Citation: SUN Li-zhi, YI Qing-feng, LIU Xiao-ping. Electrocatalytic oxidation of propanol and butanol isomers on palladium-nickel catalyst[J]. Journal of Fuel Chemistry and Technology, ;2013, 41(10): 1274-1280. shu

Electrocatalytic oxidation of propanol and butanol isomers on palladium-nickel catalyst

1.
School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan 411201, China

Corresponding author: YI Qing-feng,
Received Date: 25 February 2013
Available Online: 20 April 2013
Fund Project: 国家自然科学基金(21376070, 20876038) (21376070, 20876038)湖南省高校创新平台开放基金(11K023) (11K023)湖南省发委科技基本建设项目([2010]1060)。 ([2010]1060)

β-cyclodextrin (β-CD) with a special cavity structure was firstly grafted on the surface of multi-walled carbon nanotubes (MWCNTs), which were then immobilized on Ti plates to obtain the β-CD/MWCNT/Ti substrate. Binary Pd-Ni nanoparticles were electrodeposited on the surface of β-CD/MWCNT/Ti substrate to prepare the PdNi-β-CD/MWCN/Ti electrode; its activity in electrocatalytic oxidation of propanol and butanol isomers in alkaline media was then investigated by voltammetry, chronoamperometry and electrochemical impedance spectroscopy. The results indicated that the binary PdNi nanoparticles are highly dispersed with the size of 90~130 nm on the β-CD/MWCNT/Ti substrate. The configuration of alcohols plays a significant role in their electrochemical oxidation activity in alkaline media on the PdNi-β-CD/MWCNT/Ti electrode. For the two propanol isomers, the PdNi-β-CD/MWCNT/Ti electrode exhibits much higher electroactivity for 1-propanol oxidation than that for 2-propanol oxidation. For the four butanol isomers, the electrocatalytic activity of the PdNi-β-CD/MWCNT/Ti electrode towards their oxidation follows the order of 1-butanol > 2-methyl-propanol > 2-butanol >> 2-methyl-2-propanol; the electrode shows almost no electrocatalytic activity in the oxidation of tertiary butanol. The mechanism for the electrocatalytic oxidation of various propanol and butanol isomers was also analyzed by considering the Muliken net charge on the different carbon atoms bonded with hydroxyl –OH, which indicates that the alcohol molecule with lower Muliken net charge value will be more easily oxidized over the PdNi-β-CD/MWCNT/Ti electrode.
- PdNi electrocatalyst,
- propanol oxidation,
- butanol oxidation,
- β-cyclodextrin,
- Muliken charge
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沈阳化工大学材料科学与工程学院沈阳 110142