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
AuthorsKrier, James M.
Michalak, William D.
Somorjai, Gabor A.
Permanent link to this recordhttp://hdl.handle.net/10754/599798
MetadataShow full item record
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.
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.
SponsorsThis 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.
PublisherAmerican Chemical Society (ACS)