WO2019119459A1 - 一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法 - Google Patents

一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法 Download PDF

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WO2019119459A1
WO2019119459A1 PCT/CN2017/118139 CN2017118139W WO2019119459A1 WO 2019119459 A1 WO2019119459 A1 WO 2019119459A1 CN 2017118139 W CN2017118139 W CN 2017118139W WO 2019119459 A1 WO2019119459 A1 WO 2019119459A1
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diamino
graphene
azofurazan
nitrogen
daaf
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PCT/CN2017/118139
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French (fr)
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卓海涛
陈少军
朱佳平
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深圳大学
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/15—Nano-sized carbon materials
    • C01B32/182—Graphene
    • C01B32/194—After-treatment

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  • the invention belongs to the technical field of material preparation, and in particular relates to a preparation method of a nitrogen-doped graphene material based on diamino azofurazan.
  • Graphene (G) is a two-dimensional honeycomb lattice material formed by the close combination of planar single-layer carbon atoms. It has a thickness of about 0.35 nm and is the world's thinnest two-dimensional material.
  • Graphene electrons pass through without any resistance, generate less heat, and have high electrical conductivity. They are the most excellent materials with known conductivity and have unique properties, such as tensile strength up to 130 GPa and carrier mobility up to 15000-25000 cm 2 /Vs (square centimeters per volt second), can exceed 10 times of silicon wafer; thermal conductivity can reach 5000 W/mK (watt per millimeter thermal conductivity), which is 3 times that of diamond; it also has room temperature Special properties such as quantum Hall effect and room temperature ferromagnetism.
  • graphene has no band gap, its electrical conductivity cannot be controlled like a conventional semiconductor, and its surface is smooth and inert, which is not conducive to recombination with other materials.
  • the above disadvantages limit the application of graphene.
  • the invention provides a preparation method of a nitrogen-doped graphene material based on diamino azofurazane, which aims to solve the problem that the graphene material is not easily compounded with other materials, resulting in limited application.
  • the invention provides a method for preparing a nitrogen-doped graphene material based on diamino azofurazan, comprising:
  • the graphene is dispersed in water, added with diamino azofurazene solution, heated at 50-70 ° C for 30-60 min, cooled to 20-40 ° C, and dried to obtain graphene-coated diamino azofurazene eutectic.
  • the mass ratio of graphene to diamino azofurazan in the diamino azofusan solution is 1:1 ⁇ 10;
  • the diamino azofusan eutectic is ground into a powder and heated at 500-800 ° C for 3 to 5 hours to obtain a nitrogen-doped graphene material.
  • the method for preparing a nitrogen-doped graphene material utilizes diamino azofurazan to react with graphene to obtain a graphene material having a high nitrogen doping content.
  • the graphene is uniformly coated on the surface of the diamino azofurazan crystal, and does not require the use of an auxiliary agent such as an adhesive, and completely maintains the surface properties of the diamino azofurazan crystal.
  • FIG. 1 is a schematic flow chart of a method for preparing a nitrogen-doped graphene material based on diamino azofurazan according to an embodiment of the present invention
  • Example 2 is a scanning electron microscope test chart of the nitrogen-doped graphene material prepared in Example 1 of the present invention
  • Example 3 is a X-ray photoelectron spectroscopy test chart of the nitrogen-doped graphene material prepared in Example 1 of the present invention
  • Example 4 is a X-ray photoelectron spectroscopy test chart of the nitrogen-doped graphene material N1s prepared in Example 1 of the present invention
  • Fig. 5 is a X-ray photoelectron spectroscopy test chart of C1s of the nitrogen-doped graphene material prepared in Example 1 of the present invention.
  • FIG. 1 is a schematic flow chart of a method for preparing a nitrogen-doped graphene material based on diamino azofurazane according to an embodiment of the present invention, wherein the method includes:
  • Step 1 Disperse graphene in water, add diamino azofurazan (DAAF) solution, heat at 50 ⁇ 70 °C for 30 ⁇ 60min, cool down to 20 ⁇ 40 °C, and dry to obtain graphene coated DAAF.
  • the mass ratio of graphene to DAAF is 1:1 ⁇ 10;
  • Step 2 The DAAF eutectic is ground into a powder and heated at 500 to 800 ° C for 3 to 5 hours to obtain a nitrogen-doped graphene material.
  • the preparation method of the nitrogen-doped graphene material provided by the invention utilizes DAAF to react with graphene to obtain a graphene material with a high nitrogen doping content.
  • the graphene is uniformly coated on the surface of the DAAF crystal, and does not require the use of an auxiliary agent such as an adhesive, and completely maintains the surface properties of the diamino azofurazan crystal.
  • the material opens the band gap, adjusts the conductivity type, changes the electronic structure, increases the free carrier density, improves the conductivity and stability, and introduces a nitrogen-containing functional group to increase the surface adsorption of the metal particles.
  • the active site enhances the interaction of metal particles with graphene and expands the application of graphene.
  • step one In step one,
  • the graphene is 1 to 3 layers, and the chip diameter is 0.2 to 100 ⁇ m.
  • the deionized water bath is used for graphene mixing.
  • the DAAF solution is a mixture of DAAF and ethanol, wherein the concentration of DAAF is 1 to 5 mg/mL.
  • the mass ratio of graphene to deionized water is 1:20 ⁇ 30.
  • the DAAF solution is a mixture of DAAF and ethanol, wherein the concentration of DAAF is 1 to 5 mg/mL.
  • the concentration of the DAAF solution is 3 mg/L.
  • the mass ratio of graphene to DAAF in the DAAF solution is 1:1 to 10, preferably 1:4 to 8, more preferably 1:8.
  • step two In step two,
  • the DAAF eutectic has a heating temperature of 600 ° C and a heating time of 4 h.
  • the DAAF eutectic was ground into a powder, heated in a tube furnace to 500 ° C, and kept for 3 h to obtain a nitrogen-doped graphene material having a nitrogen content of 5.16%.
  • the DAAF eutectic was ground into a powder, heated in a tube furnace to 800 ° C, and kept for 5 h to obtain a nitrogen-doped graphene material having a nitrogen content of 4.29%.
  • FIG. 2 shows an SEM test chart of the nitrogen-doped graphene material obtained in Example 1. It can be seen from Fig. 2 that the graphene is uniformly coated on the surface of the DAAF crystal, and the surface properties of the diamino azofurazan crystal are completely maintained without using an auxiliary agent such as an adhesive.
  • X-ray photoelectron spectroscopy (XPS) tests were performed on the nitrogen-doped graphene material and the nitrogen-doped graphene material prepared in Example 1. As shown in Fig. 3, it can be seen from Fig. 3 that the binding energy shows a sharp peak at 398-403 eV, which indicates that DAAF can effectively combine with graphene as a nitrogen source to obtain nitrogen-doped graphene.
  • XPS X-ray photoelectron spectroscopy
  • XPS analysis was performed on the N1s of the nitrogen-doped graphene. As shown in Fig. 4, pyridine type N, pyrrole type N, graphite type N, and pyridine N oxide appeared at 398.4, 404.1, 401.2, and 402.4 eV, respectively. .

