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

doi:10.1021/jacs.8b07627

IMR OpenIR

	Electrocatalytic Water Oxidation at Quinone-on-Carbon: A Model System Study
	Lin, Yangming 1; Wu, Kuang-Hsu 2; Lu, Qing 1; Gu, Qingqing 1,3; Zhang, Liyun 3; Zhang, Bingsen 3; Su, Dangsheng 3; Plodinec, Milivoj 4; Schloegl, Robert 1,4; Heumann, Saskia 1
通讯作者	Heumann, Saskia(saskia.heumann@cec.mpg.de)
	2018-11-07
发表期刊	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN	0002-7863
卷号	140 期号:44 页码:14717-14724
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.
资助者	Max Planck society
DOI	10.1021/jacs.8b07627
收录类别	SCI
语种	英语
资助项目	Max Planck society
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:000449887800030
出版者	AMER CHEMICAL SOC
引用统计	被引频次：57[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/130565
专题	中国科学院金属研究所
通讯作者	Heumann, Saskia
作者单位	1.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
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.