Catalysis with Supported Size-selected Pt Clusters: Fundamental UHV and Applied Ambient Experiments PDF
Preview Catalysis with Supported Size-selected Pt Clusters: Fundamental UHV and Applied Ambient Experiments
Springer Theses Recognizing Outstanding Ph.D. Research Florian Frank Schweinberger Catalysis with Supported Size- selected Pt Clusters Fundamental UHV and Applied Ambient Experiments Springer Theses Recognizing Outstanding Ph.D. Research For furthervolumes: http://www.springer.com/series/8790 Aims and Scope The series ‘‘Springer Theses’’ brings together a selection of the very best Ph.D. theses from around the world and across the physical sciences. Nominated and endorsed by two recognized specialists, each published volume has been selected for its scientific excellence and the high impact of its contents for the pertinent fieldofresearch.Forgreateraccessibilitytonon-specialists,thepublishedversions includeanextendedintroduction,aswellasaforewordbythestudent’ssupervisor explaining the special relevance of the work for the field. As a whole, the series will provide a valuable resource both for newcomers to the research fields described, and for other scientists seeking detailed background information on specialquestions.Finally,itprovidesanaccrediteddocumentationofthevaluable contributions made by today’s younger generation of scientists. Theses are accepted into the series by invited nomination only and must fulfill all of the following criteria • They must be written in good English. • ThetopicshouldfallwithintheconfinesofChemistry,Physics,EarthSciences, Engineering andrelatedinterdisciplinaryfieldssuchasMaterials, Nanoscience, Chemical Engineering, Complex Systems and Biophysics. • The work reported in the thesis must represent a significant scientific advance. • Ifthethesisincludespreviouslypublishedmaterial,permissiontoreproducethis must be gained from the respective copyright holder. • They must have been examined and passed during the 12 months prior to nomination. • Each thesis should include a foreword by the supervisor outlining the signifi- cance of its content. • The theses should have a clearly defined structure including an introduction accessible to scientists not expert in that particular field. Florian Frank Schweinberger Catalysis with Supported Size-selected Pt Clusters Fundamental UHV and Applied Ambient Experiments Doctoral Thesis accepted by the Technische Universität München, Germany 123 Author Supervisor Dr. FlorianFrank Schweinberger Prof.UeliHeiz Catalysis Research Center Department of Chemistry, Technische Universität München Catalysis Research Center Garching Technische Universität München Germany Garching Germany ISSN 2190-5053 ISSN 2190-5061 (electronic) ISBN 978-3-319-01498-2 ISBN 978-3-319-01499-9 (eBook) DOI 10.1007/978-3-319-01499-9 SpringerChamHeidelbergNewYorkDordrechtLondon LibraryofCongressControlNumber:2013945844 (cid:2)SpringerInternationalPublishingSwitzerland2014 Thisworkissubjecttocopyright.AllrightsarereservedbythePublisher,whetherthewholeorpartof the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation,broadcasting,reproductiononmicrofilmsorinanyotherphysicalway,andtransmissionor informationstorageandretrieval,electronicadaptation,computersoftware,orbysimilarordissimilar methodology now known or hereafter developed. Exempted from this legal reservation are brief excerpts in connection with reviews or scholarly analysis or material supplied specifically for the purposeofbeingenteredandexecutedonacomputersystem,forexclusiveusebythepurchaserofthe work. Duplication of this publication or parts thereof is permitted only under the provisions of theCopyright Law of the Publisher’s location, in its current version, and permission for use must always be obtained from Springer. Permissions for use may be obtained through RightsLink at the CopyrightClearanceCenter.ViolationsareliabletoprosecutionundertherespectiveCopyrightLaw. The use of general descriptive names, registered names, trademarks, service marks, etc. in this publicationdoesnotimply,evenintheabsenceofaspecificstatement,thatsuchnamesareexempt fromtherelevantprotectivelawsandregulationsandthereforefreeforgeneraluse. While the advice and information in this book are believed to be true