CN109999870A - 一种碳化硅/石墨烯纳米片状复合材料及其制备方法 - Google Patents
一种碳化硅/石墨烯纳米片状复合材料及其制备方法 Download PDFInfo
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Abstract
本发明涉及一种碳化硅/石墨烯纳米片状复合材料制备方法,包括如下步骤:1)制备石墨烯纳米片和一氧化硅粉末混合分散液,所述混合分散液中石墨烯与氧化硅的摩尔比为(2‑1):(1‑2.5);2)对所述混合分散液进行干燥得到前驱体;3)将所述前驱体在真空度为0.03‑0.1MPa,温度为1000‑1250℃条件下煅烧,得到碳化硅/石墨烯纳米片粗产物;4)对所述粗产物进行除硅处理得到碳化硅/石墨烯纳米片。根据本发明的碳化硅/石墨烯纳米片复合材料制备方法,工艺简单、成本较低,易于工业化生产。
Description
技术领域
本发明涉及半导体复合材料领域,具体涉及一种碳化硅/石墨烯纳米片状复合材料及其制备方法。
背景技术
二维原子半导体材料一直备受关注,尤其是石墨烯,由于其具有优异的电学、光学和力学性质,如高载流子迁移率,较高吸光率等,被广泛应用在电子器件、光电器件等领域。近年来,由于石墨烯合成技术、材料表征方法的快速进步,及对高质量半导体材料和设备越来越高的需求,研究人员已经把目光从石墨烯材料本身,转移到研究不同的二维半导体复合材料及异质结构。碳化硅(SiC)是第三代半导体的核心材料之一,具有很多优异的性能,如高带隙、高强度、高导热性、高电导性,又由于其独特的光、电和优异的机械性能,使得碳化硅纳米材料在许多领域都有极为广泛及潜在的应用价值。因此,碳化硅/石墨烯纳米片状异质结构结合了众所周知的半导体的优势及石墨烯的独特优势,在光催化、光电器件等领域有潜在应用价值,是一种很有前途的复合材料。一般的碳化硅/石墨烯复合结构是通过SiC热分解[Berger C,Song Z,Li T,et al.Ultrathin Epitaxial Graphite:2DElectronGas Properties and a Route toward Graphene-based Nanoelectronics[J].J.phys.chem,2004,108(52):19912-19916.]、化学气相沉积(CVD)[Michon A,VeZian S,Ouerghi A,et al.Direct growth of few-layer graphene on 6H-SiC and 3C-SiC/Sivia propane chemical vapor deposition[J].Applied Physics Letters,2010,97(17):171909.]和分子束外延(MBE)[Razadocolambo I,Avila J,Chen C,et al.Probing theelectronic properties of graphene on C-face SiC down to single domains bynanoresolved photoelectron spectroscopies[J].Physical Review B,2015,92(3).]方法制备得到,这些方法因为生长温度高、设备昂贵、操作成本高和安全性等问题,仅适用于高价值应用,无法进行大规模工业化生产。基于此,有必要提供一种反应温度低、制备方法简单、成本低的碳化硅/石墨烯复合材料制备方法。
发明内容
本发明解决的技术问题是:提供一种碳化硅/石墨烯纳米片状复合材料制备方法,制备得到的碳化硅颗粒均匀分散于所述石墨烯表面,且工艺简单,成本低,易于工业化生产。
本发明提供的具体解决方案包括如下步骤:
1)制备石墨烯(GNS)纳米片和氧化硅(SiO)粉末混合分散液,所述混合分散液中石墨烯与一氧化硅摩尔比为(2-1):(1-2.5);
2)对所述混合分散液进行干燥得到前驱体;
3)将所述前驱体在真空度为0.03-0.1MPa,温度为1000-1250℃条件下煅烧,得到碳化硅/石墨烯纳米片粗产物。
4)对所述粗产物进行除硅处理得到碳化硅/石墨烯纳米片。
该制备过程中涉及到的化学反应为:
2C(s)+SiO(g)=SiC(s)+CO(g) 公式(1)
