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Asymmetric Oxo-Bridged ZnPb Bimetallic Electrocatalysis Boosting CO2 -to-HCOOH Reduction.


ABSTRACT: Electrochemical CO2 reduction (ECR) is one of the promising CO2 recycling technologies sustaining the natural carbon cycle and offering more sustainable higher-energy chemicals. Zn- and Pb-based catalysts have improved formate selectivity, but they suffer from relatively low current activities considering the competitive CO selectivity on Zn. Here, lead-doped zinc (Zn(Pb)) electrocatalyst is optimized to efficiently reduce CO2 to formate, while CO evolution selectivity is largely controlled. Selective formate is detected with Faradaic efficiency (FEHCOOH ) of ≈95% at an outstanding partial current density of 47 mA cm-2 in a conventional H-Cell. Zn(Pb) is further investigated in an electrolyte-fed device achieving a superior conversion rate of ≈100 mA cm-2 representing a step closer to practical electrocatalysis. The in situ analysis demonstrates that the Pb incorporation plays a crucial role in CO suppression stem from the generation of the Pb-O-C-O-Zn structure rather than the CO-boosted Pb-O-C-Zn. Density functional theory (DFT) calculations reveal that the alloying effect tunes the adsorption energetics and consequently modifies the electronic structure of the system for an optimized asymmetric oxo-bridged intermediate. The alloying effect between Zn and Pb controls CO selectivity and achieves a superior activity for a selective CO2 -to-formate reduction.

SUBMITTER: Mohamed AGA 

PROVIDER: S-EPMC8811806 | biostudies-literature | 2022 Feb

REPOSITORIES: biostudies-literature

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Asymmetric Oxo-Bridged ZnPb Bimetallic Electrocatalysis Boosting CO<sub>2</sub> -to-HCOOH Reduction.

Mohamed Aya Gomaa Abdelkader AGA   Zhou Enbo E   Zeng Zipeng Z   Xie Jiafang J   Gao Dunfeng D   Wang Yaobing Y  

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20211110 4


Electrochemical CO<sub>2</sub> reduction (ECR) is one of the promising CO<sub>2</sub> recycling technologies sustaining the natural carbon cycle and offering more sustainable higher-energy chemicals. Zn- and Pb-based catalysts have improved formate selectivity, but they suffer from relatively low current activities considering the competitive CO selectivity on Zn. Here, lead-doped zinc (Zn(Pb)) electrocatalyst is optimized to efficiently reduce CO<sub>2</sub> to formate, while CO evolution selec  ...[more]

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