Wei Jieding, Luo Dian, Shi Manman, Guo Saiya, Lu Zhou, Ni Yonghong
College of Chemistry and Materials Science, Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, Anhui Normal University, 189 Jiuhua Southern Road, Wuhu 241002, P. R. China.
School of Physics and Electronic Information, Anhui Normal University, 189 Jiuhua Southern Road, Wuhu 241002, P. R. China.
Inorg Chem. 2024 Oct 28;63(43):20820-20829. doi: 10.1021/acs.inorgchem.4c03601. Epub 2024 Oct 9.
Efficient utilization of photogenerated charge carriers to realize photocatalytic solar fuel production and oxidative chemical synthesis is a challenging task. Herein, a conventional amidation reaction route is adopted to successfully construct a novel composite photocatalyst composed of a Ni(II)-terpyridine complex with carboxyl groups grafted on CdS nanorods (labeled as CdS@Ni(terpyC)). Experimental results have unequivocally revealed that the as-fabricated composite catalyst exhibited a remarkable enhancement in photocatalytic activity for the dehydrogenation of benzyl alcohol under visible light, demonstrating superior hydrogen evolution efficiency and benzaldehyde selectivity, surpassing both pristine CdS and the blend of CdS and Ni(terpyC). The carrier dynamics study demonstrated that the Ni(terpyC) on the surface of CdS could quickly extract the photogenerated electrons of CdS, which reduced the carrier recombination efficiency, further improving the photocatalytic activity of the catalyst. This work illustrates the effect of surface active site engineering on photocatalysis and is expected to shed substantial inspiration on future surface modulation and design of semiconductor photocatalysts.
有效利用光生电荷载流子以实现光催化太阳能燃料生产和氧化化学合成是一项具有挑战性的任务。在此,采用传统的酰胺化反应路线成功构建了一种新型复合光催化剂,该催化剂由接枝在CdS纳米棒上的带有羧基的Ni(II)-三联吡啶配合物组成(标记为CdS@Ni(terpyC))。实验结果明确表明,所制备的复合催化剂在可见光下对苯甲醇脱氢的光催化活性有显著增强,展现出优异的析氢效率和苯甲醛选择性,超过了原始CdS以及CdS与Ni(terpyC)的混合物。载流子动力学研究表明,CdS表面的Ni(terpyC)能够快速提取CdS的光生电子,降低了载流子复合效率,进一步提高了催化剂的光催化活性。这项工作阐明了表面活性位点工程对光催化的影响,有望为未来半导体光催化剂的表面调制和设计提供重要启示。