期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 6, 页码 2073-2077出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201509744
关键词
coordination polymer; copper; dyes; pigments; hydrogen; photochemistry
资金
- National Natural Science Foundation of China [21371153]
- Program for Science & Technology Innovation Talents in Universities of Henan Province [13HASTIT008]
- Key Scientific and Technological Project of Henan Province [132102210411]
- Zhengzhou University
A crystalline coordination polymer (CP) photocatalyst (Cu-RSH) which combines redox-active copper centers with photoactive rhodamine-derived ligands remains stable in acid and basic solutions from pH2 to 14, and efficiently catalyzes dihydrogen evolution at a maximum rate of 7.88mmolg(-1)h(-1) in the absence of a mediator and a co-catalyst. Cyclic voltammetry, control experiments, and DFT calculations established that copper nodes with open coordination sites and favorable redox potentials, aided by spatially ordered stacking of rhodamine-based linkers, account for the high catalytic performance of Cu-RSH. Emission quenching, time-resolved fluorescence decay, and transient photocurrent experiments disclosed the charge separation and transfer process in the catalytic system. The present study demonstrates the potential of crystalline copper CPs for the practical utilization of light.
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