Fe-N-C氧还原电催化剂中FeN_(4)位点微观环境的调节

作     者：王青 陆瑞虎 杨予琪 李玄泽 陈广波 尚露 彭力山 Dongxiao Sun-Waterhouse Bruce C.C.Cowie 孟祥敏 赵焱 张铁锐 Geoffrey I.N.Waterhouse Qing Wang;Ruihu Lu;Yuqi Yang;Xuanze Li;Guangbo Chen;Lu Shang;Lishan Peng;Dongxiao Sun-Waterhouse;Bruce C.C.Cowie;Xiangmin Meng;Yan Zhao;Tierui Zhang;Geoffrey I.N.Waterhouse

作者机构：School of Chemical SciencesThe University of AucklandAuckland 1142New Zealand State Key Laboratory of Silicate Materials for ArchitecturesInternational School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China iHuman InstituteShanghaiTech UniversityShanghai 201210China Key Laboratory of Photochemical Conversion and Optoelectronic MaterialsTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China Australian Synchrotron800 Blackburn Rd.ClaytonVictoria 3168Australia 

出 版 物：《Science Bulletin》 (科学通报（英文版）)

年 卷 期：2022年第67卷第12期

页      面：1264-1273,M0004页

核心收录：

学科分类：0808[工学-电气工程] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：supported by a James Cook Research Fellowship,administered by the Royal Society Te Apārangi funding support from Greg and Kathryn Trounson,the Energy Education Trust of New Zealand,the Mac Diarmid Institute for Advanced Materials and Nanotechnology,the National Key Projects for Fundamental Research and Development of China(2017YFA0206904 and 2017YFA0206900) the National Natural Science Foundation of China(51825205 and 21871279) the Beijing Natural Science Foundation(2191002) 

主　　题：Fe-N-C Microenvironment Optimized FeN_4 site Oxygen reduction reaction Zinc-air battery 

摘      要：Fe-N-C电催化剂,即FeN_(4)单原子位点负载于氮掺杂的碳载体上,是一种优良的氧还原催化剂,有望取代贵金属铂催化剂,应用于金属空气电池和燃料电池.目前,提高Fe-N-C材料氧还原性能的策略包括:(1)提高铁单原子活性位点的数目;(2)调节铁单原子中心与含氧中间体的吸附能,从而提高本征活性.该工作报道了一种简单NaCl熔盐煅烧Fe掺杂金属有机配合物前驱体(Fe-ZIF)的方法,可有效提高煅烧产物Fe-N-C催化剂中FeN_(4)单原子位点数量和本征活性.原位透射电子显微镜(TEM)实验结果表明:在高温煅烧过程中,NaCl蒸发后沉积附着在Fe-ZIF颗粒表面,加速Fe-ZIF中配体的分解和锌中心的挥发,从而使煅烧产物中碳载体呈多孔结构,并改变Fe单原子位点的配位环境.X射线吸收谱进一步表明,该Fe-N-C催化剂中Fe单原子位点的Fe-N键变长,Fe的氧化态降低,从而有利于氧还原反应中间体的脱附.因此,针对碱性氧还原反应过程,该催化剂表现出比商业化铂碳催化剂更优异的性能,并可作为锌空气电池阴极催化剂,用于手机充电.