兰亚乾教授课题组在ANGEWANDTE CHEMIE-INTERNATIONAL EDITION发表研究论文

时间:2020-03-23 来源:化科院 点击数:

Stable Heterometallic Cluster-Based Organic Framework Catalysts for Artificial Photosynthesis

Dong, LZ (Dong, Long-Zhang)[ 1 ] ; Zhang, L (Zhang, Lei)[ 1 ] ; Liu, J (Liu, Jiang)[ 1 ]*(刘江); Huang, Q (Huang, Qing)[ 1 ] ; Lu, M (Lu, Meng)[ 1 ] ; Ji, WX (Ji, Wen-Xin)[ 2 ] ; Lan, YQ (Lan, Ya-Qian)[ 1 ]*(兰亚乾)


[ 1 ] Nanjing Normal Univ, Sch Chem & Mat Sci, Jiangsu Key Lab New Power Batteries, Jiangsu Collaborat Innovat Ctr Biomed Funct Mat, 1 Wenyuan Rd, Nanjing 210023, Peoples R China

[ 2 ] Ningxia Univ, State Key Lab High Efficiency Coal Utilizat & Gre, Yinchuan 750021, Peoples R China


ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,202002,59(7),2659-2663


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 O-2 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 mu mol 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.

文章链接:

https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.201913284


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