Low-Valence Znδ+ (0<δ<2) Single-Atom Material as Highly Efficient Electrocatalyst for CO2 Reduction

Simin Li, Siqi Zhao, Xiuyuan Lu, Marcel Ceccato, Xin-Ming Hu*, Alberto Roldan, Jacopo Catalano, Min Liu*, Troels Skrydstrup, Kim Daasbjerg*

*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaperJournal articleResearchpeer-review

Abstract

A nitrogen-stabilized single-atom catalyst containing low-valence zinc atoms (Znδ+-NC) is reported. It contains saturated four-coordinate (Zn-N4) and unsaturated three-coordinate (Zn-N3) sites. The latter makes Zn a low-valence state, as deduced from X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, electron paramagnetic resonance, and density functional theory. Znδ+-NC catalyzes electrochemical reduction of CO2 to CO with near-unity selectivity in water at an overpotential as low as 310 mV. A current density up to 1 A cm−2 can be achieved together with high CO selectivity of >95 % using Znδ+-NC in a flow cell. Calculations suggest that the unsaturated Zn-N3 could dramatically reduce the energy barrier by stabilizing the COOH* intermediate owing to the electron-rich environment of Zn. This work sheds light on the relationship among coordination number, valence state, and catalytic performance and achieves high current densities relevant for industrial applications.
Original languageEnglish
JournalAngewandte Chemie International Edition
Volume60
Issue42
Pages (from-to)22826-22832
Number of pages7
ISSN1433-7851
DOIs
Publication statusPublished - Oct 2021

Keywords

  • CO2 reduction
  • ELECTROREDUCTION
  • METAL
  • SITES
  • coordination environment
  • electrocatalysis at scale
  • low valence
  • zinc single atoms

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