2SiO(g)=Si(s)+SiO2(s) 公式(2)
Si(s)+C(s)=SiC(s) 公式(3)
SiO2(s)+2C(s)=SiC(s)+CO2(g) 公式(4)
C(s)+CO2(g)=2CO(g) 公式(5)
SiO(g)+3CO(g)=SiC(s)+2CO2(g) 公式(6)
4CO(g)+SiO2(s)=SiC(s)+3CO2(g) 公式(7)
3C(s)+2SiO(g)=2SiC(s)+CO2(g) 公式(8)
其中反应(1)和(6)是生成SiC的主要反应,高温下SiO(s)升华形成SiO(g),与GNS表面碳反应(反应(1))生成SiC晶核,碳化硅在成核处生长得到碳化硅颗粒;由于高温下SiO自身会发生歧化反应(反应(2)),生成的Si(s)与SiO2(s)堆积在GNS表面和周围,且由于固相反应主要靠扩散进行,所以反应(3)和(4)只有极少部分进行;理论上反应(8)有可能发生,但从活化能考虑不可能成为主反应;虽然反应(6)无论是在热力学还是动力学都占有优势,但是为了使主反应(1)朝正反应方向进行,需要对反应的温度和压强进行控制。在实验过程中持续地抽真空,使得反应产生的混合气体(CO、CO2)能及时溢出,提高原位生成SiC反应的产率。温度越高,各种副反应例如(2)、(5)、(6)、(7)和(8)反应加剧,与SiC原位生成反应(1)竞争,得到的材料中含有较多的SiC杂质,而非石墨烯上原位生成碳化硅后得到的碳化硅/石墨烯复合材料。
采用上述方案的有益效果是:
(1)根据本发明的方法,在石墨烯纳米片上原位生成碳化硅颗粒,得到了碳化硅/石墨烯纳米片状复合材料,且制备得到的碳化硅颗粒均匀分散于所述石墨烯表面;
(2)制备碳化硅/石墨烯纳米片所需的原料易得,制备工艺简单,合成温度低,设备要求低,有望实现碳化硅/石墨烯纳米片的规模化生产。
进一步,步骤3)中前驱体的煅烧温度为1050-1200℃,升温速率为4-6℃/min,煅烧时间为1-24h。
反应温度低,则反应速率慢;反应温度高,升温速率快,一方面SiO气化速率快,气态SiO无法及时反应,大部分的反应气体会逸出,另一方面,温度过高,反应快,不利于原位生成碳化硅反应的充分实现(会有大量的一氧化硅参与反应(6)),此时会产生与其他许多文献报道的独立的SiC纳米线而非与所述石墨烯键连的碳化硅,即非碳化硅/石墨烯复合材料。在该条件下,得到的碳化硅/石墨烯复合材料中,SiC杂质少,碳化硅与石墨烯具有较好的复合效果,且碳化硅颗粒均匀分散于所述石墨烯表面。
进一步,步骤3)中前驱体煅烧的真空度为0.05MPa-0.08MPa。
在该条件下,得到的碳化硅/石墨烯复合材料纯度高,产率高。
进一步,步骤1)中的分散溶剂为N-甲基吡咯烷酮或N-N二甲基甲酰胺。
具体的,先将所述石墨烯纳米片充分分散于所述所述分散溶剂中,再加入一氧化硅粉末分散均匀。
由此,以N-甲基吡咯烷酮或N-N二甲基甲酰胺作为分散溶剂得到的混合分散液均匀稳定。
进一步,步骤1)中石墨烯与一氧化硅的摩尔比为(2-1):(1.5-2)。
由此,纳米薄片表面均匀生长了大量尺寸均一的2-10nm的SiC纳米颗粒。
进一步,步骤4)中除硅处理包括氢氟酸溶液浸泡洗涤或者碱溶液浸泡处理。
具体的,将粗产物在氢氟酸溶液或者碱溶液中浸泡洗涤可以除去未反应的硅及硅的氧化物,得到碳化硅/碳纳米管复合物。
优选的,所述碱溶液包括氢氧化钠、氧化钾的热水溶液。
优选的,所述氢氟酸溶液的质量分数为10%-40%,浸泡时间为2h-24h。
在该条件下,杂质硅及其氧化物的去除效果好。
本发明还提供了一种碳化硅/石墨烯纳米片状复合材料,按照如上所述的方法制备得到,且碳化硅颗粒均匀分散于所述石墨烯表面,SiC杂质少,碳化硅与石墨烯具有较好的复合效果。
本发明的附加方面和优点将在下面的描述中部分给出,部分将从下面的描述中变得明显,或通过本发明的实践了解到。
附图说明
图1是碳化硅/石墨烯纳米片制备流程图。
图2是本发明实施例1所制得的碳化硅/石墨烯纳米片XRD图谱。
图3是本发明实施例1所制得的碳化硅/石墨烯纳米片拉曼光谱。
图4是本发明实施例1所制得的碳化硅/石墨烯纳米片场发射扫描电镜照片。
图5是本发明实例1超声分散的石墨烯纳米片透射电子显微镜照片。
图6是本发明实施例1所制得的碳化硅/石墨烯纳米片透射电子显微镜照片。
具体实施方式
