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

doi:10.1021/jacs.8b07627

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	Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study
	Lin, Yangming 3; Wu, Kuang-Hsu 1; Lu, Qing 3; Gu, Qingqing 3,4; Zhang, Liyun 4; Zhang, Bingsen 4; Su, Dangsheng 4; Plodinec, Milivoj 2; Schloegl, Robert 2,3; Heumann, Saskia 3
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2018-11-07
卷号	140 期号:44 页码:14717-14724
ISSN号	0002-7863
DOI	10.1021/jacs.8b07627
通讯作者	Heumann, Saskia(saskia.heumann@cec.mpg.de)
英文摘要	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 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.
资助项目	Max Planck society
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000449887800030
资助机构	Max Planck society
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/130559]
专题	金属研究所_中国科学院金属研究所
通讯作者	Heumann, Saskia
作者单位	1.Univ New South Wales, Sch Chem Engn, Kensington, NSW 2052, Australia 2.Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, Faradayweg 4-6, D-14195 Berlin, Germany 3.Max Planck Inst Chem Energy Convers, Stiftstr 34-36, D-45470 Mulheim, Germany 4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	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.