Hydrothermal synthesis of highly nitrogen-doped few-layer graphene via solid–gas reaction

Hydrothermal synthesis of highly nitrogen-doped few-layer graphene via solid–gas reaction
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固-气反应水热合成高氮掺杂少层石墨烯

DOI:
10.1016/j.materresbull.2014.09.088
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发表时间:
2015
影响因子:
5.4
通讯作者:
Caihao Hong
Caihao Hong
中科院分区:
材料科学2区
文献类型:
--
作者:
Xianqing Liang;Jun Zhong;Yalin Shi;Jin Guo;Guolong Huang;Yidong Zhao;Caihao Hong

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在自行设计的水热体系中,利用氧化石墨烯(GO)与氨气的固气反应制备了高掺杂浓度的掺氮(N)石墨烯薄片。用透射电子显微镜、原子力显微镜、X射线衍射仪、X射线光电子能谱、X射线光电子能谱和拉曼光谱对N掺杂石墨烯的形貌、表面化学和电子结构进行了研究。水热处理后,可将高达13.22%的氮引入皱缩的几层石墨烯薄片中。XPS和XANES分析表明,GO中的氧官能团与氨蒸气反应生成水热处理GO(HTGO)中的酰胺和胺物种。随后的热退火导致石墨烯中的氮键构型随退火温度的升高而逐渐从胺N转变为吡啶和石墨质N。本研究为大规模制备N掺杂石墨烯材料提供了一种简单、经济、环保的方法,具有潜在的应用前景。
Nitrogen-doped (N-doped) graphene sheets with high doping concentration were facilely synthesized through solid–gas reaction of graphene oxide (GO) with ammonia vapor in a self-designed hydrothermal system. The morphology, surface chemistry and electronic structure of N-doped graphene sheets were investigated by TEM, AFM, XRD, XPS, XANES and Raman characterizations. Upon hydrothermal treatment, up to 13.22 at% of nitrogen could be introduced into the crumpled few-layer graphene sheets. Both XPS and XANES analysis reveal that the reaction between oxygen functional groups in GO and ammonia vapor produces amide and amine species in hydrothermally treated GO (HTGO). Subsequent thermal annealing of the resultant HTGO introduces a gradual transformation of nitrogen bonding configurations in graphene sheets from amine N to pyridinic and graphitic N with the increase of annealing temperature. This study provides a simple but cost-effective and eco-friendly method to prepare N-doped graphene materials in large-scale for potential applications.
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