and accurate at the date of publication,neithertheauthorsnortheeditorsnorthepublishercanacceptanylegalresponsibilityfor anyerrorsoromissionsthatmaybemade.Thepublishermakesnowarranty,expressorimplied,with respecttothematerialcontainedherein. Printedonacid-freepaper SpringerispartofSpringerScience+BusinessMedia(www.springer.com) Parts of this Thesis have been Published in the Following Journal Articles: Schweinberger, F.F.; Beer, M.J; Döblinger, M.; Ridge, C.J.; Crampton, A.S.; Wolff,C.;Jäckel,F.;Feldmann,J.;Tschurl,M.;Heiz,U.2013,J.Am.Chem.Soc. 135 (36): 13262. doi: 10.1021/ja406070q Beer, M.J.; Schweinberger, F.F.; Döblinger, M.; Sanwald, K.E.; Wolff, C.; Breimeier, J.; Crampton, A.S.; Ridge, C.J.; Tschurl, M.; Heiz, U.; Jäckel, F.; Feldmann, J. 2012, Nano. Lett. 12 (11): 5903. doi: 10.1021/nl3033069 Schweinberger, F.F.; Crampton, A.S.; Zimmermann, T.; Kwon, G.; Ridge, C.J.; Günther, S.; Heiz, U. 2013, Surf. Sci. 609: 18. doi: 10.1016/j.susc.2012.09.005 Spirkl,F.S.;Kunz,S.;Schweinberger,F.F.;Farnbacher,A.;Schröter,R.;Heiz,U. 2012, Rev. Sci. Instr. 83: 013144. doi: 10.1063/1.3677648 Kunz, S.; Hartl, K.; Nesselberger, M.; Schweinberger, F.F.; Kwon, G.; Hanzlik, M.; Mayrhofer, K. J.J.; Heiz, U.; Arenz, M. 2010, PCCP 12: 10288. doi: 10.1039/c0cp00288g Don’t waste time, or time will waste you — Muse For Lisa Supervisor’s Foreword Studying the influence of the precise size of the catalytically active species on reactivityisofmajorinterestincatalyticresearchbutisstillextremelydemanding. TherearefewexamplescarriedoutintheUHVshowingthatacatalyticprocesscan indeedbetunedbytheprecisenumberofatomsinthecatalyst.Undermorerealistic conditions, e.g. ambient pressure or liquid environment, such investigations are almost completely missing. Florian Schweinberger tackled in his doctoral thesis CatalysiswithSupportedSize-SelectedPlatinumClusters:FundamentalUHVand AppliedAmbientExperimentsbothtopicsandpresentsresultsbothfromUHVand ambient studies. His work has been exceptionally well received and the doctoral thesis is particularlywell written. Fromthewealthoftheobtainedresults,Iwouldliketohighlightjustafew.One research topic was the building of a UPS/MIES spectroscopic setup for the investigationoftheelectronicstructureofmodelcatalystsatUHVconditions. He succeeded to develop a state-of-the-art experiment with superior sensitivity and measuredthemolecularstateofadsorbedTCEonavarietyofsurfaces.Fromthese data, he could describe the bonding behavior of the molecule to the surface; furthermore,hestudiedtheinteractionofTCEwithsize-selectedplatinumclusters anddescribedthecorrespondingbondingbehavior.Theseresultsformedthebasis forfurtherstudiesontheinteractionofethenewithplatinumclustersandongoing studies on the hydrogenation of olefins in the UHV. A further highlight is the investigation of the water splitting reaction on size- selected platinum clusters on CdS nanorods that he performed in a collaborative effort between the Technische Universität München and the Ludwig-Maximilian- UniversitätMünchen.Hepreparedthemetal-cluster-semiconductorphotocatalysts intheUHVandmeasuredtheH evolutioninliquidwateruponradiationofvisible 2 light.Heobservedthatjustabout40platinumclustersonasingleCdSnanorodare enough for reaching maximal reactivity. This important finding will contribute to minimize the amount of precious platinum in industrial photocatalysts. Further- more,hediscovereddistinctsizeeffectswithPt tobethemostactivecatalystfor 46 theH evolution reaction.Forthe rationalizationofthissurprising sizeeffects, he 2 could formulate a simple model where the position of the cluster’s LUMO with respect to the lower edge of the conduction band of the semiconductor and the H?/H electrochemical potential is key for the photochemical reaction rate. 2 xi xii Supervisor’sForeword Theseimpressiveresultsareunderlaidbyathoroughcharacterizationbymeansof highresolutionSTEMandXPS,showingthatthephotocatalystsdoindeedconsist ofsize-selectedclustersand are surprisingly stable inaqueous solution. Overall,thedoctoralthesisthatFlorianpresentsisnotonlyinterestingforallof those who want to perform similar experiments but also because of the superb scientific insights. Munich, April 2013 Prof. Ueli Heiz
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