Stable Heterometallic Cluster-Based Organic Framework Catalysts for Artificial Photosynthesis |
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| Authors: | Long-Zhang Dong Lei Zhang Dr. Jiang Liu Qing Huang Meng Lu Dr. Wen-Xin Ji Prof. Ya-Qian Lan |
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| Affiliation: | 1. Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, No. 1, Wenyuan Road, Nanjing, 210023 China;2. State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering, Ningxia University, Yinchuan, 750021 China |
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| Abstract: | A series of stable heterometallic Fe2M cluster-based MOFs ( NNU-31-M , M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. The heterometallic cluster units and photosensitive ligands excited by visible light generate separated electrons and holes. Then, low-valent metal M accepts electrons to reduce CO2, and high-valent Fe uses holes to oxidize H2O. This is the first MOF photocatalyst system to finish artificial photosynthetic full reaction. It is noted that NNU-31-Zn exhibits the highest HCOOH yield of 26.3 μmol g−1 h−1 (selectivity of ca. 100 %). Furthermore, the DFT calculations based on crystal structures demonstrate the photocatalytic reaction mechanism. This work proposes a new strategy for how to design crystalline photocatalyst to realize artificial photosynthetic overall reaction. |
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| Keywords: | Heterometallische Katalysatoren Kohlendioxid-Reduktion Metall-organische Gerüste Photokatalysatoren |
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