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Cooperative Syngas Production and C−N Bond Formation in One Photoredox Cycle
Author(s) -
Han Chuang,
Li YueHua,
Li JingYu,
Qi MingYu,
Tang ZiRong,
Xu YiJun
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202015756
Subject(s) - syngas , dehydrogenation , chemistry , redox , catalysis , photoredox catalysis , catalytic cycle , photochemistry , chemical engineering , partial oxidation , photocatalysis , combinatorial chemistry , inorganic chemistry , organic chemistry , engineering
Solar‐driven syngas production by CO 2 reduction provides a sustainable strategy to produce renewable feedstocks. However, this promising reaction often suffers from tough CO 2 activation, sluggish oxidative half‐reaction kinetics and undesired by‐products. Herein, we report a function‐oriented strategy of deliberately constructing black phosphorus quantum dots‐ZnIn 2 S 4 (BP/ZIS) heterostructures for solar‐driven CO 2 reduction to syngas, paired with selectively oxidative C−N bond formation, in one redox cycle. The optimal BP/ZIS heterostructure features the enhanced charge‐carrier separation and enriched active sites for cooperatively photocatalytic syngas production with a tunable ratio of CO/H 2 and efficient oxidation of amines to imines with high conversion and selectivity. This prominent catalytic performance arises from the efficient electronic coupling between black phosphorus quantum dots and ZnIn 2 S 4 , as well as the optimized adsorption strength for key reaction intermediates, as supported by both experimental and theoretical investigations. We also demonstrate a synergistic interplay between CO 2 reduction and amine dehydrogenation oxidation, rather than simply collecting these two single half‐reactions in this dual‐functional photoredox system.