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  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Nanotechnology (AREA)
  • Inorganic Chemistry (AREA)
  • Carbon And Carbon Compounds (AREA)

Abstract

一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法，涉及材料制备技术领域。其中，该方法包括：将石墨烯分散于水中，加入二氨基偶氮呋咱乙醇溶液，在50～70℃下加热30～60min，降温至20～40℃，干燥，得到石墨烯包覆的二氨基偶氮呋咱共晶物，其中，石墨烯与二氨基偶氮呋咱溶液中的二氨基偶氮呋咱的质量比为1∶1～10，将二氨基偶氮呋咱共晶物研磨成粉末，在500～800℃下加热3～5h，得到氮掺杂石墨烯材料。利用二氨基偶氮呋咱与石墨烯进行反应，得到氮掺杂含量较高的石墨烯材料。该材料中石墨烯均匀包覆在DAAF晶体的表面，不需要使用胶黏剂等助剂，完整的保持了二氨基偶氮呋咱晶体的表面性能。

Description

一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法
本发明属于材料制备技术领域，尤其涉及一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法。
石墨烯（G）是平面单层碳原子紧密结合在一起形成的二维蜂窝晶格材料，厚度为0.35 nm 左右，是世界上最薄的二维材料。
石墨烯的电子穿过没有任何阻力，产生的热量少、导电效率高，是已知导电性能最优异的材料，具有独特的性能，例如，拉伸强度可达130GPa；载流子迁移率可达15000-25000 cm2/Vs（平方厘米每伏秒），可超过硅片的10 倍；热导率可达5000 W/mK（瓦每毫导热系数），是金刚石的3倍；它还具有室温量子霍尔效应及室温铁磁性等特殊性质。
但是，石墨烯没有能带隙，其电导性不能像传统的半导体一样被控制，而且它表面光滑呈惰性，不利于与其它材料复合。以上缺点限制了石墨烯的应用。
发明内容
本发明提供一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法，旨在解决石墨烯材料不容易与其它材料复合，导致应用受限制的问题。
本发明提供的一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法，包括：
将石墨烯分散于水中，加入二氨基偶氮呋咱溶液，在50~70℃下加热30~60min，降温至20~40℃，干燥，得到石墨烯包覆的二氨基偶氮呋咱共晶物；其中，石墨烯与二氨基偶氮呋咱溶液中的二氨基偶氮呋咱的质量比为1:1~10；
将二氨基偶氮呋咱共晶物研磨成粉末，在500~800℃下加热3~5h，得到氮掺杂石墨烯材料。
本发明提供的氮掺杂石墨烯材料的制备方法，利用二氨基偶氮呋咱与石墨烯进行反应，得到氮掺杂含量较高的石墨烯材料。该材料中石墨烯均匀包覆在二氨基偶氮呋咱晶体的表面，不需要使用胶黏剂等助剂，完整的保持了二氨基偶氮呋咱晶体的表面性能。
附图说明
为了更清楚地说明本发明实施例或现有技术中的技术方案，下面将对实施例或现有技术描述中所需要使用的附图作简单地介绍，显而易见地，下面描述中的附图仅仅是本发明的一些实施例。
图1是本发明实施例提供的一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法的流程示意图；
图2是本发明实施例1制备得到的氮掺杂石墨烯材料的扫描电镜测试图；
图3是本发明实施例1制备得到的氮掺杂石墨烯材料的X射线光电子能谱测试图；
图4是本发明实施例1制备得到的氮掺杂石墨烯材料N1s的X射线光电子能谱测试图；
图5是本发明实施例1制备得到的氮掺杂石墨烯材料的C1s的X射线光电子能谱测试图。
具体实施方式
为使得本发明的发明目的、特征、优点能够更加的明显和易懂，下面将结合本发明实施例中的附图，对本发明实施例中的技术方案进行清楚、完整地描述，显然，所描述的实施例仅仅是本发明一部分实施例，而非全部实施例。基于本发明中的实施例，本领域技术人员在没有做出创造性劳动前提下所获得的所有其他实施例，都属于本发明保护的范围。
