A Tandem Strategy for Enhancing Electrochemical CO Reduction Activity of Single-Atom Cu-S N Catalysts via Integration with Cu Nanoclusters.

Angew Chem Int Ed Engl

National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin, 300130, P. R. China.

Published: November 2021

AI Article Synopsis

  • A new tandem electrocatalyst, Cu-S N /Cu, combines a single copper site coordinated with nitrogen and sulfur in a carbon matrix with atomically dispersed copper clusters.
  • This catalyst achieves a 100% Faradaic efficiency for CO generation at -0.65 V and maintains over 90% efficiency between -0.55 to -0.75 V, outperforming similar catalysts like Cu-N and Cu-S N.
  • The structure allows for an optimized reaction pathway, enhancing the conversion of CO to CO by efficiently facilitating proton-coupled electron transfer through the interaction between the copper sites.

Article Abstract

We developed a tandem electrocatalyst for CO -to-CO conversion comprising the single Cu site co-coordinated with N and S anchored carbon matrix (Cu-S N ) and atomically dispersed Cu clusters (Cu ), denoted as Cu-S N /Cu . The as-prepared Cu-S N /Cu composite presents a 100 % Faradaic efficiency towards CO generation (FE ) at -0.65 V vs. RHE and high FE over 90 % from -0.55 to -0.75 V, outperforming the analogues with Cu-N (FE only 54 % at -0.7 V) and Cu-S N (FE 70 % at -0.7 V) configurations. The unsymmetrical Cu-S N atomic interface in the carbon basal plane possesses an optimized binding energy for the key intermediate *COOH compared with Cu-N site. At the same time, the adjacent Cu effectively promotes the protonation of *CO by accelerating water dissociation and offering *H to the Cu-S N active sites. This work provides a tandem strategy for facilitating proton-coupled electron transfer over the atomic-level catalytic sites.

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http://dx.doi.org/10.1002/anie.202109579DOI Listing

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