Regenerative Electrocatalytic Redox Cycle of Copper Sulfide for Sustainable NH3Production under Ambient Conditions

Hee Soo Kim, Jihyun Choi, Jimin Kong, Hansung Kim, Sung Jong Yoo, Hyun S. Park

Research output: Contribution to journalArticlepeer-review

37 Citations (Scopus)

Abstract

Electrochemical nitrogen reduction reaction (NRR) is a promising method for energy-efficient and low-emission NH3 production. Herein, we report electrochemical NH3 production using a copper sulfide-based electrocatalyst. A solid-state synthesis is employed to prepare the Cu9S5 catalyst for artificial N2 fixation in a neutral aqueous electrolyte. Despite an excellent NRR activity of 10.8 ± 0.4 μg/hcm2 at -0.5 VRHE, however, the catalyst itself is reductively degraded during the NRR. To achieve continuous electrochemical NH3 production, a regenerative electrochemical sulfur cycle is introduced that revives the Cu9S5 crystal structure and NRR activities. The electrochemical regeneration process reconstructing the metal-sulfur bond in between sequential NH3 production processes restores the NRR activity. Importantly, catalytic surfaces providing a labile sulfhydryl functional group attached to the N2-adsorption metal center are required to achieve efficient NRR activity under ambient conditions.

Original languageEnglish
Pages (from-to)435-445
Number of pages11
JournalACS Catalysis
Volume11
Issue number1
DOIs
Publication statusPublished - 2021 Jan 1

Bibliographical note

Publisher Copyright:
© 2020 American Chemical Society.

All Science Journal Classification (ASJC) codes

  • Catalysis
  • General Chemistry

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