Boosting Electrochemical Carbon Dioxide Reduction on Atomically Dispersed Nickel Catalyst

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Qi Hao - , Jilin University, CAS - Changchun Institute of Applied Chemistry (Author)
  • Dong Xue Liu - , Jilin University (Author)
  • Ruiping Deng - , CAS - Changchun Institute of Applied Chemistry (Author)
  • Hai Xia Zhong - , Chair of Molecular Functional Materials (cfaed), CAS - Changchun Institute of Applied Chemistry (Author)

Abstract

Single-atom catalysts (SACs) with metal–nitrogen (M–N) sites are one of the most promising electrocatalysts for electrochemical carbon dioxide reduction (ECO2R). However, challenges in simultaneously enhancing the activity and selectivity greatly limit the efficiency of ECO2R due to the improper interaction of reactants/intermediates on these catalytic sites. Herein, we report a carbon-based nickel (Ni) cluster catalyst containing both single-atom and cluster sites (NiNx-T, T = 500–800) through a ligand-mediated method and realize a highly active and selective electrocatalytic CO2R process. The catalytic performance can be regulated by the dispersion of Ni–N species via controlling the pyrolysis condition. Benefitting from the synergistic effect of pyrrolic-nitrogen coordinated Ni single-atom and cluster sites, NiNx-600 exhibits a satisfying catalytic performance, including a high partial current density of 61.85 mA cm−2 and a high turnover frequency (TOF) of 7,291 h−1 at −1.2 V vs. RHE, and almost 100% selectivity toward carbon monoxide (CO) production, as well as good stability under 10 h of continuous electrolysis. This work discloses the significant role of regulating the coordination environment of the transition metal sites and the synergistic effect between the isolated single-site and cluster site in enhancing the ECO2R performance.

Details

Original languageEnglish
Article number837580
JournalFrontiers in chemistry
Volume9
Publication statusPublished - 20 Jan 2022
Peer-reviewedYes

Keywords

Research priority areas of TU Dresden

ASJC Scopus subject areas

Keywords

  • atomic dispersion, carbon dioxide reduction, ligand-mediated, nickel clusters and single atoms, nickel-nitrogen catalytic sites