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

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
JournalJournal of Materials Chemistry A
DOIs
Publication statusAccepted/In press - 2022

Bibliographical note

Funding Information:
This work was supported by NSFC (51802157 and 61725402), and the International Cooperation Program (BZ2020063) of Jiangsu Province, the Fundamental Research Funds for the Central Universities (30919012107, 30918012202). Beijing National Laboratory for Molecular Sciences (BNLMS201911) and the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning (NRF-2019R1A2C3010479), the Korea government (MSIP) (NRF-2019M3D1A1079309). J. H. Park acknowledges the support from International Energy Joint R&D Program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP), granted financial resource from the Ministry of Trade, Industry & Energy, Republic of Korea. (20208510010310).

Publisher Copyright:
© 2022 The Royal Society of Chemistry.

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

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