氮掺杂泡沫碳电催化剂的制备及氧还原性能
Nitrogen-Doped Carbon Foam: Preparation and Oxygen Reduction Reaction Performance
作者单位E-mail
李婧晗 江苏大学材料科学与工程学院, 镇江 212013  
宋亚乘 江苏大学材料科学与工程学院, 镇江 212013  
周亚洲 江苏大学材料科学与工程学院, 镇江 212013  
程晓农 江苏大学材料科学与工程学院, 镇江 212013  
杨娟 江苏大学材料科学与工程学院, 镇江 212013 yangjuan6347@ujs.edu.cn 
摘要: 利用水解乙烯基咪唑鎓硝酸盐([Hvim]NO3)作为发泡剂和一次氮源,在碳化过程中实现材料自发泡。创造性地引入二次氮源三聚氰胺(C3H6N6),通过调控一次、二次氮源比例和碳化温度,制备得到氮掺杂泡沫碳材料(HxMy-T,其中xy为一次和二次氮源的质量比,T对应不同的碳化温度)。该方法提升了催化剂的氮掺杂含量,构建了更多有利于氧还原反应(ORR)的活性氮位点。电镜结果显示,催化剂H1M1-1000呈现出典型的泡沫碳孔洞结构和丰富的层状褶皱结构;X射线光电子能谱测试结果表明,该样品具有较高的活性氮含量(原子分数6.77%),吡啶氮和石墨氮的原子分数分别高达22.23%和55.59%;电化学测试结果表明,该样品在碱性环境中的半波电位为0.834 V (vs RHE),与商业Pt/C相当,且具有优于商业Pt/C的抗甲醇性能和稳定性。
关键词: 氮掺杂泡沫碳  三聚氰胺  氧还原反应  燃料电池
基金项目: 国家自然科学基金(No.51672112,51702129)资助。
Abstract: Nitrogen-doped carbon foam material was prepared by using hydrolyzed vinyl imidazolium nitrate ([Hvim] NO3) as a blowing agent and a primary nitrogen source to realize self-foaming of the material during the carbonization process. The secondary nitrogen source melamine (C3H6N6) was innovatively introduced. The nitrogen doped carbon foam material (HxMy-T, where x:y was the mass ratio of the primary and secondary nitrogen source, T corresponded the carbonization temperature) were obtained. This method increased the nitrogen doping content of the catalyst and constructed more active nitrogen sites which improved the oxygen reduction reaction (ORR) activity. Electron microscope images showed that the H1M1-1000 with typical foam -like pore structure and abundant layered fold. The X-ray photoelectron spectroscopy indicated that the H1M1-1000 possessed a high N atomic fraction of 6.77%, and the content of pyridinic-N and graphitic-N were up to 22.23% and 55.59% (atomic fraction), respectively. For electrochemistry test, the half wave potential of H1M1 1000 in alkaline medium was 0.834 V (vs RHE), which was comparable to that of commercial Pt/C. In addition, the catalyst had superior long-time stability and methanol resistance than that of commercial Pt/C.
Keywords: nitrogen-doped carbon foam  melamine  oxygen reduction reaction  fuel cells
投稿时间:2020-09-15 修订日期:2020-12-02
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李婧晗,宋亚乘,周亚洲,程晓农,杨娟.氮掺杂泡沫碳电催化剂的制备及氧还原性能[J].无机化学学报,2021,37(3):457-464.
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