请参照图1，图1为本发明实施例提供一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法的流程示意图，其中，该方法包括：
步骤一、将石墨烯分散于水中，加入二氨基偶氮呋咱（DAAF）溶液，在50~70℃下加热30~60min，降温至20~40℃，干燥，得到石墨烯包覆的DAAF共晶物；
其中，石墨烯与DAAF的质量比为1:1~10；
步骤二、将DAAF共晶物研磨成粉末，在500~800℃下加热3~5h，得到氮掺杂石墨烯材料。
本发明提供的氮掺杂石墨烯材料的制备方法，利用DAAF与石墨烯进行反应，得到氮掺杂含量较高的石墨烯材料。该材料中石墨烯均匀包覆在DAAF晶体的表面，不需要使用胶黏剂等助剂，完整的保持了二氨基偶氮呋咱晶体的表面性能。进一步地，该材料打开了能带隙，调整了导电类型，改变了电子结构；提高了自由载流子密度，提高了导电性能和稳定性；引入含氮的官能团，增加了表面吸附金属粒子的活性位，增强了金属粒子与石墨烯的相互作用，扩大了石墨烯的应用。
步骤一中，
具体地，石墨烯为１~３层，且片径为0.2~100 μm。选用去离子水浴石墨烯混合。DAAF溶液为DAAF与乙醇的混合液，其中，DAAF的浓度为1~5mg/mL。
进一步地，将石墨烯分散于水中后，利用磁力搅拌器搅拌30~90min，并置于超声分散器中，超声抖动30~60min。其中，石墨烯与去离子水的质量比为1:20~30。
具体地，DAAF溶液为DAAF与乙醇的混合液，其中，DAAF的浓度为1~5mg/mL。优选地，DAAF溶液的浓度为3mg/L。其中，石墨烯与DAAF溶液中的DAAF的质量比为1:1~10，优选为1:4~8，更优选为1:8。
步骤二中，
优选地，DAAF共晶物的加热温度为600℃，加热时间为4h。
实施例1
将0.1 g片径为0.2μm的石墨烯加入25 ml去离子水中，在600 r/min转速下磁力搅拌60 分钟，然后将置于超声分散仪中，超声60 分钟，得到4 mg/ml的石墨烯溶液。
将0.8 g DAAF融入25ml乙醇中，加入上述石墨烯溶液，在50℃下加热30 min，降温至20℃，干燥48h，得到石墨烯包覆的DAAF共晶物。
将DAAF共晶物研磨成粉末，置于管式炉中加热至500℃，保温3h，得到含氮量为5.16%氮掺杂石墨烯材料。
实施例2
将0.1 g片径为100μm的石墨烯加入25 ml去离子水中，在600 r/min转速下磁力搅拌60 分钟，然后将置于超声分散仪中，超声30 分钟，得到4 mg/ml的石墨烯溶液。
将0.4g DAAF融入25ml乙醇中，加入上述石墨烯溶液，在70℃下加热60 min，降温至40℃，干燥48h，得到石墨烯包覆的DAAF共晶物。
将DAAF共晶物研磨成粉末，置于管式炉中加热至800℃，保温5h，得到含氮量为4.29%氮掺杂石墨烯材料。
对实施例1制得的氮掺杂石墨烯材料进行SEM（扫描电镜）测试，如图2所示，图2示出了实施例1制得的氮掺杂石墨烯材料的SEM测试图。由图2可知该材料中石墨烯均匀包覆在DAAF晶体的表面，不需要使用胶黏剂等助剂，完整的保持了二氨基偶氮呋咱晶体的表面性能。
对实施例1制得的氮掺杂石墨烯材料和未掺杂氮的石墨烯材料进行X射线光电子能谱（XPS）测试。如图3所示，由图3可以看出，结合能在398-403 eV出现一尖峰，可以说明，DAAF作为氮源能够有效的与石墨烯结合，得到氮掺杂石墨烯。
进一步地，对氮掺杂石墨烯的N1s处进行 XPS分析，如图4所示，在398.4、400.1、401.2和402.4 eV分别出现了吡啶型N、吡咯型N、石墨型N以及吡啶N氧化物。
进一步地，对氮掺杂石墨烯的C1s处进行 XPS分析，如图4所示，在284.4、285.2、286.4和289.2 eV分别出现了C–C、C–N、C–O以及C=O(C=N)键，说明DAAF作为氮源制备氮掺杂石墨烯对石墨烯的机构产生了作用。
综合以上测试，说明DAAF作为氮源掺杂石墨烯是可行的。
以上所述仅为本发明的较佳实施例而已，并不用以限制本发明，凡在本发明的精神和原则之内所作的任何修改、等同替换和改进等，均应包含在本发明的保护范围之内。

