期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 2, 页码 2710-2722出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c19856
关键词
metal-organic frameworks (MOFs); energy transfer in porphyrinic array; photocatalytic CO2 reduction; catalyst immobilization; heterogeneous catalysis
资金
- Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Education [NRF-2014R1A6A1030732]
- MSIT of Republic of Korea [NRF-2017M1A2A2046738]
This study presents a novel porphyrinic metal-organic framework-Re(I) hybrid photocatalyst with high catalytic activity achieved through efficient exciton migration and funneling, as supported by serial photophysical measurements including decisive Stern-Volmer interpretation.
A porphyrinic metal-organic framework (PMOF) known as PCN-222(Zn) was chemically doped with a molecular Re(I) catalyst-bearing carboxylate anchoring group to form a new type of metal-organic framework (MOF)-Re(I) hybrid photocatalyst. The porphyrinic MOF-sensitized hybrid (PMOF/Re) was prepared with an archetypical CO2 reduction catalyst, (L)-Re-I(CO)(3)Cl (Re(I); L = 4,4'-dicarboxylic-2,2'-bipyridine), in the presence of 3 vol % water produced CO with no leveling-off tendency for 59 h to give a turnover number of >= 1893 [1070 +/- 80 mu mol h(-1) (g MOF)(-1)]. The high catalytic activity arises mainly from efficient exciton migration and funneling from photoexcited porphyrin linkers to the peripheral Re(I) catalytic sites, which is in accordance with the observed fast exciton (energy) migration (approximate to 1 ps) in highly ordered porphyrin photoreceptors and the effective funneling into Re(I) catalytic centers in the Re(I)-doped PMOF sample. Enhanced catalytic performance is convincingly supported by serial photophysical measurements including decisive Stern-Volmer interpretation.
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