Wang Jin, Xia Tong, Wang Lei, Zheng Xusheng, Qi Zeming, Gao Chao, Zhu Junfa, Li Zhengquan, Xu Hangxun, Xiong Yujie
Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Normal University, Jinhua, Zhejiang, 321004, P. R. China.
Angew Chem Int Ed Engl. 2018 Dec 10;57(50):16447-16451. doi: 10.1002/anie.201810550. Epub 2018 Nov 14.
Quantum dots (QDs), a class of promising candidates for harvesting visible light, generally exhibit low activity and selectivity towards photocatalytic CO reduction. Functionalizing QDs with metal complexes (or metal cations through ligands) is a widely used strategy for improving their catalytic activity; however, the resulting systems still suffer from low selectivity and stability in CO reduction. Herein, we report that doping CdS QDs with transition-metal sites can overcome these limitations and provide a system that enables highly selective photocatalytic reactions of CO with H O (100 % selectivity to CO and CH ), with excellent durability over 60 h. Doping Ni sites into the CdS lattice leads to effective trapping of photoexcited electrons at surface catalytic sites and substantial suppression of H evolution. The method reported here can be extended to various transition-metal sites, and offers new opportunities for exploring QD-based earth-abundant photocatalysts.
量子点（QDs）作为一类有望用于收集可见光的材料，通常对光催化CO还原表现出较低的活性和选择性。用金属配合物（或通过配体的金属阳离子）对量子点进行功能化是提高其催化活性的一种广泛使用的策略；然而，所得体系在CO还原中仍存在选择性低和稳定性差的问题。在此，我们报道，用过渡金属位点掺杂CdS量子点可以克服这些限制，并提供一种能够实现CO与H₂O发生高选择性光催化反应（对CO和CH₄的选择性为100%）的体系，且具有超过60小时的优异耐久性。将Ni位点掺杂到CdS晶格中会导致光激发电子在表面催化位点处有效捕获，并显著抑制H₂析出。本文报道的方法可以扩展到各种过渡金属位点，并为探索基于量子点的储量丰富的光催化剂提供了新的机会。
