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“Enzymatic” Photoreduction of Carbon Dioxide using Polymeric Metallofoldamers Containing Nickel–Thiolate Cofactors
Author(s) -
Thanneeru Srinivas,
Nganga John K.,
Amin Alireza Shirazi,
Liu Ben,
Jin Lei,
AngelesBoza Alfredo M.,
He Jie
Publication year - 2017
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201601661
Subject(s) - intramolecular force , nickel , artificial photosynthesis , cofactor , active center , chemistry , polymer , copolymer , thiol , photochemistry , enzyme , polymer chemistry , active site , combinatorial chemistry , catalysis , stereochemistry , organic chemistry , photocatalysis
The photoreduction of CO 2 by using enzyme‐mimicking polymeric metallofoldamers containing Ni–thiolate cofactors was explored. Metallofoldamers consisting of folded polymers incorporated with Ni–thiolate complexes were prepared by intramolecular Ni–thiolate coordination with thiol‐functionalized linear copolymers. The folded polymer backbone may resemble the protein framework to provide a second coordination environment to the active sites. We showed that Ni–metallofoldamers were superiorly active and selective for CO 2 photoreduction. At 80 °C, the turnover frequency of the Ni–metallofoldamers could reach 0.69 s −1 , which corresponds to 2500 turnovers per hour per Ni site. Our findings are expected to provide useful guidelines to investigate artificial enzymes and to understand the role of protein frameworks in photosynthesis.