气候变化领域集成服务门户(CCPortal): Constructing canopy-shaped molecular architectures to create local Pt surface sites with high tolerance to H2S and CO for hydrogen electrooxidation

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DOI	10.1039/c7ee02641b
	Constructing canopy-shaped molecular architectures to create local Pt surface sites with high tolerance to H2S and CO for hydrogen electrooxidation
	Wang T.; Chen Z.-X.; Yu S.; Sheng T.; Ma H.-B.; Chen L.-N.; Rauf M.; Xia H.-P.; Zhou Z.-Y.; Sun S.-G.
发表日期	2018
ISSN	17545692
起始页码	166
结束页码	171
卷号	11 期号:1
英文摘要	Rational design and construction of the local environment of active sites on noble metal surfaces is a promising, but challenging, approach for developing high-selectivity catalysts. This study presents an effective approach, via engineering local active sites, aiming to solve the critical problem of H2S and CO poisoning of Pt catalysts for H2 electrooxidation, the anode reaction of polymer electrolyte membrane fuel cells. A canopy-shaped molecular architecture was constructed by immobilizing an organic molecule, 2,6-diacetylpyridine (DAcPy), on Pt surface, which exhibits high H2S (1 ppm) and CO (100 ppm) tolerance. Through electrochemical, spectroscopic, and DFT studies, as well as comparative investigation of analogous structure molecules, it was revealed that DAcPy can be strongly adsorbed on Pt surface through tridentate coordination (two Pt-C and one Pt-N bonds), allowing it to compete with CO and H2S adsorption. The pyridine ring of DAcPy is in a tilted orientation, providing some protection underneath the ring for Pt atoms. Such a height-limited space is just accessible for small-sized H2, but not for relatively large H2S and CO. This study demonstrates that regulating steric hindrance to protect active sites is a promising approach for designing highly selective electrocatalysts. © The Royal Society of Chemistry.
英文关键词	Catalyst activity; Catalyst poisoning; Catalyst selectivity; Catalysts; Cell engineering; Design for testability; Electrocatalysts; Electrolytes; Electrooxidation; Fuel cells; Molecules; Polyelectrolytes; Precious metals; Proton exchange membrane fuel cells (PEMFC); Analogous structures; Critical problems; Effective approaches; Hydrogen electrooxidation; Local environments; Molecular architecture; Organic molecules; Steric hindrances; Platinum; catalyst; design; electrochemical method; electrolyte; fuel cell; hydrogen; membrane; polymer; reaction kinetics
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190347
作者单位	Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China; College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241000, China
推荐引用方式 GB/T 7714	Wang T.,Chen Z.-X.,Yu S.,et al. Constructing canopy-shaped molecular architectures to create local Pt surface sites with high tolerance to H2S and CO for hydrogen electrooxidation[J],2018,11(1).
APA	Wang T..,Chen Z.-X..,Yu S..,Sheng T..,Ma H.-B..,...&Sun S.-G..(2018).Constructing canopy-shaped molecular architectures to create local Pt surface sites with high tolerance to H2S and CO for hydrogen electrooxidation.Energy & Environmental Science,11(1).
MLA	Wang T.,et al."Constructing canopy-shaped molecular architectures to create local Pt surface sites with high tolerance to H2S and CO for hydrogen electrooxidation".Energy & Environmental Science 11.1(2018).