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

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

Pu Zhang ^a, ,
Yi Wei ^a ,
Jun Cai ^a ,
Yan-Xia Chen ^a ,
Zhong-Qun Tian ^b

a. Hefei National Laboratory for Physical Sciences at Microscale Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, Anhui, China;
b. State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, Fujian, China

Received Date: 14 March 2016
Revised Date: 14 April 2016

Fund Project: This work was supported by the National Natural Science Foundation of China (21473175), the National Instrumentation Program (2011YQ03012416) and the National Basic Reserarch Program of China (973 Program, 2015CB932301).

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.
- Carbon monoxide,
- Surface-enhanced Raman spectroscopy,
- Palladium,
- Density functional theory,
- Stark effect
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