下面结合附图和实施例,对本发明的具体实施方式作进一步详细描述。以下实施例用于说明本发明,但不用来限制本发明的范围。
实施例1(请参阅图1):
(1)将一氧化硅在砂磨机中砂磨30min得到一氧化硅粉末,然后将石墨烯纳米片在NMP溶液中超声分散2h,将分散后的石墨烯纳米片与一氧化硅按照摩尔比为1:1在研钵中研磨混合30min,过滤掉滤液后在100℃烘箱中干燥得到前驱体。
(2)将前驱体在真空管式炉中进行煅烧,真空度为0.06MPa,煅烧温度为1150℃,煅烧时间为4h,得到粗产物;
(3)将粗产物在温度为60℃,质量分数为20%的HF溶液中进行浸泡除硅,浸泡时间为4h,过滤清洗后在100℃烘箱干燥得到最终产物。
对实施例1中的产物进行表征,图2为碳化硅/石墨烯纳米片的XRD图谱,图谱表明产物由SiC和石墨烯两种物相组成;图3为碳化硅/石墨烯纳米片的拉曼光谱,进一步证实了产物物相组成;图4所示为碳化硅/石墨烯纳米片的场发射扫描电镜照片,从照片中可以看出,制备出的碳化硅/石墨烯纳米复合材料为表面粗糙的片状结构;图5、6分别为石墨烯纳米片、碳化硅/石墨烯纳米片的TEM照片,可以看出在石墨烯纳米片表面生长了大量的SiC纳米颗粒。
实施例2:
(1)将一氧化硅在砂磨机中砂磨30min得到一氧化硅粉末,然后将石墨烯纳米片在NMP分散剂中超声分散2h,将分散后的石墨烯纳米片与一氧化硅按照摩尔比为2:1在研钵中研磨混合30min,过滤掉滤液后在100℃烘箱中干燥得到前驱体。
(2)将前驱体在真空管式炉中进行煅烧,真空度为0.03MPa,煅烧温度为1000℃,煅烧时间为24h,得到粗产物;
(3)将粗产物在温度为60℃,质量分数为10%的HF溶液中进行浸泡除硅,浸泡时间为24h,过滤清洗后在100℃烘箱干燥得到最终产物。
实施例3:
(1)将一氧化硅在砂磨机中砂磨30min,干燥后得到一氧化硅粉末,然后将石墨烯纳米片在NMP分散剂中超声分散2h,将分散后的石墨烯纳米片与一氧化硅按照摩尔比为1:2.5在研钵中研磨混合30min,过滤掉滤液后在100℃烘箱中干燥得到前驱体。
(2)将前驱体在真空管式炉中进行煅烧,真空度为0.1MPa,煅烧温度为1250℃,煅烧时间为1h,得到粗产物;
(3)将粗产物在温度为60℃,质量分数为40%的HF溶液中进行浸泡除硅,浸泡时间为2h,过滤清洗后在100℃烘箱干燥得到最终产物。
实施例4:
(1)将一氧化硅在砂磨机中砂磨30min,干燥后得到一氧化硅粉末,然后将石墨烯纳米片在NMP分散剂中超声分散2h,将分散后的石墨烯纳米片与一氧化硅按照摩尔比为1:2在研钵中研磨混合30min,过滤掉滤液后100℃烘箱中干燥得到前驱体。
(2)将前驱体在真空管式炉中进行煅烧,真空度为0.05MPa,煅烧温度为1150℃,煅烧时间为4h,得到粗产物;
(3)将粗产物在温度为60℃,质量分数为40%的HF溶液中进行浸泡除硅,浸泡时间为4h,过滤清洗后在100℃烘箱干燥得到最终产物。
实施例5:
(1)将一氧化硅在砂磨机中砂磨30min,干燥后得到一氧化硅粉末,然后将石墨烯纳米片在NMP分散剂中超声分散2h,将分散后的石墨烯纳米片与一氧化硅按照摩尔比为2:1在研钵中研磨混合30min,过滤掉滤液后在100℃烘箱中干燥得到前驱体。
(2)将前驱体在真空管式炉中进行煅烧,真空度为0.08MPa,煅烧温度为1200℃,煅烧时间为8h,得到粗产物;
(3)将粗产物在温度为60℃,质量分数为40%的HF溶液中进行浸泡除硅,浸泡时间为4h,过滤清洗后在100℃烘箱干燥得到最终产物。
实施例6
(1)将一氧化硅在砂磨机中砂磨30min得到一氧化硅粉末,然后将石墨烯纳米片在NMP分散剂中超声分散2h,将分散后的石墨烯纳米片与一氧化硅按照摩尔比为2:1.5在研钵中研磨混合30min,过滤掉滤液后在100℃烘箱中干燥得到前驱体。
(2)将前驱体在真空管式炉中进行煅烧,真空度为0.06MPa,煅烧温度为1100℃,煅烧时间为12h,得到粗产物;
(3)将粗产物在温度为60℃,质量分数为10%的HF溶液中进行浸泡除硅,浸泡时间为12h,过滤清洗后在100℃烘箱干燥得到最终产物。
对比例1:
与实施例1相似,不同之处在于,步骤(2)中的煅烧温度800℃。
对比例2:
与实施例1相似,不同之处在于,步骤(2)中的煅烧温度1400℃。
对比例3:
与实施例1相似,不同之处在于,步骤(2)中的煅烧温度1600℃.
