Achieving Efficient CO<sub>2</sub> Electrolysis to CO by Local Coordination Manipulation of Nickel Single-Atom Catalysts.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 37470490.
- Also identified by DOI 10.1021/acs.nanolett.3c01808.
- No licence information is recorded for this record.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
Selective electroreduction of CO<sub>2</sub> to C<sub>1</sub> feed gas provides an attractive avenue to store intermittent renewable energy. However, most of the CO<sub>2</sub>-to-CO catalysts are designed from the perspective of structural reconstruction, and it is challenging to precisely design a meaningful confining microenvironment for active sites on the support. Herein, we report a local sulfur doping method to precisely tune the electronic structure of an isolated asymmetric nickel-nitrogen-sulfur motif (Ni<sub>1</sub>-NSC). Our Ni<sub>1</sub>-NSC catalyst presents >99% faradaic efficiency for CO<sub>2</sub>-to-CO under a high current density of -320 mA cm<sup>-2</sup>. <i>In situ</i> attenuated total reflection surface-enhanced infrared absorption spectroscopy and differential electrochemical mass spectrometry indicated that the asymmetric sites show a significantly weaker binding strength of *CO and a lower kinetic overpotential for CO<sub>2</sub>-to-CO. Further theoretical analysis revealed that the enhanced CO<sub>2</sub> reduction reaction performance of Ni<sub>1</sub>-NSC was mainly due to the effectively decreased intermediate activation energy.