Theoretical Studies on the Synergetic Effects of Au-Pd Bimetallic Catalysts in the Selective Oxidation of Methanol

	Theoretical Studies on the Synergetic Effects of Au-Pd Bimetallic Catalysts in the Selective Oxidation of Methanol
	Chang, Chun-Ran 1,2,3; Long, Bo 2,3,5; Yang, Xiao-Feng 2,3,4; Li, Jun 2,3
刊名	journal of physical chemistry c
	2015-07-16
卷号	119 期号:28 页码:16072-16081
英文摘要	the selective oxidation of methanol to formaldehyde with molecular o-2 on au-pd alloy surfaces has been studied by using density functional theory (dft). we show that the existence of pd remarkably improves the adsorption and activation of o-2 on au-pd surfaces. in particular, the second-neighbor pd monomer pair (pd-snmp) surrounded by gold atoms can provide unique active sites for the coadsorption of o-2 center dot center dot center dot ch3oh, thus facilitating the activation of o2 via a hydroperoxyl radical (ooh). with the involvement of ooh and its decomposed fragments (o and oh), the oxidative dehydrogenation of methanol to formaldehyde is facilely achieved on bimetallic au-pd surfaces, the barriers of which are calculated to be 0.02-0.45 ev on au2pd/(111) and aupd/(100) surfaces. importantly, we find that the unusual activation of o-2 via an ooh pathway instead of direct dissociation on au-pd catalysts is mainly responsible for the enhanced activity and selectivity in the selective oxidation of alcohols. this hydroperoxyl-based mechanism reveals the intrinsic synergy of au-pd bimetallic catalysts in the selective oxidation of alcohols and may provide insights for designing better bimetallic catalysts
WOS标题词	science & technology ; physical sciences ; technology
类目[WOS]	chemistry, physical ; nanoscience & nanotechnology ; materials science, multidisciplinary
研究领域[WOS]	chemistry ; science & technology - other topics ; materials science
关键词[WOS]	active heterogeneous catalyst ; transition-metal surfaces ; density-functional theory ; liquid-phase oxidation ; solvent-free oxidation ; free aerobic oxidation ; anionic gold clusters ; supported gold ; co oxidation ; alcohol oxidation
收录类别	SCI
语种	英语
WOS记录号	WOS:000358337700033
公开日期	2016-05-09
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/146601]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
作者单位	1.Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Xian 710049, Peoples R China 2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China 3.Tsinghua Univ, Key Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing 100084, Peoples R China 4.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 5.Guizhou Minzu Univ, Coll Informat Engn, Guiyang 550025, Peoples R China
推荐引用方式 GB/T 7714	Chang, Chun-Ran,Long, Bo,Yang, Xiao-Feng,et al. Theoretical Studies on the Synergetic Effects of Au-Pd Bimetallic Catalysts in the Selective Oxidation of Methanol[J]. journal of physical chemistry c,2015,119(28):16072-16081.
APA	Chang, Chun-Ran,Long, Bo,Yang, Xiao-Feng,&Li, Jun.(2015).Theoretical Studies on the Synergetic Effects of Au-Pd Bimetallic Catalysts in the Selective Oxidation of Methanol.journal of physical chemistry c,119(28),16072-16081.
MLA	Chang, Chun-Ran,et al."Theoretical Studies on the Synergetic Effects of Au-Pd Bimetallic Catalysts in the Selective Oxidation of Methanol".journal of physical chemistry c 119.28(2015):16072-16081.