Hydrogen-generating behavior of Pd-decorated gold nanoparticles via formic acid decomposition

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dc.citation.firstpage24en_US
dc.citation.journalTitleCatalysis Todayen_US
dc.citation.lastpage31en_US
dc.citation.volumeNumber330en_US
dc.contributor.authorZhao, Zhunen_US
dc.contributor.authorHeck, Kimberly N.en_US
dc.contributor.authorLimpornpipat, Pongsaken_US
dc.contributor.authorQian, Huifengen_US
dc.contributor.authorMiller, Jeffrey T.en_US
dc.contributor.authorWong, Michael S.en_US
dc.date.accessioned2019-08-28T15:02:59Zen_US
dc.date.available2019-08-28T15:02:59Zen_US
dc.date.issued2019en_US
dc.description.abstractFormic acid is a promising hydrogen storage material where hydrogen is generated via metal-catalyzed decomposition. Bimetallic catalysts are active for this reaction, but the mechanism has not been fully proven. Palladium metal supported on gold nanoparticles (Pd-on-Au NPs) has structural properties that are advantageous for studying aqueous-phase catalytic reactions. In this work, a series of Pd-on-Au NPs of varying Pd loadings (calculated in terms of Pd surface coverage, sc%) were synthesized, immobilized onto carbon, and studied for formic acid decomposition at room temperature. Pd-on-Au NPs were catalytically active, with a reaction rate constant as high as 137 m L-H2/gPd/min (corresponding to an initial turnover frequency TOF of 123 h−1) at a Pd loading of 300 sc%. In contrast, Au NPs were inactive, and Pd NPs were slightly active (5 mL-H2/gPd/min and TOF of 38 h−1). The Pd metal of Pd-on-Au catalysts are partially oxidized, and is readily reduced without changing the metal-on-metal structure during reaction, according to in situ x-ray adsorption spectroscopy measurements. CO formation was inhibited at a Pd loading of 300 sc%, suggesting that three-dimensional Pd ensembles favored the desired dehydrogenation pathway while single-atom and small two-dimensional Pd ensembles are active for the undesired dehydration pathway.en_US
dc.identifier.citationZhao, Zhun, Heck, Kimberly N., Limpornpipat, Pongsak, et al.. "Hydrogen-generating behavior of Pd-decorated gold nanoparticles via formic acid decomposition." <i>Catalysis Today,</i> 330, (2019) Elsevier: 24-31. https://doi.org/10.1016/j.cattod.2018.06.044.en_US
dc.identifier.doihttps://doi.org/10.1016/j.cattod.2018.06.044en_US
dc.identifier.urihttps://hdl.handle.net/1911/107364en_US
dc.language.isoengen_US
dc.publisherElsevieren_US
dc.rightsThis is an author's peer-reviewed final manuscript, as accepted by the publisher. The published article is copyrighted by Elsevier.en_US
dc.subject.keywordNanoparticlesen_US
dc.subject.keywordPalladiumen_US
dc.subject.keywordGolden_US
dc.subject.keywordBimetallicen_US
dc.subject.keywordFormic aciden_US
dc.subject.keywordHydrogenen_US
dc.subject.keywordCatalysten_US
dc.titleHydrogen-generating behavior of Pd-decorated gold nanoparticles via formic acid decompositionen_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpost-printen_US
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