| 杨建.多巴胺为前驱体过渡金属与N共同掺杂的碳纳米管催化剂ORR性能研究[J].分子催化,2016,30(5):409-419 |
| 多巴胺为前驱体过渡金属与N共同掺杂的碳纳米管催化剂ORR性能研究 |
| Study Electrocatalytic Performance for Oxygen Reduction Reaction of Dopamine Derived Transition Metal-Nitrogen Codoped Carbon Nanotube |
| 投稿时间：2016-10-17 修订日期：2016-10-20 |
| DOI： |
| 中文关键词: 聚多巴胺 过渡金属掺杂 多壁碳纳米管 氧还原反应 |
| 英文关键词:Polydopamine Transition metal doping Multi-walled carbon nanotube ORR |
| 基金项目:国家自然科学基金项目（青年基金项目）;国家自然科学基金项目（面上项目，重点项目，重大项目） |
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| 中文摘要: |
| 本文采用多巴胺的自氧化聚合在多壁碳纳米管表面进行聚合沉积修饰，经热处理可得到氮掺杂的碳纳米管催化剂，通过调整沉积次数可控制表面聚多巴胺C-N膜的厚度，从而调控N的掺杂量。研究沉积次数对多壁碳纳米管催化剂表面形貌、化学组成及原子结合形态的影响，并考察N掺杂的多壁碳纳米管催化剂的氧还原反应活性。在此基础上，用多巴胺络合Mn、Fe离子进行共同聚合沉积，热处理后得到Mn（Fe）、N共同掺杂的多壁碳纳米管催化剂，对催化剂进行了多种测试和电化学表征。循环伏安和线性扫描的电化学表征表明，N掺杂可有效提高催化剂的氧还原反应（ORR）活性， C-N膜的厚度会影响催化剂性能，Mn(Fe)-N@MWCNTs催化剂的氧还原活性高于只有N掺杂的催化剂，两种催化剂氧还原反应均为4电子反应路径，可直接将氧气还原成H2O，且Fe-N@MWCNTs催化剂表现出较好的抗甲醇能力。SEM照片可以看到聚多巴胺在碳纳米管表面形成C-N膜；Raman分析表明聚多巴胺沉积后提高了催化剂表面的无序性，缺陷增多；XPS表征显示过渡金属的掺杂改变了CNx的结合状态。 |
| 英文摘要: |
| In this paper, polydopamine was deposited on the surface of multi-walled carbon nanotube through self-polymerization of dopamine, and then N-doped carbon nanotube was obtained pyrolysis. The influence of deposition time on the surface morphology,chemical composition and atomic bonding mode was studied, and the catalytic activity of N-doped carbon nanotube for oxygen reduction reaction was investigated. On this basis, dopamine complexing Mn or Fe ion codeposited on the carbon nanotube, and Mn (Fe), Ndoped carbon nanotube was obtained by pyrolysis. Cyclic voltammograms and linear sweep voltammetry showed that doped N can effectively improve the catalyst activity for oxygen reduction reaction, and the catalytic activity was further improved after Fe, N doped. The oxygen reduction reaction on all the catalyst exhibited 4 electron reaction pathway. And Fe-N@MWCNTs contains good methanol-tolerant property. SEM photos showed obviously that polydopamine nanofilm was formed on the surface of carbon nanotube; Raman spectra indicated that the disorder and defects of catalyst increased, compared with carbon nanotube. XPS result showed that the combination of the transition metal changed the CNx bonding mode. |
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