p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction

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

*Corresponding author for this work

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


Electrochemical CO2 reduction represents a promising path toward the production of value-added chemicals. Atomically dispersed metal sites on nitrogen-doped carbon have demonstrated outstanding catalytic performance in this reaction. However, challenges remain in developing such catalysts beyond transition metals. Herein, we present two types of p-block indium single-atom catalysts: one with four nitrogen coordinated (In-N4) and another with three nitrogen coordinated with one vacancy nearby (In-N3-V). In electrochemical CO2 reduction, the In-N3-V site can achieve maximum CO Faradic efficiency (FECO) of 95% at -0.57 V vs reversible hydrogen electrode (RHE) in an aqueous medium. This outperforms the intact In-N4 catalyst with the maximum FECO of 80% at -0.47 V vs RHE. Density functional theory calculations on the mechanism suggest that structural change from In-N4 to In-N3-V brings the In orbital (s and pz) energies closer to the Fermi energy. These hybridized orbitals are responsible for lowering the energy barrier for COOH∗ intermediate formation, thus enhancing the catalytic performance. This work sheds light on the relationship between catalytic performance and structure of In single-atom sites, highlighting the importance of tailoring the electron state of s and pz orbitals in developing efficient p-block single-atom catalysts for electrochemical CO2 reduction.

Original languageEnglish
JournalACS Catalysis
Pages (from-to)7386-7395
Number of pages10
Publication statusPublished - Jun 2022


  • CO2 reduction
  • coordination environment
  • electrocatalysis
  • indium single atoms
  • metal-organic frameworks


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