Show simple item record

dc.contributor.advisorFriend, Cynthia M.
dc.contributor.authorXu, Yunfei
dc.date.accessioned2019-05-17T14:17:40Z
dc.date.created2017-11
dc.date.issued2017-09-07
dc.date.submitted2017
dc.identifier.urihttp://nrs.harvard.edu/urn-3:HUL.InstRepos:39987993*
dc.description.abstractThe thesis has focused on revealing the mechanistic insights of the gaseous alcohol coupling/dehydrogenation/oxidation reactions for selectively making value-added products on the solid gold/copper single-crystal surfaces under ultrahigh vacuum (UHV) conditions. Those molecular-level insights about the selectivity, reactivity, and kinetics of metal-based heterogeneous catalysis, combined with density functional theory (DFT) calculations and ambient-pressure studies, provided guiding principles for the rational design of efficient real-life catalysts, which are crucial for a sustainable future. First, the background of gold/copper-based catalysis and the motivation of UHV model studies were discussed (Chapter 1). Relative binding strengths of intermediates on a catalyst surface govern the competition for the reactive sites and thus the overall reaction selectivity. The critical contribution of the noncovalent van der Waals (vdW) interactions to alkoxys’ overall binding strengths was revealed on both gold (Chapter 2) and copper (Chapter 5) combining experiment and theory. Similar results on two metals suggest the generality of such effect on metal-based catalysts. Then, kinetic parameters were measured for the gaseous alcohol reactions on Au(110) using temperature-programmed reaction/desorption (TPR/TPD) studies (Chapter 3). Next, the structure-dependent reactivity of methanol and ethanol with surface atomic oxygen as active sites on Au(110) was revealed combining TPR/TPD and scanning tunneling microscopy (STM) (Chapter 4). Furthermore, the critical role of defects as the active sites for the gaseous alcohol dehydrogenation reactions on Cu(111) and Cu(110) was studied using TPR/TPD and STM (Chapter 6). Detailed quantification of the defect active sites was discussed subsequently (Chapter 7). Finally, the methods used in this work were described (Chapter 8). Chapters 2-4 are about the research on gold and Chapters 5-7 are about the research on copper.
dc.description.sponsorshipChemistry and Chemical Biology
dc.format.mimetypeapplication/pdf
dc.language.isoen
dash.licenseLAA
dc.subjectChemistry, Physical
dc.subjectEnergy
dc.titleFundamental Studies of Alcohol Reactions on Gold and Copper
dc.typeThesis or Dissertation
dash.depositing.authorXu, Yunfei
dc.date.available2019-05-17T14:17:40Z
thesis.degree.date2017
thesis.degree.grantorGraduate School of Arts & Sciences
thesis.degree.levelDoctoral
thesis.degree.nameDoctor of Philosophy
dc.contributor.committeeMemberBetley, Theodore A.
dc.contributor.committeeMemberKaxiras, Efthimios
dc.type.materialtext
thesis.degree.departmentChemistry and Chemical Biology
dash.identifier.vireohttp://etds.lib.harvard.edu/gsas/admin/view/1868
dc.description.keywordsSurface Chemistry; Heterogeneous Catalysis
dc.identifier.orcid0000-0001-6394-2706
dash.author.emailxuyunfei69@gmail.com


Files in this item

Thumbnail

This item appears in the following Collection(s)

Show simple item record