Fan Zhaobo, Guo Xin, Jin Zhiliang, Li Xin, Li Youji
School of Chemistry and Chemical Engineering, Ningxia Key Laboratory of Solar Chemical Conversion Technology, Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University, Yinchuan 750021, PR China.
Institute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization, Ministry of Agriculture and Rural Affairs, South China Agricultural University, Guangzhou 510642, PR China.
Langmuir. 2022 Mar 15;38(10):3244-3256. doi: 10.1021/acs.langmuir.1c03379. Epub 2022 Feb 28.
The construction of interfacial effects and chemical bonds between catalysts is one of the effective strategies to facilitate photogenerated electron transfer. A novel hollow cubic CoS is derived from Co-ZIF-9 and the S-C bond is successfully constructed between CoS and g-CN. The S-C bond acts as a bridge for electronic transmission, allowing the rapid transmission of photoelectron to hydrogen evolution active site in CoS. In addition, the results of electrochemical impedance spectroscopy and time-resolved photoluminescence spectroscopy show that the S-C bond acts as a bridge to quickly transfer photogenerated carriers in the composite material, and achieves the effect of high-efficiency hydrogen evolution. The hydrogen production of SgZ-45 reaches 9545 μmol·g in 5 h, which is 53 and 12 times that of g-CN and ZIF-9, respectively. The intrinsic mechanism of photoelectron transfer through S-C bonds can be further confirmed by density functional theory (DFT) calculations. This work provides new insights for building a chemical bond electron transfer bridge between MOF derivatives and nonmetallic photocatalytic materials.
构建催化剂之间的界面效应和化学键是促进光生电子转移的有效策略之一。一种新型的中空立方CoS由Co-ZIF-9衍生而来,并且在CoS和g-CN之间成功构建了S-C键。S-C键作为电子传输的桥梁,使光电子能够快速传输到CoS中的析氢活性位点。此外,电化学阻抗谱和时间分辨光致发光光谱的结果表明,S-C键作为桥梁在复合材料中快速转移光生载流子,并实现了高效析氢的效果。SgZ-45在5小时内的产氢量达到9545 μmol·g,分别是g-CN和ZIF-9的53倍和12倍。通过密度泛函理论(DFT)计算可以进一步证实光电子通过S-C键转移的内在机制。这项工作为在MOF衍生物和非金属光催化材料之间构建化学键电子转移桥提供了新的见解。