TY - JOUR
T1 - 2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO2 Reduction
AU - Yang, Sizhuo
AU - Hu, Wenhui
AU - Zhang, Xin
AU - He, Peilei
AU - Pattengale, Brian
AU - Liu, Cunming
AU - Cendejas, Melissa
AU - Hermans, Ive
AU - Zhang, Xiaoyi
AU - Zhang, Jian
AU - Huang, Jier
N1 - Funding Information:
S.Y. J.H., X.Z., and J.Z. thank the support from National Science Foundation (CBET-1706971). Use of the Advanced Photon Source and TEM at Center for Nanomaterials at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science Office of Basic Energy Sciences, under Award No. DE-AC02-06CH11357.
Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/11/7
Y1 - 2018/11/7
N2 - Covalent organic framework (COF) represents an emerging class of porous materials that have exhibited great potential in various applications, particularly in catalysis. In this work, we report a newly designed 2D COF with incorporated Re complex, which exhibits intrinsic light absorption and charge separation (CS) properties. We show that this hybrid catalyst can efficiently reduce CO2 to form CO under visible light illumination with high electivity (98%) and better activity than its homogeneous Re counterpart. More importantly, using advanced transient optical and X-ray absorption spectroscopy and in situ diffuse reflectance spectroscopy, we unraveled three key intermediates that are responsible for CS, the induction period, and rate limiting step in catalysis. This work not only demonstrates the potential of COFs as next generation photocatalysts for solar fuel conversion but also provide unprecedented insight into the mechanistic origins for light-driven CO2 reduction.
AB - Covalent organic framework (COF) represents an emerging class of porous materials that have exhibited great potential in various applications, particularly in catalysis. In this work, we report a newly designed 2D COF with incorporated Re complex, which exhibits intrinsic light absorption and charge separation (CS) properties. We show that this hybrid catalyst can efficiently reduce CO2 to form CO under visible light illumination with high electivity (98%) and better activity than its homogeneous Re counterpart. More importantly, using advanced transient optical and X-ray absorption spectroscopy and in situ diffuse reflectance spectroscopy, we unraveled three key intermediates that are responsible for CS, the induction period, and rate limiting step in catalysis. This work not only demonstrates the potential of COFs as next generation photocatalysts for solar fuel conversion but also provide unprecedented insight into the mechanistic origins for light-driven CO2 reduction.
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U2 - 10.1021/jacs.8b09705
DO - 10.1021/jacs.8b09705
M3 - Article
C2 - 30352504
AN - SCOPUS:85056138881
VL - 140
SP - 14614
EP - 14618
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 44
ER -