基于脱卤反应的碳材料的可控制备及其电化学应用

Carbon materials (CMs) have shown great potentials in the fields of energy conversion and storage due to their merits of low costs, wide availability of raw materials, and rich transformation pathways. Pyrolysis of organic matters is one very common strategy to fabricate CMs yet it inevitably leads to a series of problems such as high energy input, the generation of large amount of harmful waste gases, and collapse of pore structures. We intend to ease the situations of heavily involved pyrolysis by exploring clean and efficient synthetic ways based on dehalogenation reactions. By applying dehalogenation, we can accomplish the clean and efficient fabrication of CMs at room temperatures. By taking advantage of ultrahigh activity of dehalogenating carbon sites, we can synthesize multiply doped CMs and explore the synergistic effects of various combinations of heteroatoms and even metal conponents on electrocatalytic reactions. By employing alkaline with various species and dimensions for the dehalogenation reactions, we can realize the fine tuning of pore structure and morphology by designing different dehalogenation pathways. After the multiply doping and optimized synthesis, we shall obtain a series of CMs with enhanced electrochemical performance. We will also apply the dehalogenation strategy to dispose PVC plastic wastes in clean, highly efficient, and environmental friendly ways and convert them into high-quality carbon products. Our proposal will not only enrich the field of CMs fabrication but also push CMs forwards into the practical applications because of the clean, environmentally friendly, and highly efficient features.

碳材料以其低廉成本、来源广泛、转化路径丰富等优势已在能量的转化及存储等领域展现出重要价值。高温条件下有机分子脱官能团是制备碳材料的常用策略，但常常造成能耗高、有害废气多，孔结构塌陷等问题。申请人针对上述局限，拟发展基于低温碱性脱卤反应制备碳材料的新方法。利用强碱条件下的快速脱卤，实现纳米碳材料的室温高效制备；利用脱卤反应过程中产生的高活性中间体，实现硫、氮和金属等多元素掺杂与复合；通过选择碱性物种的种类和尺寸，设计不同的反应途径和条件，实现纳米碳材料孔结构及形貌的调控；通过多组分掺杂和后处理方式的优化，获得一系列具有优异性能的碳基电极材料。利用有机脱卤策略，实现废旧聚氯乙烯塑料的清洁、高效、无污染处理及转化为高品质碳材料。上述研究成果将不仅丰富碳材料合成方法，也将发展出含卤素高分子材料（如聚氯乙烯塑料）废料的清洁、高效、廉价的处理手段，将其转化为高品质碳电极材料。

碳材料来源广泛、成本低廉、转化路径丰富、可调可控性高，目前已在电化学能量存储与转化领域展现重要的应用价值。通过使用有机质碳源如生物质、高分子等，经历高温热处理脱除官能团，自下而上制备功能碳材料是常规合成策略，但往往能耗较高、有害废气多、孔结构易塌陷。申请人针对上述局限，发展了基于常/低温脱卤策略制备功能碳材料的新方法、新体系。具体包括：①基于有机脱卤反应策略，实现了碳材料的室温合成，特别的，实现了废旧PVC塑料的高效清洁处理及其向高质量碳材料的转化；②利用脱卤过程产生的高活性碳中间体，实现碳材料温和条件下的多组分掺杂，赋予产品功能化；③利用碱性物种物性不同，实现了碳材料孔结构、形貌等方面的调控；④优化掺杂组分、孔结构和形貌调控，获得一系列优异性能的碳基催化、储能材料；上述研究丰富了碳材料可控合成的方法、体系，为电化学催化、储能领域提供多种高性能廉价电极材料，推进碳材料在实际电催化、储能中的应用。