重油残渣基高性能石墨烯的可控制备及其作为太阳能电池电极的研究

The heavy oil residues are the bottom product obtained after the distillation process of petroleum, showing a tremendous potential as a low-cost carbon source for industrial synthesis of various value-added new carbon materials. On the other hand, owing to its outstanding chemical and physical properties, graphene has been attracting great potential applications in many research fields. However, it is still a bottleneck to synthesize high-performance graphene from heavy oil residue in large scale. In the proposed research, a new technique to synthesize the high-performance graphene (with high conductivity, high surface area, high catalysis activity and high dispersity) from heavy oil residue by using catalyst template will be developed. The formation mechanism of graphene from pyrolysis of oil residue will be studied. The catalyst template will be reused after the synthesis of graphene in order to obtain the optimal technological process for industrial production. In addition, the heteroatom doping will be explored to tailor the intrinsic catalytic activities of synthesized graphene as a counter electrode for high-performance dye-sensitized solar cells. The proposed study will be helpful to develop a new technology for economically converting heavy oil residue into high-performance graphene in large scale, and it will open up new avenues in deep processing and comprehensive utilization of heavy oil residue.

廉价的重油残渣是工业化生产各种高附加值新型碳材料的潜在理想原料。而另一方面，石墨烯具有优异的物理和化学性质，在众多领域展现出了巨大的应用前景。但目前利用重油残渣规模化制备高性能石墨烯材料仍是一大瓶颈难题。本研究拟以重油残渣为碳源，采用模板催化法开展定向构筑高性能石墨烯（高导电性、高比表面积、高催化活性及高分散性）的制备研究，探索重质油残渣模板法热裂解合成石墨烯的反应规律，对反应后的模板重复利用进行研究，获得批量制备高性能石墨烯的最佳工艺路线。通过杂原子原位掺杂调控石墨烯电子结构及催化活性，实现其在染料敏化太阳能电池对电极领域的高效利用。本研究预期将研发出重油残渣基高性能石墨烯材料的低成本、批量化制备技术，为扩展传统石油加工过程的产品链、实现资源的高附加值综合利用提供新的途径。

廉价的重油残渣是工业化生产各种高附加值新型碳材料的潜在理想原料。而另一方面，石墨烯具有优异的物理和化学性质，在众多领域展现出了巨大的应用前景。但目前利用重油残渣规模化制备高性能石墨烯材料仍是一大瓶颈难题。本项目以重油残渣的高附加值利用为出发点，开展重油残渣基碳材料的可控制备，开发了低成本制备高孔体积富氮多孔石墨烯材料的新工艺，揭示了碳基复合电极材料在使役过程中的结构演变规律。掌握了高导电性、高比表面积和高催化活性的石墨烯材料的成套制备工艺，揭示了其可控定向生长机理，从实验和理论上揭示石墨烯电极材料表面活性位点对电催化性能的影响，掌握了成套高效稳定电池组装的技术。此外，通过缺陷工程耦合Co单原子，对纳米孔石墨烯进行改性来进一步提升了其催化还原I3-的活性，提升了染料敏化太阳能电池能量转换效率。重点通过实验分析和理论计算来揭示出了石墨烯表面Co-Nx-C组分的催化活性，可为今后石墨烯基对电极的设计提供指导依据。此外，首次实现了石油沥青基电磁波吸收材料的制备，揭示了材料内部的电磁波损耗机制，提出了低成本、批量制备“薄、轻、宽、强”电磁波吸收材料的新工艺，拓展了石油沥青的高附加值利用范围。