低缺陷密度石墨烯与Co3O4复合材料的制备及电化学性能

doi:10.11896/cldb.19030268

材料导报

2019, Vol. 33

Issue (18): 3156-3160 https://doi.org/10.11896/cldb.19030268

第20届全国高技术陶瓷学术年会

低缺陷密度石墨烯与Co₃O₄复合材料的制备及电化学性能

王永亮¹, 王春锋¹, 马荣鑫¹, 韩志东^{1, 2}

1 哈尔滨理工大学材料科学与工程学院,哈尔滨 150040
2 哈尔滨理工大学工程电介质及其应用教育部重点实验室,哈尔滨 150040

Preparation and Electrochemical Property of Graphene/Co₃O₄ Composite

WANG Yongliang¹, WANG Chunfeng¹, MA Rongxin¹, HAN Zhidong^1,2

1 School of Materials Science and Engineering, Harbin University of Science and Technology, Harbin 150040
2 Key Laboratory of Engineering Dielectrics and Its Application, Ministry of Education, Harbin University of Science and Technology, Harbin 150040

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摘要 Co₃O₄/石墨烯复合材料以其较高的比电容和良好的稳定性成为研究的热点。该材料研究中大多采用含官能团较多及分散性较好的氧化石墨烯,然而氧化石墨烯的缺陷较多,将其用于制备复合材料会限制复合材料电化学性能的提高。此外,复合材料制备往往涉及将氢氧化钴/氧化石墨烯复合物热处理获得Co₃O₄/石墨烯复合材料的过程。本工作选用了机械剥离法制备低缺陷密度石墨烯纳米片(Graphene nanoplatelets, GNP),实现了石墨烯纳米片与钴离子均匀稳定的分散,进而采用一步法(无需煅烧)制备Co₃O₄/GNP复合材料,探讨了Co₃O₄/GNP复合材料的相关性能。
机械剥离法制备的GNP的碳原子层数约为5层,层间距为3.6 ,且拉曼光谱中I_D/I_G比值仅为0.07,表明机械剥离法制备的GNP比还原法制备的氧化石墨烯具有较低的缺陷密度。以H₂O₂为氧化剂,采用一步法制备了Co₃O₄/GNP复合材料。Co₃O₄纳米颗粒以方形为主,平均粒径约为12 nm,且均匀负载于GNP片层。电化学研究结果表明,当m(Co₃O₄):m(GNP)=8:1时,Co₃O₄/GNP复合材料具有最优的比电容值,达到了542 F·g^-1,内阻仅为1.57 Ω。复合材料的内阻与GNP的添加量成反比,当m(Co₃O₄):m(GNP)=3:1时,复合材料的内阻仅为0.89 Ω。
本工作创新性地实现了一步法制备Co₃O₄/GNP复合材料。机械剥离法制备石墨烯确保了GNP具有低缺陷密度,一步法确保了Co₃O₄纳米颗粒均匀负载于GNP表面。优化Co₃O₄和GNP配比,制得的复合材料的比电容可达542 F·g^-1。

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	王永亮
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	韩志东

关键词: 石墨烯四氧化三钴超级电容器电化学性能

Abstract: Co₃O₄/graphene composites have drawn more and more attentions, which was due to their high specific capacitance and good stability. However, reduced graphene oxide was commonly used for Co₃O₄/graphene composites, which was due to the groups on graphene sheets and its good dispersibility. The defects of reduced graphene oxide (RGO) limited the electrochemical properties of the composite. Moreover, heat treating of hydroxide/graphene oxide was commonly involved for synthesis of Co₃O₄/graphene composite. In this paper, low-defect density graphene nanoplatelets (GNP) were prepared by mechanical exfoliation, and a stable suspension of GNP and Co ions was obtained. The Co₃O₄/GNP composites were obtained by one-step method without further heat treatment. The thickness of the GNP sheets synthesized via mechanical exfoliation was about five layers and the layer spacing was 3.6 . The I_D/I_G ratio from the Raman spectrum was only 0.07, indicating that the GNP has lower defects density than that of RGO. Co₃O₄/GNP composites were prepared by one-step method using H₂O₂ as oxidant. The average particle size of square Co₃O₄ nanoparticles was about 12 nm. Electrochemical studies show that the specific capacitance of Co₃O₄/GNP composites reached 542 F·g^-1 when weight ratio of Co₃O₄ and GNP was 8:1, and the internal resistance was only 1.57 Ω. The internal resistance of the composite increased with the amount of GNP. When weight ratio of Co₃O₄ and GNP was 3:1, the internal resistance was only 0.89 Ω. This work realized one-step synthesis of Co₃O₄/graphene composites. The graphene synthesized via mechanical exfoliation has a low defect density, and the one-step method ensures uniformly distribution of Co₃O₄ nanoparticles on GNP surface. The specific capacitance of composites reached 542 F·g^-1.

Key words: graphene Co₃O₄ supercapacitor electrochemical property

出版日期: 2019-09-25 发布日期: 2019-07-31

ZTFLH:

TQ02

基金资助: 国家自然科学基金(51602084);黑龙江省高校青年创新人才项目(UNPYSCT-2017090);黑龙江省自然科学基金(YQ2019E030);黑龙江省普通高校基本科研业务费专项资金资助(LGYC2018JC032)

作者简介: 王永亮于2005年6月在哈尔滨工业大学无机非金属材料工程专业获得工学学士学位,于2011年6月在哈尔滨工业大学材料科学与工程专业获得工学博士学位,现为哈尔滨理工大学副教授。已发表学术论文20余篇,申请国家发明专利8项,其中授权5项。同时,入选黑龙江省高校青年创新人才。研究方向主要围绕石墨烯及其复合材料和有机/无机纳米复合材料,开展材料结构与性能调控研究,主持包括国家自然科学基金青年项目、中国博士后科学基金面上项目、黑龙江省高校青年创新人才项目、黑龙江省自然科学基金项目等。

引用本文:

王永亮, 王春锋, 马荣鑫, 韩志东. 低缺陷密度石墨烯与Co₃O₄复合材料的制备及电化学性能[J]. 材料导报, 2019, 33(18): 3156-3160.
WANG Yongliang, WANG Chunfeng, MA Rongxin, HAN Zhidong. Preparation and Electrochemical Property of Graphene/Co₃O₄ Composite. Materials Reports, 2019, 33(18): 3156-3160.

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http://www.mater-rep.com/CN/10.11896/cldb.19030268 或 http://www.mater-rep.com/CN/Y2019/V33/I18/3156

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