摘要
能源问题是事关国家发展和安全的重大问题,氧还原反应作为燃料电池阴极半反应近年来成为能源和电催化领域的研究热点之一。通过利用2,9-二甲基-1,10-邻菲啰啉与钴离子的配位形成配合物,将该配合物与炭黑混合均匀,经过中温热解和浓硝酸氧化后得到钴、氮表面修饰的碳负载纳米催化剂Co-N/C。实验首先利用旋转圆盘电极和旋转环盘电极(RRDE)考察了催化剂在不同pH值下的电催化氧还原性能。电化学测试结果表明,在碱性条件下,该催化剂具有与商业Pt/C相近的4电子氧还原催化性能。随后,通过SEM、TEM、XPS、XRD和FT-IR等设备对催化剂进行表征,以揭示Co-N/C催化剂4电子氧还原催化活性增强的来源。运用功能化修饰策略调控碳材料表面的催化活性位点和碳的电子结构,克服了本征碳材料催化活性不高的缺陷,为设计新型非贵金属氧还原反应催化剂提供了一种新的思路。
The energy issue is a significant concern for national development and security.In recent years,oxygen reduction reaction,as a cathode half reaction of fuel cell,has become one of the research hotspots in the field of energy and electrocatalysis.In this study,2,9-dimethyl-1,10-phenanthroline were used to coordinate with cobalt ions to form a complex.The complex was uniformly mixed with carbon black.After medium temperature pyrolysis and concentrated nitric acid oxidation,cobalt and nitrogen surface-modified carbon supported nanocatalyst Co-N/C was obtained.Firstly,the electrocatalytic oxygen reduction performance of the catalyst under different pH values was investigated by rotating disk electrode and rotating ring disk electrode.The electrochemical test results indicated that the catalyst exhibits four-electron oxygen reduction catalytic performance similar to commercial Pt/C under alkaline conditions.Subsequently,the catalyst was characterized using SEM,TEM,XPS,XRD and FT-IR to reveal the origin of the enhanced four-electron oxygen reduction catalytic activity.In this work,functional modification strategies were used to regulate the catalytic active sites and the electronic structure of surface carbon atoms,which overcame the drawback of low catalytic activity of intrinsic carbon materials.It provides a new perspective for the design of novel non-precious metal oxygen reduction catalysts.
作者
胡鹏
张琪婧
路肖栋
左自豪
HU Peng;ZHANG Qi-jing;LU Xiao-dong;ZUO Zi-hao(College of Chemistry and Pharmaceutical Engineering,Huanghuai University,Zhumadian 463000,China;College of Science,Shenyang University of Chemical Technology,Shenyang 110142,China)
出处
《化学试剂》
CAS
2024年第2期74-79,共6页
Chemical Reagents
基金
河南省科技发展计划项目(222102320377)。
关键词
Co-N/C
热解
表面调控
电催化剂
氧还原反应
Co-N/C
pyrolysis
surface regulation
electrocatalyst
oxygen reduction reaction
