化工进展 ›› 2019, Vol. 38 ›› Issue (9): 4174-4182.DOI: 10.16085/j.issn.1000-6613.2018-2309

• 材料科学与技术 • 上一篇    下一篇

熔盐体系组成对二氧化碳电化学合成新型碳材料形貌影响

李志达(),李金莲,吴红军()   

  1. 东北石油大学化学化工学院,黑龙江 大庆 163318
  • 收稿日期:2018-11-27 出版日期:2019-09-05 发布日期:2019-09-05
  • 通讯作者: 吴红军
  • 作者简介:李志达(1991—),男,博士研究生,研究方向为CO2熔盐捕集与转化。E-mail:dongyou1234@163.com
  • 基金资助:
    国家自然科学基金(21476046);黑龙江省杰出青年科学基金(JC2017002);东北石油大学科研项目(GLJHB201901)

Impact of molten salts conformation on the morphology of the electrochemically synthesized carbon materials

Zhida LI(),Jinlian LI,Hongjun WU()   

  1. College of Chemistry & Chemical Engineering, Northeast Petroleum University, Daqing 163318, Heilongjiang, China
  • Received:2018-11-27 Online:2019-09-05 Published:2019-09-05
  • Contact: Hongjun WU

摘要:

以碳酸盐为电解质,以铁、镍、镍铬合金等廉价金属材料为电极,研究构建了高温熔盐电解池,将CO2一步法转化为新型碳材料,并考察了熔盐组成及配比、电解温度、电流密度、电极材料等实验条件对碳材料形貌结构的影响。采用X射线能谱分析仪(EDS)、扫描电镜(SEM)、透射电镜(TEM)、比表面积测试仪(BET)、X射线衍射仪(XRD)及拉曼光谱仪(Raman)等手段对碳材料的元素组成、形貌结构、比表面积、结晶度、有序度等特性进行表征分析。研究结果表明,450~600℃温度范围内,电解多元混合熔盐体系主要生成无定形碳;同时,电解温度、电流密度、电解质组成及配比等对碳产物的比表面积具有明显影响;通过改变电解质体系,辅以调控电流密度及电解温度等实验参数,可实现碳纳米管、碳球及蜂窝状多孔碳等特定形貌碳材料的可控合成,其中碳纳米管的石墨化程度较高,且由碳原子组成的层状六方石墨晶体排列规则有序。

关键词: 二氧化碳, 熔融碳酸盐, 碳纳米管, 碳球, 蜂窝状多孔碳

Abstract:

This research aims to provide a feasible route to achieve the CO2 reduction and utilization. With carbonate used as electrolyte, and inexpensive Fe, Ni and Ni-Cr as electrodes, a molten carbonate electrolyzer is established and CO2 is facilely converted into novel carbon materials. Moreover, the impact of the electrolyte conformation, electrolytic temperature, current density and electrode material on the morphology of the synthesized carbon products are studied. Electron dispersive spectroscope (EDS), scanning electron microscope (SEM), transmission electron microscope (TEM), Brunauer-Emmett-Teller (BET) analyzer, X-ray diffractometer (XRD) and Raman spectroscope (Raman) are employed to characterize the element composition, morphology & structure, BET surface area, crystallinity and graphite crystal regularity of the prepared carbon materials. The results demonstrate that hybrid carbonates electrolysis under 450℃ to 600℃ prefers amorphous carbons generation. BET surface area significantly depends on the applied temperature, current density and electrolyte composition, where lower temperature and elevated current density provide carbon products with a higher BET surface area. Moreover, the ambient CO2 could be controllably transformed into carbon materials with desirable microstructures such as carbon nanotubes, carbon spheres and honeycomb-like carbon through regulating the electrolytic parameters of electrolyte conformation, temperature, electrode materials, etc. Of all the synthetic carbon materials, carbon nanotubes exhibit the highest graphitization and the most ordered hexagonal graphite crystals. This work demonstrates a feasible route for the direct CO2 conversion and facile synthesis of nanostructured carbons, fitting well with the sustainable concept.

Key words: carbon dioxide, molten carbonates, carbon nanotubes, carbon spheres, honeycomb-like carbon

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