Premium
Stable Heterometallic Cluster‐Based Organic Framework Catalysts for Artificial Photosynthesis
Author(s) -
Dong LongZhang,
Zhang Lei,
Liu Jiang,
Huang Qing,
Lu Meng,
Ji WenXin,
Lan YaQian
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201913284
Subject(s) - photocatalysis , artificial photosynthesis , catalysis , cluster (spacecraft) , photosensitizer , photochemistry , selectivity , yield (engineering) , metal , crystal structure , photosynthesis , chemistry , excited state , materials science , visible spectrum , crystallography , organic chemistry , optoelectronics , physics , biochemistry , computer science , nuclear physics , metallurgy , programming language
A series of stable heterometallic Fe 2 M cluster‐based MOFs ( NNU‐31‐M , M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO 2 and H 2 O 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 CO 2 , and high‐valent Fe uses holes to oxidize H 2 O. 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.
Accelerating Research
Robert Robinson Avenue,
Oxford Science Park, Oxford
OX4 4GP, United Kingdom
Address
John Eccles HouseRobert Robinson Avenue,
Oxford Science Park, Oxford
OX4 4GP, United Kingdom