Electroreduction of CO2 Catalyzed by a
Heterogenized Zn–Porphyrin Complex with a Redox-Innocent Metal
Center
Version 2 2017-08-23, 04:19
Version 1 2017-07-26, 12:12
Posted on 2017-08-23 - 04:19
Transition-metal-based
molecular complexes are a class of catalyst
materials for electrochemical CO2 reduction to CO that
can be rationally designed to deliver high catalytic performance.
One common mechanistic feature of these electrocatalysts developed
thus far is an electrogenerated reduced metal center associated with
catalytic CO2 reduction. Here we report a heterogenized
zinc–porphyrin complex (zinc(II) 5,10,15,20-tetramesitylporphyrin)
as an electrocatalyst that delivers a turnover frequency as high as
14.4 site–1 s–1 and a Faradaic
efficiency as high as 95% for CO2 electroreduction to CO
at −1.7 V vs the standard hydrogen electrode in an organic/water
mixed electrolyte. While the Zn center is critical to the observed
catalysis, in situ and operando X-ray absorption spectroscopic studies
reveal that it is redox-innocent throughout the potential range. Cyclic
voltammetry indicates that the porphyrin ligand may act as a redox
mediator. Chemical reduction of the zinc–porphyrin complex
further confirms that the reduction is ligand-based and the reduced
species can react with CO2. This represents the first example
of a transition-metal complex for CO2 electroreduction
catalysis with its metal center being redox-innocent under working
conditions.
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Wu, Yueshen; Jiang, Jianbing; Weng, Zhe; Wang, Maoyu; Broere, Daniël L.
J.; Zhong, Yiren; et al. (2017). Electroreduction of CO2 Catalyzed by a
Heterogenized Zn–Porphyrin Complex with a Redox-Innocent Metal
Center. ACS Publications. Collection. https://doi.org/10.1021/acscentsci.7b00160
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AUTHORS (9)
YW
Yueshen Wu
JJ
Jianbing Jiang
ZW
Zhe Weng
MW
Maoyu Wang
DB
Daniël L.
J. Broere
YZ
Yiren Zhong
GB
Gary W. Brudvig
ZF
Zhenxing Feng
HW
Hailiang Wang