Tuning Carbon Dioxide Reduction Reaction Selectivity of Bi Single-Atom Electrocatalysts with Controlled Coordination Environments

Saswati Santra, Verena Streibel, Laura I. Wagner, Ningyan Cheng, Pan Ding, Guanda Zhou, Elise Sirotti, Ryan Kisslinger, Tim Rieth, Siyuan Zhang, Ian D. Sharp

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Control over product selectivity of the electrocatalytic CO2 reduction reaction (CO2RR) is a crucial challenge for the sustainable production of carbon-based chemical feedstocks. In this regard, single-atom catalysts (SACs) are promising materials due to their tunable coordination environments, which could enable tailored catalytic activities and selectivities, as well as new insights into structure-activity relationships. However, direct evidence for selectivity control via systematic tuning of the SAC coordination environment is scarce. In this work, we have synthesized two differently coordinated Bi SACs anchored to the same host material (carbon black) and characterized their CO2RR activities and selectivities. We find that oxophilic, oxygen-coordinated Bi atoms produce HCOOH, while nitrogen-coordinated Bi atoms generate CO. Importantly, use of the same support material assured that alternation of the coordination environment is the dominant factor for controlling the CO2RR product selectivity. Overall, this work demonstrates the structure-activity relationship of Bi SACs, which can be utilized to establish control over CO2RR product distributions, and highlights the promise for engineering atomic coordination environments of SACs to tune reaction pathways.

Original languageEnglish
Article numbere202301452
JournalChemSusChem
Volume17
Issue number10
DOIs
StatePublished - 21 May 2024

Keywords

  • CO2 reduction
  • Electrochemistry
  • Energy conversion
  • Selectivity
  • Single-atom catalysis

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