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钯-多壁碳纳米管气体扩散电极在水介质中对二氧化碳进行电化学还原生成有机酸

Electrochemical reduction of CO₂ to organic acids by a Pd-MWNTs gas-diffusion electrode in aqueous medium.

作者信息

Lu Guang, Wang Hui, Bian Zhaoyong, Liu Xin

机构信息

College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China.

College of Water Sciences, Beijing Normal University, Beijing 100875, China.

出版信息

ScientificWorldJournal. 2013 Dec 22;2013:424617. doi: 10.1155/2013/424617. eCollection 2013.

Abstract

Pd-multiwalled carbon nanotubes (Pd-MWNTs) catalysts for the conversion of CO₂ to organic acids were prepared by the ethylene glycol reduction and fully characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV) technologies. The amorphous Pd particles with an average size of 5.7 nm were highly dispersed on the surface of carbon nanotubes. Functional groups of the MWNTs played a key role in the palladium deposition. The results indicated that Pd-MWNTs could transform CO₂ into organic acid with high catalytic activity and CO₂ could take part in the reduction reaction directly. Additionally, the electrochemical reduction of CO₂ was investigated by a diaphragm electrolysis device, using a Pd-MWNTs gas-diffusion electrode as a cathode and a Ti/RuO₂ net as an anode. The main products in present system were formic acid and acetic acid identified by ion chromatograph. The selectivity of the products could be achieved by reaction conditions changing. The optimum faraday efficiencies of formic and acetic acids formed on the Pd-MWNTs gas-diffusion electrode at 4₂V electrode voltages under 1 atm CO₂ were 34.5% and 52.3%, respectively.

摘要

通过乙二醇还原法制备了用于将二氧化碳转化为有机酸的钯-多壁碳纳米管(Pd-MWNTs)催化剂,并采用傅里叶变换红外光谱(FTIR)、X射线衍射(XRD)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)和循环伏安法(CV)技术对其进行了全面表征。平均粒径为5.7 nm的非晶态钯颗粒高度分散在碳纳米管表面。多壁碳纳米管的官能团在钯的沉积过程中起关键作用。结果表明,Pd-MWNTs能够以高催化活性将二氧化碳转化为有机酸,且二氧化碳可直接参与还原反应。此外,使用Pd-MWNTs气体扩散电极作为阴极、Ti/RuO₂网作为阳极的隔膜电解装置对二氧化碳的电化学还原进行了研究。通过离子色谱法确定该体系中的主要产物为甲酸和乙酸。通过改变反应条件可以实现产物的选择性。在1 atm二氧化碳压力下,4₂V电极电压时,Pd-MWNTs气体扩散电极上生成甲酸和乙酸的最佳法拉第效率分别为34.5%和52.3%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a3f3/3885284/3331c4febd2b/TSWJ2013-424617.001.jpg

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