二氧化碳的电化学还原
摘要
二氧化碳的电催化还原是当前电化学研究领域中相当活跃的课题，它的发展对解决人类面临的能源和环境问题，对推动电催化理论研究的进展都具有重要的意义。
本论文基于化学修饰电极的原理，以期实现其对二氧化碳电催化还原性能的提高，主要开展了以下几个方面的工作：
第一章在查阅百余份参考文献的基础上，对二氧化碳电化学还原的发展和现状进行了综述。
第二章通过FT-IR、SEM和XRD研究了CuO/TiO2-Cu修饰电极在光电解前、后的表面结构特征，并通过循环伏安法和恒电位光电解等手段研究了CuO/TiO2-Cu修饰电极对CO2的光电催化活性。
第三章在铂电极上电化学沉积了Se/CdSe纳米薄膜并以SEM、XRD对薄膜进行了表征，利用循环伏安、恒电位光电解等方法研究修饰电极对CO2的光电催化活性。
第四章通过循环伏安法在铂电极上电聚合了PAni/PMo12/CuHCF薄膜，并对二氧化碳在该修饰电极上的电催化还原进行了研究。
第五章通过化学方法把RuO2分别担载在TiO2纳米管和TiO2纳米粒子上，在NaHCO3水溶液中，利用循环伏安、稳态极化和恒电位极化等方法分别研究了RuO2/TiO2纳米粒子和RuO2/TiO2纳米管复合物薄膜修饰Pt电极对CO2的电催化还原活性。
第六章通过超声方法在三乙醇胺和乙醇的混合水溶液中将RuO2担载在单壁碳纳米管上，并以0.05% Nafion溶液在铂电极上制备成修饰电极。在NaHCO3水溶液中，利用循环伏安、稳态极化和恒电位极化等方法分别研究了RuO2/SWNTs，RuO2和SWNTs薄膜修饰电极对CO2的电催化还原活性。
The electrocatalytic and photoelectrocatalytic reduction of CO2 is of importance in application of electrochemical synthesis. The development of the study may contribute to solve the energy and environment problems that our societies are facing nowadays. In this thesis, based on the principle of chemically modified electrodes, the improved electrochemical performance for CO2 reduction was investigated. The main results and conclusions are summarized as following:
The first chapter is introduction. The development and present researches of CO2 reduction were summarized based on a lot of references.
The second chapter is the photoelectrochemical reduction of CO2 at CuO2/TiO2-Cu modified electrode. The surface characteristics of CuO/TiO2-Cu composites electrode were fully investigated before and after the photoelectrochemical reduction of CO2 by using FT-IR、SEM and XRD. The photoelectrochemical catalytic activity of this CuO/TiO2-Cu composites electrode for CO2 was further proved by means of such electrochemical measurements as cyclic voltammetry and photoelectrolysis.
The third chapter is the photoelectrocatalytic activity for the reduction of CO2 on Se/CdSe-Pt nanometer films electrode. The Se/CdSe thin film was prepared on the platinum electrode by potentiostatic at –0.69 V vs.SCE. This film was characterized by SEM and XRD, respectively. The photoelectrocatalytic activity of this modified electrode for the CO2 reduction was investigated by cyclic voltammetry and potentiostatic electrolysis.
The fourth chapter is the electrocatalytic reduction of carbon dioxide on PAni/PMo12/CuHCF-Pt electrode. The PAni/PMo12/CuHCF-Pt modified electrode was prepared by the electrochemical method, and applied to the electrochemical reduction of
CO2 in KHCO3 aqueous solution.
The fifth chapter is the electrochemical catalytic reduction of CO2 on the RuO2 /TiO2 nanotubes and RuO2/TiO2 nanoparticles composites modified Pt electrode. The electrocatalytic activity of two composites modified electrode for CO2 reduction were investigated by using CV、steady-state polarization and electrolysis in aqueous solution, respectively.
The sixth chapter is the enhanced electrocatalytic reduction of CO2 at RuO2/SWNTs composites-Nafion modified platinum electrode. RuO2/SWNTs composites were prepared by loading of RuO2 on SWNTs in a mixed aqueous solution of thiethanolamine + ethanol by ultrasound irradiation. The RuO2/SWNTs composites were dispersed into 0.05% Nafion aqueous solution via ultrasonication, and subsequently, the RuO2/SWNTs composites-Nafion film coated Pt electrode was obtained through evaporating solvent from the RuO2/SWNTs composites-Nafion suspension. The electrocatalytic reduction of CO2 at RuO2/SWNTs composites-Nafion modified Pt electrode were investigated by CV、steady-state polarization and potentiostatic polarization in aqueous solution, respectively.
