氮掺杂石墨烯的制备及其表面增强拉曼散射效应  

Preparation of Nitrogen-Doped Graphene Films for Surface-Enhanced Raman Scattering

作　　者：郑楠楠 岳玉琛 沈永涛[1] 冯奕钰[1] 封伟[1,2] ZHENG Nannan;YUE Yuchen;SHEN Yongtao;FENG Yiyu;FENG Wei(School of Materials Science and Engineering,Tianjin University,Tianjin 300072,China;Collaborative Innovation Center of Chemical Science and Engineering(Tianjin),Tianjin 300072,China)

机构地区：[1]天津大学材料科学与工程学院,天津300072 [2]天津化学化工协同创新中心,天津300072

出　　处：《功能高分子学报》2020年第3期262-268,共7页Journal of Functional Polymers

基　　金：国家重点基础研究发展(973)计划(2016YFA0202302);国家自然科学杰出青年基金(51425306);国家自然科学基金(51573125,51573147,51803151)。

摘　　要：为了提高氮掺杂石墨烯(NG)薄膜的氮掺杂浓度(氮原子质量分数)并控制掺氮类型,通过化学气相沉积法,采取气态源与固态源相结合的方式制备了高质量的单层NG薄膜。通过调控生长时间、三聚氰胺用量(碳/氮源)、制备温度等工艺参数,研究了NG薄膜的形貌、氮掺杂浓度、掺氮类型。结果表明:NG薄膜在生长过程中包括成核、生长、成膜等;适宜的制备温度(990℃)有利于氮原子掺入到碳碳平面内;高温(超过1000℃)不利于石墨氮的生成,而有助于吡咯氮的生长;氮掺杂浓度随三聚氰胺用量的增加先升后降,最大氮掺杂浓度可达6.98%;在一定范围内,增加三聚氰胺的用量有利于吡啶氮的生成;此外,与石墨烯相比,NG薄膜可以将罗丹明B分子的检出限降低至10-5 mol/L。Graphene is a zero-gap semiconductor with low work function and high leakage current which limit its applications.Doping of nitrogen is one of the ways to tailor the properties of graphene.However,there remain some defects,such as the low nitrogen content and poor controllability.In order to enhance the content of nitrogen and control the bonding characters to embed nitrogen atoms inside the carbon lattice,solid-state sources(melamine)and gas-state sources(methane)were used to prepare nitrogen doped graphene(NG)films.The preparation time,the dosage of melamine and temperature were set as tunable parameters.The morphology of NG,the content of nitrogen(mass fraction of nitrogen atoms)and the bonding characters for the embedding of N atoms were studied.The results indicated that the preparation process of NG films was involved with nucleation,growth and aggregation.Proper temperature(990℃)was conductive for the improvement of the content of nitrogen.Pyrrolic N was produced at high temperature(>1000℃),while graphitic N was on the opposite.With increasing the dosage of melamine,the content of nitrogen was increased and then decreased with the maximum value of 6.98%.The content of Pyridinic N will be elevated with increasing the amount of melamine.Compared with graphene,NG films were capable of detecting the Raman signals from Rhodamine B molecules even at the concentration as low as 10-5 mol/L.

关 键 词：化学气相沉积法 氮掺杂石墨烯 表面增强拉曼散射 

分 类 号：TQ126.2[化学工程—无机化工]