Carbon nanotubes modified with electrodeposited metal porphyrins and phenanthrolines for electrocatalytic applications

Carbon nanotubes modified with electrodeposited metal porphyrins and phenanthrolines for electrocatalytic applications
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DOI:
10.1016/j.electacta.2009.11.092
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发表时间:
2010-11
影响因子:
6.6
通讯作者:
Thorsten Schilling;A. Okunola;Justus Masa;W. Schuhmann;M. Bron
Thorsten Schilling;A. Okunola;Justus Masa;W. Schuhmann;M. Bron
中科院分区:
材料科学2区
文献类型:
--
作者:
Thorsten Schilling;A. Okunola;Justus Masa;W. Schuhmann;M. Bron

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采用自下而上的合成方法,在玻碳电极上直接制备了多壁碳纳米管(MWCNTs)和含铁氮化合物作为酸性介质中氧电还原催化剂的复合材料。在第一步中,MWCNTs以墨水的形式滴涂在电极上。然后,通过脉冲电位沉积技术,用具有催化活性的卟啉铁(FeTMPP-Cl)或菲罗啉铁(Fe(phen)3)膜对纳米管进行修饰。最后在惰性气体气氛中对制备的电极进行热处理。通过使用循环伏安法和旋转圆盘电极测量表明,这种复合材料的氧还原反应(ORR)的活性随着每一个应用的合成步骤逐渐增加,表明在电极上直接合成催化剂的可能性。该工艺制备的fempp - cl /MWCNT和Fe(phen)3/MWCNT复合材料的活性均高于湿浸渍和热处理制备的同类电催化剂。所提出的方法打开了系统调整电极结构的可能性,例如通过逐步建立气体扩散电极。
Composites consisting of multi-walled carbon nanotubes (MWCNTs) and iron–nitrogen containing compounds as catalysts for the electroreduction of oxygen in acidic media were directly prepared on a glassy carbon (GC) electrode in a bottom-up synthesis. In a first step, MWCNTs were drop-coated in form of an ink onto the electrode. Afterwards the nanotubes were modified with catalytically active films of iron porphyrin (FeTMPP-Cl) or iron phenanthroline (Fe(phen)3) through a pulsed potential deposition technique. Finally the prepared electrodes were heat-treated in an inert gas atmosphere. By employing cyclic voltammetry and rotating disc electrode measurements it is shown that the activity for the oxygen reduction reaction (ORR) at such composites increases progressively with every applied synthesis step showing the possibility for direct synthesis of a catalyst on an electrode. The activities of FeTMPP-Cl/MWCNT and Fe(phen)3/MWCNT composites prepared by this technique are higher than that of similar electrocatalysts prepared by wet impregnation and heat treatment. The presented approach opens possibilities for systematic tuning of electrode structures, for example by stepwise build-up of gas diffusion electrodes.