镍氮掺杂石墨炔用作高效氧还原电催化剂  

Nickel-Nitrogen-Doped Graphdiyne as an Efficient Catalyst for Oxygen Reduction

作　　者：惠连成 庄鉴行 肖顺 李美平 靳梦圆 吕青 HUI Lian-Cheng;ZHUANG Jian-Xing;XIAO Shun;LI Mei-Ping;JIN Meng-Yuan;LYU Qing(Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion,Science Center for Material Creation and Energy Conversion,School of Chemistry and Chemical Engineering,Shandong University,Jinan 250100,China)

机构地区：[1]山东大学化学与化工学院,物质创制与能量转换科学研究中心,山东省物质创制与能量转换科学重点实验室,济南250100

出　　处：《应用化学》2023年第8期1205-1213,共9页Chinese Journal of Applied Chemistry

基　　金：国家自然科学基金(No.22172090);山东省自然科学基金(No.ZR2021MB015);山东大学青年学者未来计划;电分析化学国家重点实验室开放课题(No.SKLEAC202202)资助

摘　　要：氧还原反应是燃料电池中至关重要的一环。常规的氧还原反应催化剂是贵金属铂,但鉴于铂的高成本,研究者希望寻找一种低成本的替代催化剂,它更便宜并且具有相当于铂的催化效果。在前期研究中,已经对铁氮共掺杂石墨炔和钴氮共掺杂石墨炔进行了研究,它们均表现出了高效的氧还原反应活性,而与之具有相似电子结构的金属镍尚未研究。因此,此工作以氢取代石墨炔为基底,设计并合成了多种镍氮掺杂的石墨炔电催化剂,并进行了氧还原电化学测试,其中,镍质量分数2%并加入三聚氰胺进行烧制的镍氮掺杂石墨炔催化剂表现出最佳的氧还原电催化性能。对催化剂进行了一系列的物理表征:X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)和扫描电子显微镜(SEM),进一步分析了其结构和形貌。从物理表征及电化学测试结果可以看出,氮原子是构建催化活性位点的关键,而镍原子在提高催化剂性能方面起着至关重要的作用,氮和镍的协同作用使得镍氮掺杂石墨炔催化剂表现出优异的催化性能,这使其具有良好的应用前景。Oxygen reduction reaction is a crucial process for fuel cells.Conventional oxygen reduction catalysts are the precious metal platinum,but given the high cost of platinum,researchers want to find a low-cost alternative catalyst that is cheaper and has the equivalent catalytic activity to platinum.In previous studies,iron-nitrogen-doped graphdiyne and cobalt-nitrogen-doped graphdiyne have been studied,and they all show efficient oxygen reduction reaction activity,while nickel,with similar electronic structure with iron and cobalt,has not been studied.Therefore,in this work we design and synthesize various nickel-nitrogen-doped graphdiyne electrocatalysts using hydrogen as a substitute for graphiyne,and conduct redox electrochemical tests.The nickel-nitrogen-doped graphdiyne catalyst containing 2%nickel and melamine shows the best electrocatalytic performance for oxygen reduction.We conduct a series of physical characterizations for the catalysts:X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),transmission electron microscope(TEM),scanning electron microscope(SEM)to further analyze their structure and morphology.It can be seen from the physical characterization and electrochemical tests that nitrogen atoms are the key to construct the catalytic active site,and nickel atoms play a vital role in improving the performance of the catalysts.With the synergistic effect of nitrogen and nickel,the nickel nitrogen-doped graphdiyne catalyst shows excellent catalytic performance,which makes it have a good application prospect.

关 键 词：镍氮掺杂石墨炔 氧还原反应 电催化 协同作用 

分 类 号：O646[理学—物理化学]