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Rational Design of FeNi Bimetal Modified Covalent Organic Frameworks for Photoconversion of Anthropogenic CO 2 into Widely Tunable Syngas
Author(s) -
Han Bin,
Ou Xinwen,
Zhong Zuqi,
Liang Shujie,
Deng Hong,
Lin Zhang
Publication year - 2020
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.202002985
Subject(s) - syngas , bimetal , catalysis , materials science , metal organic framework , covalent bond , chemical engineering , metal , chemistry , organic chemistry , adsorption , composite material , engineering , metallurgy
Direct photoconversion of low‐concentration CO 2 into a widely tunable syngas (i.e., CO/H 2 mixture) provides a feasible outlet for the high value‐added utilization of anthropogenic CO 2 . However, in the low‐concentration CO 2 photoreduction system, it remains a huge challenge to screen appropriate catalysts for efficient CO and H 2 production, respectively, and provide a facile parameter to tune the CO/H 2 ratio in a wide range. Herein, by engineering the metal sites on the covalent organic frameworks matrix, low‐concentration CO 2 can be efficiently photoconverted into tunable syngas, whose CO/H 2 ratio (1:19–9:1) is obviously wider than reported systems. Experiments and density functional theory calculations indicate that Fe sites serve as the H 2 evolution sites due to the much stronger binding affinity to H 2 O, while Ni sites act as the CO production sites for the higher affinity to CO 2 . Notably, the widely tunable syngas can also be produced over other Fe/Ni‐based bimetal catalysts, regardless of their structures and supporting materials, confirming the significant role of the metal sites in regulating the selectivity of CO 2 photoreduction and providing a modular design strategy for syngas production.