Yu Yongzhuo, Li Wei, Yang Huixing, Wei Qiuming, Hou Linlin, Wu Zhiliang, Jiang Yangyang, Lv Chaoyu, Huang Yuxin, Tang Jiyu
Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials, Guangdong Engineering Technology Research Center of Efficient Green Energy and Environmental Protection Materials, School of Physics and Telecommunication Engineering, School of Electronic and Information Engineering, South China Normal University, Guangzhou 510006, PR China.
Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials, Guangdong Engineering Technology Research Center of Efficient Green Energy and Environmental Protection Materials, School of Physics and Telecommunication Engineering, School of Electronic and Information Engineering, South China Normal University, Guangzhou 510006, PR China.
J Colloid Interface Sci. 2023 Dec;651:221-234. doi: 10.1016/j.jcis.2023.07.210. Epub 2023 Aug 1.
The construction of heterojunction systems is an effective way to efficiently generate hydrogen by water photolysis. In this work, Ni-MOF (trimesic acid, (BTC)) and g-CN (denoted as CN) were combined, and then Ni-MOF/CN was modified by 4-Methyl-5-vinyl thiazole (denoted as MVTh). Finally, CdS was loaded on the surface of Ni-MOF/CN/MVTh to prepare the photocatalyst Ni-MOF/g-CN/MVTh/CdS (denoted as Ni/CN/M/Cd) with a triangular closed-loop path heterojunction for the first time. As a photocatalyst without precious metal cocatalysts, Ni/CN/M/Cd displayed high H evolution (17.844 mmol·g·h) under an optimum CdS loading of 40 wt%. The H evolution rate was approximately 79 times that of Ni-MOF/CN and exceeded those of almost all catalysts based on MOF/CN in the literature. The triangular closed-loop heterojunction formed between Ni-MOF, g-CN, and CdS could realize the directional migration of photocarriers and significantly diminished the transfer resistance of carriers. The Ni in Ni-MOF provided many cocatalytic sites for H evolution via g-CN and CdS. Furthermore, charge carrier separation in Ni-MOF/CN/CdS improved after the innovative addition of MVTh. This study provides a reference for the construction of a closed-loop heterojunction system without precious metal cocatalysts.
构建异质结体系是通过水光解高效产氢的有效途径。在本工作中，将镍基金属有机框架（均苯三甲酸，（BTC））与石墨相氮化碳（记为CN）复合，然后用4-甲基-5-乙烯基噻唑（记为MVTh）对Ni-MOF/CN进行改性。最后，将硫化镉负载在Ni-MOF/CN/MVTh表面，首次制备出具有三角形闭环路径异质结的光催化剂Ni-MOF/g-CN/MVTh/CdS（记为Ni/CN/M/Cd）。作为一种不含贵金属助催化剂的光催化剂，在40 wt%的最佳硫化镉负载量下，Ni/CN/M/Cd表现出高析氢量（17.844 mmol·g·h）。析氢速率约为Ni-MOF/CN的79倍，超过了文献中几乎所有基于MOF/CN的催化剂。Ni-MOF、g-CN和CdS之间形成的三角形闭环异质结能够实现光生载流子的定向迁移，并显著降低载流子的转移电阻。Ni-MOF中的镍通过g-CN和CdS为析氢提供了许多共催化位点。此外，创新性地添加MVTh后，Ni-MOF/CN/CdS中的电荷载流子分离得到改善。本研究为构建无贵金属助催化剂的闭环异质结体系提供了参考。
