Sum Frequency Generation Vibrational Spectroscopy of 1,3-Butadiene Hydrogenation on 4 nm Pt@SiO 2 , Pd@SiO 2 , and Rh@SiO 2 Core–Shell Catalysts

Handle URI:
http://hdl.handle.net/10754/599798
Title:
Sum Frequency Generation Vibrational Spectroscopy of 1,3-Butadiene Hydrogenation on 4 nm Pt@SiO 2 , Pd@SiO 2 , and Rh@SiO 2 Core–Shell Catalysts
Authors:
Krier, James M.; Michalak, William D.; Cai, Xiaojun; Carl, Lindsay; Komvopoulos, Kyriakos; Somorjai, Gabor A.
Abstract:
© 2014 American Chemical Society. 1,3-Butadiene (1,3-BD) hydrogenation was performed on 4 nm Pt, Pd, and Rh nanoparticles (NPs) encapsulated in SiO2 shells at 20, 60, and 100 °C. The core-shells were grown around polyvinylpyrrolidone (PVP) coated NPs (Stöber encapsulation) prepared by colloidal synthesis. Sum frequency generation (SFG) vibrational spectroscopy was performed to correlate surface intermediates observed in situ with reaction selectivity. It is shown that calcination is effective in removing PVP, and the SFG signal can be generated from the metal surface. Using SFG, it is possible to compare the surface vibrational spectrum of Pt@SiO2 (1,3-BD is hydrogenated through multiple paths and produces butane, 1-butene, and cis/trans-2-butene) to Pd@SiO2 (1,3-BD favors one path and produces 1-butene and cis/trans-2-butene). In contrast to Pt@SiO2 and Pd@SiO2, SFG and kinetic experiments of Rh@SiO2 show a permanent accumulation of organic material.
Citation:
Krier JM, Michalak WD, Cai X, Carl L, Komvopoulos K, et al. (2015) Sum Frequency Generation Vibrational Spectroscopy of 1,3-Butadiene Hydrogenation on 4 nm Pt@SiO 2 , Pd@SiO 2 , and Rh@SiO 2 Core–Shell Catalysts . Nano Lett 15: 39–44. Available: http://dx.doi.org/10.1021/nl502566b.
Publisher:
American Chemical Society (ACS)
Journal:
Nano Letters
Issue Date:
14-Jan-2015
DOI:
10.1021/nl502566b
PubMed ID:
25272243
Type:
Article
ISSN:
1530-6984; 1530-6992
Sponsors:
This work was supported by the Director, Office of Basic Energy Sciences, Materials Sciences and Engineering Division of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. One of the authors (K.K.) also acknowledges funding provided by the UCB-KAUST Academic Excellence Alliance (AEA) Program for this research.
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Full metadata record

DC FieldValue Language
dc.contributor.authorKrier, James M.en
dc.contributor.authorMichalak, William D.en
dc.contributor.authorCai, Xiaojunen
dc.contributor.authorCarl, Lindsayen
dc.contributor.authorKomvopoulos, Kyriakosen
dc.contributor.authorSomorjai, Gabor A.en
dc.date.accessioned2016-02-28T06:10:04Zen
dc.date.available2016-02-28T06:10:04Zen
dc.date.issued2015-01-14en
dc.identifier.citationKrier JM, Michalak WD, Cai X, Carl L, Komvopoulos K, et al. (2015) Sum Frequency Generation Vibrational Spectroscopy of 1,3-Butadiene Hydrogenation on 4 nm Pt@SiO 2 , Pd@SiO 2 , and Rh@SiO 2 Core–Shell Catalysts . Nano Lett 15: 39–44. Available: http://dx.doi.org/10.1021/nl502566b.en
dc.identifier.issn1530-6984en
dc.identifier.issn1530-6992en
dc.identifier.pmid25272243en
dc.identifier.doi10.1021/nl502566ben
dc.identifier.urihttp://hdl.handle.net/10754/599798en
dc.description.abstract© 2014 American Chemical Society. 1,3-Butadiene (1,3-BD) hydrogenation was performed on 4 nm Pt, Pd, and Rh nanoparticles (NPs) encapsulated in SiO2 shells at 20, 60, and 100 °C. The core-shells were grown around polyvinylpyrrolidone (PVP) coated NPs (Stöber encapsulation) prepared by colloidal synthesis. Sum frequency generation (SFG) vibrational spectroscopy was performed to correlate surface intermediates observed in situ with reaction selectivity. It is shown that calcination is effective in removing PVP, and the SFG signal can be generated from the metal surface. Using SFG, it is possible to compare the surface vibrational spectrum of Pt@SiO2 (1,3-BD is hydrogenated through multiple paths and produces butane, 1-butene, and cis/trans-2-butene) to Pd@SiO2 (1,3-BD favors one path and produces 1-butene and cis/trans-2-butene). In contrast to Pt@SiO2 and Pd@SiO2, SFG and kinetic experiments of Rh@SiO2 show a permanent accumulation of organic material.en
dc.description.sponsorshipThis work was supported by the Director, Office of Basic Energy Sciences, Materials Sciences and Engineering Division of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. One of the authors (K.K.) also acknowledges funding provided by the UCB-KAUST Academic Excellence Alliance (AEA) Program for this research.en
dc.publisherAmerican Chemical Society (ACS)en
dc.subject1,3-Butadiene hydrogenationen
dc.subjectcore-shell nanoparticlesen
dc.subjectsurface vibrational spectroscopyen
dc.titleSum Frequency Generation Vibrational Spectroscopy of 1,3-Butadiene Hydrogenation on 4 nm Pt@SiO 2 , Pd@SiO 2 , and Rh@SiO 2 Core–Shell Catalystsen
dc.typeArticleen
dc.identifier.journalNano Lettersen
dc.contributor.institutionLawrence Berkeley National Laboratory, Berkeley, United Statesen
dc.contributor.institutionUC Berkeley, Berkeley, United Statesen
kaust.grant.programAcademic Excellence Alliance (AEA)en
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