期刊
SCIENTIFIC REPORTS
卷 7, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41598-017-00574-1
关键词
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资金
- Global Frontier R&D Program of the Center for Hybrid Interface Materials (HIM) [2013M3A6B1078884]
- Korea Center of the Artificial Photosynthesis [2009-0093881]
- National Research Foundation of Korea - Ministry of Science, ICT & Future Planning [2016R1A2B3012053]
- Basic Science Research Program through the National Research Foundation of Korea [2016R1C1B1010781]
- National Research Foundation of Korea [2016R1A2B3012053] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
A metal-organic framework (MOF) is composed of secondary building units (SBUs) of metal ions and organic ligands to link each SBU. Moreover, the photosynthetic synthesis of a valuable CO chemical from carbon dioxide (CO2) represents an important class of appealing methods. Herein, we find that a molecular photocatalyst with high selectivity and activity can be designed via a fine balance in the proximity of Re complex (ReI(CO)(3)(BPYDC)(Cl), BPYDC = 2,2'-bipyridine-5,5'-dicarboxylate) and -NH2 functionalized multiple ligands composing a MOF photocatalyst, denoted as Re-MOF-NH2. These ligands in Re-MOF-NH2 has been confirmed by infrared, UV-visible, and H-1 nuclear magnetic resonance spectra. Moreover, we show from extended X-ray absorption fine structure and in-situ infrared spectra that the bond corresponding to Re-CO upon introduction of-NH2 functional groups is divided into asymmetric bonds of 1.4 angstrom and 2.3 angstrom along with different CO2 vibrations, thus making the configuration of carbonyl groups in a Re metal complex become asymmetric in addition to aiding formation of CO2 intermediates within Re-MOF-NH2. Indeed, both of the uneven electron distribution in asymmetric carbonyl groups for Re-CO and the intermolecular stabilization of carbamate intermediates are proven to give the approximately 3-fold increase in photocatalytic activity for conversion of CO2 into CO.
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