300071, P. R. China.
Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Nankai University, Tianjin, 300071, P. R. China.
Angew Chem Int Ed Engl. 2018 Jul 26;57(31):9790-9794. doi: 10.1002/anie.201805425. Epub 2018 Jul 2.
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/Zn Cd 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/Zn Cd S exhibits an optimal HER rate of 16.78 mmol g h 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.
利用可持续阳光进行光催化水分解制氢是工业制氢的一种有前景的替代方法。然而，高活性、可回收、廉价的光催化剂的稀缺阻碍了光催化析氢反应（HER）方案的发展。在此，开发了一种金属有机框架（MOF）模板策略来制备具有优异光催化HER活性的非贵金属助催化剂/固溶体异质结NiS/Zn Cd S。通过调节MOF中的掺杂金属浓度，可以微调异质结的化学成分和带隙，并进一步优化光吸收能力和光催化活性。NiS/Zn Cd S在可见光照射（λ>420 nm）下表现出16.78 mmol g h的最佳HER速率以及高稳定性和可回收性。详细的表征和深入的DFT计算揭示了异质结与光催化活性之间的关系，并证实了NiS在加速水解离动力学中的重要性，这是光催化HER的关键因素。
