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CaCl2基熔盐捕集CO2制备高附加值碳材料阴极过程协同调控机制研究
结题报告
批准号:
51804056
项目类别:
青年科学基金项目
资助金额:
24.0 万元
负责人:
胡丽文
依托单位:
学科分类:
E0410.冶金物理化学与冶金原理
结题年份:
2021
批准年份:
2018
项目状态:
已结题
项目参与者:
黎江玲、游志雄、邓青宇、范刚强、吕泽鹏、张润、武义杰
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中文摘要
近年来,高温熔盐捕集CO2电化学转化制备碳纳米管和石墨烯等高附加值碳材料,已成为CO2减排和资源化利用领域的研究热点。但现有研究仍然存在诸多问题,首先未阐明多因素条件下CO32-在阴极的还原机理和动力学,其次阴极产物形貌与电解条件的协同调控机制不明晰且产物纯度较低。针对上述问题,本项目拟首先在含氧氯化物熔体中,采用自制耐腐蚀惰性阳极,以石墨为工作电极,Ag/AgCl为参比电极,通过循环/方波伏安法结合气相质谱等分析方法研究多因素条件下CO32-的阴极还原动力学,并通过高斯拟合解析阴极还原机理;其次,采用原位分析结合高分辨表征技术,研究不同电解条件下阴极产物形核和生长的协同调控机理;最后,通过优化电解条件,实现高纯度和高附加值碳产物的可控制备。项目研究成果可期望与可再生能源(如太阳能)利用相结合,从而为CO2的减排及其向高附加值碳资源的转化与综合利用提供新途径。
英文摘要
Recently, the capture and electrochemical conversion of CO2 by molten salt electrolysis into value-added materilais, such as carbon nanotube and graphene, has became a hot research spot in the area of reduction and comprehensive utilization of CO2. However, the cathodic reduction mechanism of CO2 in molten salt is still not clear, and the relationship between morphologies and electrolytic conditions is also confusing. Moreover, the cathodic product is still of poor quality. In this paper, cyclic voltammogram and square wave voltammetry together with gas mass spectrometry will be employed to investigate the cathodic reduction kinetics of CO32- in molten CaCl2 first, using the as-prepared inert anode, graphite as the cathode and Ag/AgCl as the reference electrode. And the cathodic reduction mechanism will be further clarified by processing data with gaussian fitting. Secondly, the nucleation and growth mechanism of the carbon at the cathode under different electrolytic conditions will also be investigated in situ by high resolution characterization techniques. At last, the successful capture and electrochemical conversion of CO2 into desired pure and value-added carbonaceous materials will be realized, by optimizing the electrolytic condition, and clarifying the cooperative regulation mechanism of the nucleation and growth of carbon at the cathode. The obtained results can be applied with renewable energy such as solar energy, which will offer a new approach for CO2 emission reduction, its conversion into value-added materials and comprehensive utilization of CO2.
近年来,高温熔盐捕集CO2电化学转化制备碳纳米管和石墨烯等高附加值碳材料,已成为CO2减排和资源化利用领域的研究热点。但现有研究仍然存在诸多问题,首先未阐明多因素条件下CO32-在阴极的还原机理和动力学,其次阴极产物形貌与电解条件的协同调控机制不明晰且产物纯度较低。本项目通过固相烧结制备了RuO2-TiO2及TiO2-Ni惰性阳极,并对RuO2-TiO2惰性阳极耐化学腐蚀和电化学腐蚀的性能进行了测试,结合在线气体分析了电解过程中阳极气体成分;采用电分析技术获得了RuO2-TiO2阳极极化电位和析氧阻抗;揭示了RuO2-TiO2及TiO2-Ni阳极对电解槽压、电流效率和阴极产物形貌与结构的影响;通过调节电解温度、熔盐成分、电极种类,获得碳酸根阴极还原产物结构与形貌协同调控机制,并结合COMSOL Multiphysics模拟仿真软件,揭示了不同电极交换电流密度对阴极碳沉积动力学及电流效率的影响;通过电解过程多因素的协同调控,揭示了阴极产物形貌和石墨化程度的演变规律,并成功制备出高纯度硫掺杂碳纤维和碳纳米管。
期刊论文列表
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专利列表
DOI:10.1016/j.jallcom.2020.154003
发表时间:2020
期刊:Journal of Alloys and Compounds
影响因子:6.2
作者:Liu Pengjie;Hu Mengjun;Hu Liwen;Yin Mingzhu;Wu Hongfei;Hu Meilong
通讯作者:Hu Meilong
Transient shrinkage behavior of wustite-centered binary/ternary/quaternary/quinary-component oxide packed beds in a reducing atmosphere up to 1773 K
维氏体中心二元/三元/四元/五元组分氧化物填充床在高达 1773 K 的还原气氛中的瞬态收缩行为
DOI:10.1016/j.ceramint.2020.01.220
发表时间:2020-06
期刊:Ceramics International
影响因子:5.2
作者:Deng Junyi;Ma Kaihui;Hu Liwen;Kou Mingyin;Wen Liangying;Xu Jian
通讯作者:Xu Jian
DOI:10.1149/1945-7111/aba401
发表时间:2020-08
期刊:Journal of the Electrochemical Society
影响因子:3.9
作者:Liu Pengjie;Hou Zhuoran;Hu Mengjun;Hu Liwen;Tang Rong;Wu Hongfei;Hu Meilong
通讯作者:Hu Meilong
DOI:10.1016/j.jallcom.2020.155364
发表时间:2020-09
期刊:Journal of Alloys and Compounds
影响因子:6.2
作者:Wu Hongfei;Liu Pengjie;Yin Mingzhu;Hou Zhuoran;Hua Liwen;Dang Jie
通讯作者:Dang Jie
DOI:10.1016/j.jmst.2021.06.047
发表时间:2022
期刊:Journal of Materials Science & Technology
影响因子:10.9
作者:胡丽文
通讯作者:胡丽文
熔盐电化学刻蚀制备(V/Ti)2CTx多尺度结构调控与电化学性能增强机制
  • 批准号:
    --
  • 项目类别:
    面上项目
  • 资助金额:
    54万元
  • 批准年份:
    2022
  • 负责人:
    胡丽文
  • 依托单位:
国内基金
海外基金