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Tuning of Ionic Second Coordination Sphere in Evolved Rhenium Catalyst for Efficient Visible‐Light‐Driven CO 2 Reduction
Author(s) -
Chen KaiHong,
Wang Ning,
Yang ZhiWen,
Xia ShuMei,
He LiangNian
Publication year - 2020
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.202000698
Subject(s) - catalysis , ionic bonding , rhenium , coordination sphere , chemistry , dissociation (chemistry) , photochemistry , ionic liquid , amine gas treating , steric effects , dimer , inner sphere electron transfer , visible spectrum , quantum yield , ion , inorganic chemistry , materials science , organic chemistry , fluorescence , physics , optoelectronics , quantum mechanics
Developing an efficient and easy‐to‐handle strategy in designing catalysts for CO 2 reduction into CO by harnessing sunlight is a promising project. Here, a facile strategy was developed to design a Re catalyst modified with an ionic secondary coordination sphere for photoreduction of CO 2 to CO by visible light. By adding ionic liquids or tuning a different ionic secondary coordination sphere, it was discovered that an outstanding optical property, other than CO 2 absorption ability or the ability to dissociation of chloride anion, is the prerequisite for catalyst design. Accordingly, a novel Re catalyst, {Re[BpyMe(tris(2‐hydroxyethyl)amine)](CO) 3 Cl}Br (Re‐THEA), was designed, screened, and resulted in a relative high quantum yield (up to 34 %) for visible‐light‐induced CO 2 reduction with a single‐molecule system. DFT calculations, combined with experimental outcomes, suggested the pendant ionic tris(2‐hydroxyethyl)amino (THEA) group on Re‐THEA can enhance visible‐light absorption, stabilize reaction intermediates, and suppress the Re–Re dimer formation.