Precise synthesis of single-atom Mo, W, Nb coordinated with oxygen functional groups of graphene oxide for stable and selective two-electron oxygen reduction in neutral media

Chaoran Dong, Kug Seung Lee, Yoonjun Cho, Shi Ping Wang, Xue Wen Fan, Fu Quan Bai, Jong Hyeok Park, Kan Zhang

Research output: Contribution to journalArticlepeer-review

11 Citations (Scopus)

Abstract

Herein, we propose a one-pot solvothermal method for a series of single-atom catalysts (SACs) anchored on mildly reduced graphene oxide (mrG) with active moieties of -CO3M, -CO2M and -COOM (M: Mo, W, Nb). The chemical inertness of polar aprotic dimethylsulfoxide (DMSO) enables a constant reaction environment where the MCl5 dimer can be dissociated to give monomeric pentahalides, leaving behind one unpaired electron on the metal center to coordinate with the OFGs. Theoretical studies revealed that all M-Ox-C moieties have an overwhelming preference to form H2O2 as a result of the downhill reaction. Among the materials prepared, Mo-SACs/mrG achieved the best selectivity (η ∼ 94.5%, Vonset = 0.65 V vs. RHE, Tafel slope of 53 mV dec−1) under neutral conditions. Furthermore, at the device level, the production rate of H2O2 is about 12.9 μmol min−1 with an average FE of over 80%, which is superior to other catalysts reported.

Original languageEnglish
Pages (from-to)9488-9496
Number of pages9
JournalJournal of Materials Chemistry A
Volume10
Issue number17
DOIs
Publication statusPublished - 2022 Mar 16

Bibliographical note

Publisher Copyright:
© 2022 The Royal Society of Chemistry

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • Renewable Energy, Sustainability and the Environment
  • General Materials Science

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