气候变化领域集成服务门户(CCPortal): Towards an atomistic understanding of electrocatalytic partial hydrocarbon oxidation: Propene on palladium

CCPortal

DOI	10.1039/c8ee03426e
	Towards an atomistic understanding of electrocatalytic partial hydrocarbon oxidation: Propene on palladium
	Winiwarter A.; Silvioli L.; Scott S.B.; Enemark-Rasmussen K.; Sariç M.; Trimarco D.B.; Vesborg P.C.K.; Moses P.G.; Stephens I.E.L.; Seger B.; Rossmeisl J.; Chorkendorff I.
发表日期	2019
ISSN	17545692
起始页码	1055
结束页码	1067
卷号	12 期号:3
英文摘要	The efficient partial oxidation of hydrocarbons to valuable chemicals without formation of CO2 is one of the great challenges in heterogeneous catalysis. The ever-decreasing cost of renewable electricity and the superior control over reactivity qualify electrochemistry as a particularly attractive means of addressing this challenge. Yet, to date, little is known about the factors regulating hydrocarbon oxidation at the atomic level. A relevant showcase reaction is propene electro-oxidation to key industrial commodity chemicals, such as acrolein, acrylic acid and propylene oxide. In this study, we investigate the partial electrochemical oxidation of propene on high-surface area Pd electrodes using a combination of electrochemical measurements, advanced product characterization and theoretical modeling. We report a new reaction product, propylene glycol, and high selectivity towards acrolein. We further identify key reaction intermediates and propose a mechanism dictated by the surface coverage of organic species formed in situ, where stable reactant adsorption at low coverage determines the selectivity towards allylic oxidation at high coverage. Our fundamental findings enable advances in partial hydrocarbon oxidation reactions by highlighting atomic surface structuring as the key to selective and versatile electrochemical catalyst design. © 2019 The Royal Society of Chemistry.
英文关键词	Aldehydes; Catalysis; Electrochemical oxidation; Electrochemistry; Electrooxidation; Herbicides; Industrial chemicals; Palladium; Propylene; Surface reactions; Commodity chemicals; Electrochemical catalyst; Electrochemical measurements; Hydrocarbon oxidation; Product characterizations; Reactant adsorption; Renewable electricity; Theoretical modeling; Reaction intermediates; adsorption; catalysis; catalyst; chemical reaction; electricity; electrochemical method; electrochemistry; electrode; hydrocarbon; oxidation; palladium
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/189954
作者单位	SurfCat, Department of Physics, Technical University of Denmark, Fysikvej Byg. 311, Kgs. Lyngby, 2800, Denmark; Nano-Science Center, Department of Chemistry, University of Copenhagen, Universitetsparken 5, Copenhagen, 2100, Denmark; Department of Chemistry, Technical University of Denmark, Kemitorvet, Byg. 207, Kgs. Lyngby, 2800, Denmark; Spectro Inlets, COBIS, Ole Maaløes Vej 3, Copenhagen, 2200, Denmark; Haldor Topsoe A/S, Haldor Topsøes Allé 1, Kgs. Lyngby, 2800, Denmark; Department of Materials, Imperial College London, Royal School of Mines, London, SW7 2AZ, United Kingdom
推荐引用方式 GB/T 7714	Winiwarter A.,Silvioli L.,Scott S.B.,et al. Towards an atomistic understanding of electrocatalytic partial hydrocarbon oxidation: Propene on palladium[J],2019,12(3).
APA	Winiwarter A..,Silvioli L..,Scott S.B..,Enemark-Rasmussen K..,Sariç M..,...&Chorkendorff I..(2019).Towards an atomistic understanding of electrocatalytic partial hydrocarbon oxidation: Propene on palladium.Energy & Environmental Science,12(3).
MLA	Winiwarter A.,et al."Towards an atomistic understanding of electrocatalytic partial hydrocarbon oxidation: Propene on palladium".Energy & Environmental Science 12.3(2019).