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

James M. Krier; William D. Michalak; Xiaojun Cai; Lindsay Carl; Kyriakos Komvopoulos; Gabor A. Somorjai

doi:10.1021/nl502566b

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

James M. Krier, William D. Michalak, Xiaojun Cai, Lindsay Carl, Kyriakos Komvopoulos, Gabor A. Somorjai

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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.

Original language	English (US)
Pages (from-to)	39-44
Number of pages	6
Journal	Nano Letters
Volume	15
Issue number	1
DOIs	https://doi.org/10.1021/nl502566b
State	Published - Dec 8 2014
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: 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.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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@article{da3738f34ac24accaf030a64ad97fe30,

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",

abstract = "{\textcopyright} 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 (St{\"o}ber 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.",

author = "Krier, {James M.} and Michalak, {William D.} and Xiaojun Cai and Lindsay Carl and Kyriakos Komvopoulos and Somorjai, {Gabor A.}",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: 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. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

year = "2014",

month = dec,

day = "8",

doi = "10.1021/nl502566b",

language = "English (US)",

volume = "15",

pages = "39--44",

journal = "Nano Letters",

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publisher = "American Chemical Society",

number = "1",

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T1 - 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

AU - Krier, James M.

AU - Michalak, William D.

AU - Cai, Xiaojun

AU - Carl, Lindsay

AU - Komvopoulos, Kyriakos

AU - Somorjai, Gabor A.

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: 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. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2014/12/8

Y1 - 2014/12/8

N2 - © 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.

AB - © 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.

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UR - https://pubs.acs.org/doi/10.1021/nl502566b

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U2 - 10.1021/nl502566b

DO - 10.1021/nl502566b

M3 - Article

C2 - 25272243

SN - 1530-6984

VL - 15

SP - 39

EP - 44

JO - Nano Letters

JF - Nano Letters

IS - 1

ER -

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

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