Low-valence Znδ+ (0<2) single-atom material as highly efficient electrocatalyst for CO2 reduction

Li, Simin, Zhao, Siqi, Lu, Xiuyuan, Ceccato, Marcel, Hu, Xin-Ming, Roldan, Alberto ORCID: https://orcid.org/0000-0003-0353-9004, Catalano, Jacopo, Catalano, Jacopo, Liu, Min, Skrydstrup, Troels and Daasbjerg, Kim 2021. Low-valence Znδ+ (0<2) single-atom material as highly efficient electrocatalyst for CO2 reduction. Angewandte Chemie International Edition 60 , 22826–22832. 10.1002/anie.202107550

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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.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Wiley
ISSN:	1521-3773
Date of First Compliant Deposit:	28 October 2021
Date of Acceptance:	15 August 2021
Last Modified:	25 Nov 2024 19:00
URI:	https://orca.cardiff.ac.uk/id/eprint/145102

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