Claims (7)

  1. 一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法，其特征在于，所述方法包括：
    将石墨烯分散于水中，加入二氨基偶氮呋咱乙醇溶液，在50~70℃下加热30~60min，降温至20~40℃，干燥，得到石墨烯包覆的二氨基偶氮呋咱共晶物；其中，石墨烯与二氨基偶氮呋咱溶液中的二氨基偶氮呋咱的质量比为1:1~10；
    将二氨基偶氮呋咱共晶物研磨成粉末，在500~800℃下加热3~5h，得到氮掺杂石墨烯材料。
  2. 根据权利要求1所述的方法，其特征在于，所示石墨烯的层数在１~３层，且片径为0.2~100 μm。
  3. 根据权利要求1所述的方法，其特征在于，所述石墨烯与二氨基偶氮呋咱的质量比为1:4~8。
  4. 根据权利要求1所述的方法，其特征在于，所述二氨基偶氮呋咱溶液为二氨基偶氮呋咱与乙醇的混合液，其中，二氨基偶氮呋咱的浓度为1~5mg/mL。
  5. 根据权利要求1所述的方法，其特征在于，所述二氨基偶氮呋咱共晶物的加热温度为600℃。
  6. 根据权利要求1所述的方法，其特征在于，所述二氨基偶氮呋咱共晶物的加热时间为4h。
  7. 根据权利要求1所述的方法，其特征在于，所述方法还包括：
    将所述石墨烯加入到去离子水中，搅拌30~90min，超声抖动30~60min，其中，所述石墨烯与所述去离子水的质量比为1:20~30。
PCT/CN2017/118139 2017-12-23 2017-12-23 一种基于二氨基偶氮呋咱的氮掺杂石墨烯材料的制备方法 WO2019119459A1 (zh)

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