Oxygen-Bridged Indium-Nickel Atomic Pair as Dual-Metal Active Sites Enabling Synergistic Electrocatalytic CO2 Reduction

Zhaozhong Fan; Ruichun Luo; Yanxue Zhang; Bo Zhang; Panlong Zhai; Yanting Zhang; Chen Wang; Junfeng Gao; Wu Zhou; Licheng Sun; Jungang Hou

doi:10.1002/anie.202216326

Oxygen-Bridged Indium-Nickel Atomic Pair as Dual-Metal Active Sites Enabling Synergistic Electrocatalytic CO₂ Reduction

Angew Chem Int Ed Engl. 2023 Feb 6;62(7):e202216326. doi: 10.1002/anie.202216326. Epub 2023 Jan 11.

Authors

Zhaozhong Fan¹, Ruichun Luo^{2

3}, Yanxue Zhang⁴, Bo Zhang¹, Panlong Zhai¹, Yanting Zhang¹, Chen Wang¹, Junfeng Gao⁴, Wu Zhou^{2

3}, Licheng Sun^{5

6}, Jungang Hou¹

Affiliations

¹ State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
² School of Physical Sciences and CAS Key Laboratory of Vacuum Physics, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
³ CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
⁴ Laboratory of Materials Modification by Laser, Ion and Electron Beams, Ministry of Education, Dalian University of Technology, Dalian, 116024, P. R. China.
⁵ Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, 310024, P. R. China.
⁶ Department of Chemistry, KTH Royal Institute of Technology, 10044, Stockholm, Sweden.

PMID: 36519523
DOI: 10.1002/anie.202216326

Abstract

Single-atom catalysts offer a promising pathway for electrochemical CO₂ conversion. However, it is still a challenge to optimize the electrochemical performance of dual-atom catalysts. Here, an atomic indium-nickel dual-sites catalyst bridged by an axial oxygen atom (O-In-N₆ -Ni moiety) was anchored on nitrogenated carbon (InNi DS/NC). InNi DS/NC exhibits superior CO selectivity with Faradaic efficiency higher than 90 % over a wide potential range from -0.5 to -0.8 V versus reversible hydrogen electrode (vs. RHE). Moreover, an industrial CO partial current density up to 317.2 mA cm^-2 is achieved at -1.0 V vs. RHE in a flow cell. In situ ATR-SEIRAS combined with theory calculations reveal that the synergistic effect of In-Ni dual-sites and O atom bridge not only reduces the reaction barrier for the formation of *COOH, but also retards the undesired hydrogen evolution reaction. This work provides a feasible strategy to construct dual-site catalysts towards energy conversion.

Keywords: Atomically Dispersed Pair; CO2 Electroreduction; Dual-Metal Active Sites; Dual-Site Catalysts; Synergistic Effect.