Activating Bi p-orbitals in Dispersed Clusters of Amorphous BiOx for Electrocatalytic Nitrogen Reduction

Jianxin Kang, Xiangyu Chen, Rutong Si, Xiang Gao, Shuo Zhang, Gilberto Teobaldi, Annabella Selloni, Li Min Liu, Lin Guo

Research output: Contribution to journalArticlepeer-review

10 Scopus citations

Abstract

Catalytic strategies based on main group metals are significantly less advanced than those of transition metal catalysis, leaving untapped areas of potentially fruitful research. We here demonstrate an effective approach for the modulation of Bi 6p energy levels during the construction of atomically dispersed clusters of amorphous BiOx. Bi oxidation state is proposed to strongly affects the nitrogen fixation activity, with the half-occupied pz orbitals of the Bi2+ ions being highly efficient toward electron injection into the inert N2 molecule. With sufficient catalytic sites to adsorb and activate N2, the bonding between N2 and catalyst is able to be in situ identified. The catalyst shows an outstanding Faraday efficiency (≈30 %) and high yield (≈113 μg h−1 mg−1cat) in NH3 production, outperforming most of the existing catalysts in aqueous solution. These results lay the basis for developing the potential of p-block elements for catalysis of multi-electron reactions.

Original languageEnglish (US)
Article numbere202217428
JournalAngewandte Chemie - International Edition
Volume62
Issue number15
DOIs
StatePublished - Apr 3 2023

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • Catalysis

Keywords

  • Amorphous Nanomaterial
  • Electrocatalysis
  • In Situ Identification
  • Nitrogen Fixation
  • p-Orbitals

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