Nonlinear Stark effect observed for carbon monoxide chemisorbed on gold core/palladium shell nanoparticle film electrodes, using in situ surface-enhanced Raman spectroscopy

doi:10.1016/S1872-2067(15)61106-8

Abstract

Abstract:

The potential (E)-dependent vibrational behavior of a saturated CO adlayer on Au-core Pd-shell nanoparticle film electrodes was investigated over a wide potential range, in acidic, neutral, and basic solutions, using in situ surface-enhanced Raman spectroscopy (SERS). Over the whole of the examined potential region (-1.5 to 0.55 V vs. NHE), the peak frequencies of both the C-O_M and the Pd-CO_M band (here, M denotes the multiply-bonded configuration) displayed three distinct linear regions: dν_C-OM/dE decreased from ~185-207 (from -1.5 to -1.2 V) to ~83-84 cm^-1/V (-1.2 to -0.15 V), and then to 43 cm^-1/V (-0.2 to 0.55 V); on the other hand, dν_Pd-COM/dE changed from ~-10 to -8 cm^-1/V (from -1.5 to -1.2 V) to ~-31 to -30 cm^-1/V (-1.2 to -0.15 V), and then to -15 cm^-1/V (-0.2 to 0.55 V). The simultaneously recorded cyclic voltammograms revealed that at E < -1.2 V, a hydrogen evolution reaction (HER) occurred. With the help of periodic density functional theory calculations using two different (2 × 2)-3CO slab models with Pd(111), the unusually high dν_C-OM/dE and the small dν_Pd-COM/dE in the HER region were explained as being due to the conversion of CO_ad from bridge to hollow sites, which was induced by the co-adsorbed hydrogen atoms formed from dissociated water at negative potentials.

Key words: Carbon monoxide, Surface-enhanced Raman spectroscopy, Palladium, Density functional theory, Stark effect

Pu Zhang, Yi Wei, Jun Cai,Yan-Xia Chen, Zhong-Qun Tian. Nonlinear Stark effect observed for carbon monoxide chemisorbed on gold core/palladium shell nanoparticle film electrodes, using in situ surface-enhanced Raman spectroscopy[J]. Chinese Journal of Catalysis, 2016, 37(7): 1156-1165.

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