Citation: QIU Jian-Ping, TONG Yi-Wen, ZHAO De-Ming, HE Zhi-Qiao, CHEN Jian-Meng, SONG Shuang. Electrochemical Reduction of CO₂ to Methanol at TiO₂ Nanotube Electrodes[J]. Acta Physico-Chimica Sinica, ;2017, 33(7): 1411-1420. doi: 10.3866/PKU.WHXB201704078 shu

Electrochemical Reduction of CO₂ to Methanol at TiO₂ Nanotube Electrodes

1.
College of Environment, Zhejiang University of Technology, Hangzhou 310032, P. R. China;
2.
Jinhua Polytechnic, Jinhua 321007, Zhejiang Province, P. R. China;
3.
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, P. R. China

Received Date: 21 December 2016
Revised Date: 24 March 2017

Fund Project: The project was supported by the National Natural Science Foundation of China (21477117) and Natural Science Foundation of Zhejiang Province, China (LR14E080001, LQ15E080007, LY15B070005).

A series of highly ordered TiO₂ nanotube (TiO₂NTs) electrodes are prepared via potentiostatic anodization of Ti foil followed by calcining in air. X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), X-ray photoelectron spectroscopy (XPS), and potential steps determination are used to characterize the electrodes. The electrochemical reduction of CO₂ on these three TiO₂NTs electrodes is investigated by cyclic voltammetry and potentiostatic electrolysis in 0.1 mol·L^-1 KHCO₃ aqueous solution. Methanol is found to be the major product in electrochemical CO₂ reduction, while formic acid, formaldehyde, methane, and CO are formed as minor products. Compared with the electrodes sintered at 550 and 650℃, the optimal TiO₂NTs electrode is found to be the one calcined at 450℃ (TiO₂NTs-450). After 120 min of reaction, the Faradaic efficiency and partial current density of methanol is 85.8% and 0.2 mA·cm^-2 at -0.56 V vs. reversible hydrogen electrode (RHE), respectively. The trivalent titanium in TiO₂ serves as an efficient site for adsorption of CO₂ and stabilization of the adsorbed ·CO₂^- radical. Consequently, the reduction of CO₂ on TiO₂NTs electrodes involves a fast first electron and proton transfer followed by a slow second proton transfer as the rate-limiting step.
- TiO₂ nanotube electrode,
- Electrochemical reduction,
- CO₂,
- Methanol,
- Reaction mechanism
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

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通讯作者: 陈斌, bchen63@163.com

Electrochemical Reduction of CO₂ to Methanol at TiO₂ Nanotube Electrodes