Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study
Lin, Yangming1; Wu, Kuang-Hsu2; Lu, Qing1; Gu, Qingqing1,3; Zhang, Liyun3; Zhang, Bingsen3; Su, Dangsheng3; Plodinec, Milivoj4; Schloegl, Robert1,4; Heumann, Saskia1
Corresponding AuthorHeumann, Saskia(
AbstractNanocarbon 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 species were used as model structures to investigate the explicit roles which eight kinds of aromatic molecules with designated single oxygen 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 pi 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=0 (similar to 0.323 s(-1) at eta = 340 mV) in 0.1 M KOH and the optimized current density (10 mA/cm(2) at 1.58 V vs RHE) of quinone-modified carbon systems are comparable to those of promising metal-based catalysts.
Funding OrganizationMax Planck society
Indexed BySCI
Funding ProjectMax Planck society
WOS Research AreaChemistry
WOS SubjectChemistry, Multidisciplinary
WOS IDWOS:000449887800030
Citation statistics
Cited Times:42[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Corresponding AuthorHeumann, Saskia
Affiliation1.Max Planck Inst Chem Energy Convers, Stiftstr 34-36, D-45470 Mulheim, Germany
2.Univ New South Wales, Sch Chem Engn, Kensington, NSW 2052, Australia
3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
4.Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, Faradayweg 4-6, D-14195 Berlin, Germany
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Lin, Yangming,Wu, Kuang-Hsu,Lu, Qing,et al. Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2018,140(44):14717-14724.
APA Lin, Yangming.,Wu, Kuang-Hsu.,Lu, Qing.,Gu, Qingqing.,Zhang, Liyun.,...&Heumann, Saskia.(2018).Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,140(44),14717-14724.
MLA Lin, Yangming,et al."Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 140.44(2018):14717-14724.
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