本论文基于化学修饰电极的原理，以期实现其对二氧化碳电催化还原性能的提高，主要开展了以下几个方面的工作：
第一章在查阅百余份参考文献的基础上，对二氧化碳电化学还原的发展和现状进行了综述。
第二章通过FT-IR、SEM和XRD研究了CuO/TiO2-Cu修饰电极在光电解前、后的表面结构特征，并通过循环伏安法和恒电位光电解等手段研究了CuO/TiO2-Cu修饰电极对CO2的光电催化活性。
第三章在铂电极上电化学沉积了Se/CdSe纳米薄膜并以SEM、XRD对薄膜进行了表征，利用循环伏安、恒电位光电解等方法研究修饰电极对CO2的光电催化活性。
第四章通过循环伏安法在铂电极上电聚合了PAni/PMo12/CuHCF薄膜，并对二氧化碳在该修饰电极上的电催化还原进行了研究。
第五章通过化学方法把RuO2分别担载在TiO2纳米管和TiO2纳米粒子上，在NaHCO3水溶液中，利用循环伏安、稳态极化和恒电位极化等方法分别研究了RuO2/TiO2纳米粒子和RuO2/TiO2纳米管复合物薄膜修饰Pt电极对CO2的电催化还原活性。
第六章通过超声方法在三乙醇胺和乙醇的混合水溶液中将RuO2担载在单壁碳纳米管上，并以0.05% Nafion溶液在铂电极上制备成修饰电极。在NaHCO3水溶液中，利用循环伏安、稳态极化和恒电位极化等方法分别研究了RuO2/SWNTs，RuO2和SWNTs薄膜修饰电极对CO2的电催化还原活性。
The electrocatalytic and photoelectrocatalytic reduction of CO2 is of importance in application of electrochemical synthesis. The development of the study may contribute to solve the energy and environment problems that our societies are facing nowadays. In this thesis, based on the principle of chemically modified electrodes, the improved electrochemical performance for CO2 reduction was investigated. The main results and conclusions are summarized as following:
The first chapter is introduction. The development and present researches of CO2 reduction were summarized based on a lot of references.
The second chapter is the photoelectrochemical reduction of CO2 at CuO2/TiO2-Cu modified electrode. The surface characteristics of CuO/TiO2-Cu composites electrode were fully investigated before and after the photoelectrochemical reduction of CO2 by using FT-IR、SEM and XRD. The photoelectrochemical catalytic activity of this CuO/TiO2-Cu composites electrode for CO2 was further proved by means of such electrochemical measurements as cyclic voltammetry and photoelectrolysis.
The third chapter is the photoelectrocatalytic activity for the reduction of CO2 on Se/CdSe-Pt nanometer films electrode. The Se/CdSe thin film was prepared on the platinum electrode by potentiostatic at –0.69 V vs.SCE. This film was characterized by SEM and XRD, respectively. The photoelectrocatalytic activity of this modified electrode for the CO2 reduction was investigated by cyclic voltammetry and potentiostatic electrolysis.
The fourth chapter is the electrocatalytic reduction of carbon dioxide on PAni/PMo12/CuHCF-Pt electrode. The PAni/PMo12/CuHCF-Pt modified electrode was prepared by the electrochemical method, and applied to the electrochemical reduction of
CO2 in KHCO3 aqueous solution.
The fifth chapter is the electrochemical catalytic reduction of CO2 on the RuO2 /TiO2 nanotubes and RuO2/TiO2 nanoparticles composites modified Pt electrode. The electrocatalytic activity of two composites modified electrode for CO2 reduction were investigated by using CV、steady-state polarization and electrolysis in aqueous solution, respectively.
The sixth chapter is the enhanced electrocatalytic reduction of CO2 at RuO2/SWNTs composites-Nafion modified platinum electrode. RuO2/SWNTs composites were prepared by loading of RuO2 on SWNTs in a mixed aqueous solution of thiethanolamine + ethanol by ultrasound irradiation. The RuO2/SWNTs composites were dispersed into 0.05% Nafion aqueous solution via ultrasonication, and subsequently, the RuO2/SWNTs composites-Nafion film coated Pt electrode was obtained through evaporating solvent from the RuO2/SWNTs composites-Nafion suspension. The electrocatalytic reduction of CO2 at RuO2/SWNTs composites-Nafion modified Pt electrode were investigated by CV、steady-state polarization and potentiostatic polarization in aqueous solution, respectively.
引文
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