Hierarchical Dual Single-Atom Catalysts with Coupled CoN<sub>4</sub> and NiN<sub>4</sub> Moieties for Industrial-Level CO<sub>2</sub> Electroreduction to Syngas.
basic_science · Level V
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- Record sourced from PubMed, PMID 37916602.
- Also identified by DOI 10.1021/acsnano.3c09102.
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Abstract
Renewable-driven electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to syngas is an encouraging alternative strategy to traditional fossil fuel-based syngas production, and the development of industrial-level electrocatalysts is vital. Herein, based on theoretical optimization of metal species, hierarchical Co<sub><i>x</i></sub>Ni<sub>1-<i>x</i></sub>-N-C dual single-atom catalyst (DSAC) with individual NiN<sub>4</sub> (CO preferential) and CoN<sub>4</sub> (H<sub>2</sub> preferential) moieties was constructed by a two-step pyrolysis route. The Co<sub>0.5</sub>Ni<sub>0.5</sub>-N-C exhibits a stable CO Faradaic efficiency of 50 ± 5% and an industrial-level current density of 101-365 mA cm<sup>-2</sup> in an ultrawide potential window of -0.5 to -1.1 V. The CO/H<sub>2</sub> ratio of syngas can be conveniently tuned by regulating the Co/Ni ratio. The coupled effect of NiN<sub>4</sub> and CoN<sub>4</sub> moieties under a local high-pH microenvironment is responsible for the regulation of the CO/H<sub>2</sub> selectivity and yield for the Co<sub><i>x</i></sub>Ni<sub>1-<i>x</i></sub>-N-C catalyst, which is not present in the mixed Co-N-C and Ni-N-C catalyst. This study provides a promising DSAC strategy for achieving industrial-level syngas production via CO<sub>2</sub>RR.