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  Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study

Lin, Y., Wu, K.-H., Lu, Q., Gu, Q., Zhang, L., Zhang, B., et al. (2018). Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study. Journal of the American Chemical Society, 140(44), 14717-14724. doi:10.1021/jacs.8b07627.

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 Creators:
Lin, Yangming1, Author
Wu, Kuang-Hsu2, Author
Lu, Qing1, Author
Gu, Qingqing1, 3, Author
Zhang, Liyun3, Author
Zhang, Bingsen3, Author
Su, Dangsheng3, Author
Plodinec, Milivoj4, Author           
Schlögl, Robert1, 4, Author           
Heumann, Saskia1, Author
Affiliations:
1Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion , Stiftstr. 34 - 36 45470 Mülheim an der Ruhr, Germany, ou_persistent13              
2School of Chemical Engineering, The University of New South Wales, Sydney, Kensington, New South Wales 2052, Australia, ou_persistent22              
3Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, People’s Republic of China, ou_persistent22              
4Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              

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 Abstract: Nanocarbon can promote robust and efficient electrocatalytic water oxidation through active surface oxygen moieties. The recent mechanistic understandings (e.g., active sites) of metal-free carbon catalysts in oxygen evolution reaction (OER), however, are still rife with controversies. In this work, we describe a facile protocol in which eight kinds of aromatic molecules with designated single oxygen species were used as model structures to investigate the explicit roles of each common oxygen group in OER at a molecular level. These model structures were decorated onto typical nanocarbon surfaces like onion-like carbons (OLC) or multiwalled carbon nanotubes (MWCNT) to build aromatic molecule-modified carbon systems. We show that edge (including zigzag and armchair) quinones in a conjugated π network are the true active centers, and the roles of ether and carboxyl groups are excluded in the OER process. The plausible rate-determining step could be singled out by H/D kinetic isotope effects. The turnover frequency per C═O (∼0.323 s–1 at η = 340 mV) in 0.1 M KOH and the optimized current density (10 mA/cm2 at 1.58 V vs RHE) of quinone-modified carbon systems are comparable to those of promising metal-based catalysts.

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Language(s): eng - English
 Dates: 2018-07-192018-10-162018-11-07
 Publication Status: Issued
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.8b07627
 Degree: -

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Title: Journal of the American Chemical Society
  Other : J. Am. Chem. Soc.
  Abbreviation : JACS
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 8 Volume / Issue: 140 (44) Sequence Number: - Start / End Page: 14717 - 14724 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870