对比例4:
与实施例1相似,不同之处在于,步骤(2)中真空度为0.005MPa。
对比例5:
与实施例1相似,不同之处在于,步骤(2)中真空度为0.01MPa。
对比例6:
与实施例1相似,不同之处在于,步骤(2)中真空度为0.02MPa。
光催化活性测试:
对实施例1以及对比例1-6得到的碳化硅/石墨烯纳米复合材料进行光催剂活性测试。
分别取相同重量的0.25g上述碳化硅/石墨烯纳米复合光催化剂均匀分散于100mL8mg/L的有机染料罗丹明B溶液中,在黑暗条件下搅拌1h,吸附平衡后在紫外光下进行光催化降解实验,每隔30min取一次样,对降解液中剩余罗丹明B的浓度进行检测,2h后,实施例1、对比例1、对比例2、对比例3、对比例4、对比例5以及对比例6中的催化剂对罗丹明B的降解率分别为95%、56%、80%、68%、72%和82%。由此可知,实施例1制备的碳化硅/石墨烯纳米复合材料中碳化硅和石墨烯具有最佳的复合效果,光催化活性最高。
尽管上面已经详细描述了本发明的实施例,本领域的普通技术人员可以理解:在不脱离本发明的原理和宗旨的情况下可以对这些实施例进行多种变化、修改、替换和变型,本发明的范围由权利要求及其等同物限定。
Claims (7)
1.一种碳化硅/石墨烯纳米片状复合材料制备方法,其特征在于,包括如下步骤:
1)制备石墨烯纳米片和一氧化硅粉末混合分散液,所述混合分散液中石墨烯与一氧化硅的摩尔比为(2-1):(1-2.5);
2)对所述混合分散液进行干燥得到前驱体;
3)将所述前驱体在真空度为0.03-0.1MPa,温度为1000-1250℃条件下煅烧,得到碳化硅/石墨烯纳米片粗产物;
4)对所述粗产物进行除硅处理得到碳化硅/石墨烯纳米片复合材料。
2.根据权利要求1所述的碳化硅/石墨烯纳米片状复合材料制备方法,其特征在于,步骤3)中前驱体的煅烧温度为1050-1200℃,升温速率为4-6℃/min,煅烧时间为1-24h。
3.根据权利要求1所述的碳化硅/石墨烯纳米片状复合材料制备方法,其特征在于,步骤3)中前驱体煅烧的真空度为0.05MPa-0.08MPa。
4.根据权利要求1所述的碳化硅/石墨烯纳米片状复合材料制备方法,其特征在于,步骤1)的混合分散液中的分散溶剂为N-甲基吡咯烷酮或N-N二甲基甲酰胺。
5.根据权利要求1所述的碳化硅/石墨烯纳米片状复合材料制备方法,其特征在于,步骤1)中石墨烯与一氧化硅的摩尔比为(2-1):(1.5-2)。
6.根据权利要求1-5任一所述的碳化硅/石墨烯纳米片状复合材料制备方法,其特征在于,步骤4)中除硅处理包括氢氟酸溶液浸泡洗涤或者碱溶液浸泡处理。
7.一种碳化硅/石墨烯纳米片状复合材料,其特征在于,由权利要求1-6任一所述的碳化硅/石墨烯纳米片状复合材料制备方法制备得到。
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