自蔓延高温合成功能化碳纳米材料及其性能研究

发布时间：2018-02-15 21:38

本文关键词： SHS 没食子酸功能化石墨烯 Fe/N共掺杂碳纳米盒子氧还原反应锌-空气电池　出处：《天津工业大学》2017年硕士论文　论文类型：学位论文

【摘要】：碳纳米材料由于具有良好的力学、电学及化学性能,使其在生物医学、环境和能源等领域都显示了巨大的应用前景。特别是对于具有高比表面积和高电导率的石墨烯及多孔生物质碳纳米材料更是研究的热点。本文以石墨和果糖为主要原料,设计合成了两种功能化的碳纳米材料,并对其性能进行了研究。其中包括水溶性石墨烯的制备以及导电性能研究;Fe/N共掺杂碳纳米盒子的制备及其ORR催化性能研究。具体内容包括:(1)用改性Hummers法制备GO,并用不同量没食子酸对其进行化学改性得到GOGA,发展了 SHS技术分别还原GO和GOGA制备石墨烯的方法。与传统制备方法相比,该方法具有工艺简单、环境友好等优点。并通过XRD、FI-IR、XPS、Raman、TEM和HRTEM等测试方法对rG0和rGOGA的结构进行表征。另外,通过Zeta电位、接触角测试和电导率测试对其水溶性和导电性进行表征。发现由于没食子酸的修复作用,不仅提高了石墨烯电导率(88900 S/m),还使其具有一定的水溶性。探索了石墨烯的改性和修复机理。(2)以生物质果糖为原料,采用SHS技术制备出3D多孔和高度石墨化的CNBs,其电导率为40700 S/m,高于传统方法制备的石墨烯和碳纳米管。然后将FeCl3和氨气作为氮源,以不同的温度煅烧制备出负载有Fe基纳米颗粒的Fe-N-CNBs。通过XRD表征发现Fe基纳米颗粒主要由Fe,Fe3C和Fe2N纳米晶体组成。另外通过电化学工作站和锌-空气电池装置对其进行性能测试,得出Fe-N-CNBs-600催化剂的起始电位(1.03 V vs.RHE)和半波电位(0.875 V vs.RHE),优于商业化 Pt/C(1.01 和 0.745 Vvs.RHE)。而且,Fe-N-CNBs-600 催化剂在碱性条件下还具有较好的抗甲醇性和稳定性。
[Abstract]:Because of its excellent mechanical, electrical and chemical properties, carbon nanomaterials are widely used in biomedicine. Especially for graphene and porous biomass carbon nanomaterials with high specific surface area and high conductivity, graphite and fructose are the main raw materials in this paper. Two functional carbon nanomaterials were designed and synthesized. Including the preparation of water-soluble graphene and its electrical conductivity, the preparation of Fe / N co-doped carbon nanobox and its ORR catalytic properties were studied. Goga was chemically modified with different amounts of Gallic acid, and the method of reducing go and GOGA to graphene by SHS was developed. The method has the advantages of simple process and environmental friendliness. The structure of rG0 and rGOGA is characterized by means of XRDX FI-IRI, XPSN Raman Tem and HRTEM. In addition, the structure of rG0 and rGOGA is characterized by Zeta potential. The water solubility and conductivity were characterized by contact angle test and electrical conductivity test. It was found that because of the repair effect of Gallic acid, Not only did the conductivity of graphene increase by 88900S / m ~ (-1), but also the graphene was water-soluble. The modification and repair mechanism of graphene was explored. (2) Biomass fructose was used as raw material. Three dimensional porous and highly graphitized CNBswere prepared by SHS with a conductivity of 40700 s / m, which was higher than that of graphene and carbon nanotubes prepared by traditional methods. Then FeCl3 and ammonia were used as nitrogen sources. Fe-N-CNBs loaded with Fe based nanoparticles were prepared by calcination at different temperatures. It was found that Fe based nanoparticles were mainly composed of Fe Fe 3C and Fe2N nanocrystals by XRD characterization. In addition, the properties of Fe-N CNBs were tested by electrochemical workstations and zinc air battery devices. The initial potential and half-wave potential of Fe-N-CNBs-600 catalyst (1.03 Vvs.RHE) and half-wave potential (0.875 Vvs.RHEs) are better than commercial Pt/C(1.01 and 0.745 Vvs.RHE0.The Fe-N-CNBs-600 catalyst also has good methanol resistance and stability under alkaline conditions.
【学位授予单位】：天津工业大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O613.71;TB383.1

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