g-C3N4/AB2O4催化剂的设计合成及DMFC阴极协同机制研究

Non-noble metal catalytic material has been considered as a key technology to realize Direct methanol fuel cell (DMFC) commercial applications. The research for oxygen reduction reaction is highly active and alcohol resistance of cathode catalyst is of great significance for the development of DMFCs. This project proposes to spinel AB2O4 instead of Pt, g-C3N4 instead of C, by using a facile electrodeposition process and solution method to obtain the controllable morphology, composition and structure of one-dimensionally ordered g-C3N4/AB2O4 nanotube arrays and NiCo2O4/g-C3N4/AB2O4 sandwich arrays. Based on the conditions of as-prepared composites, to clarify the controllable growth mechanism. By fully taking advantage of more active sites, good stability and alcohol resistance of g-C3N4 and spinel NiCo2O4, further study the oxygen reduction synergistic catalytic mechanism of the as-prepared cathode catalysts, in order to shorten electron transmission path, achieve the four electron transmission path, and eventually enhance the catalytic efficiency. The ultimate aim is to design and preparation of completely replaced Pt class catalysts with high catalytic activity, good stability, low cost, and alcohol resistance, and provide some important theories and technical support for selecting the high efficiency, stability and good resistant to alcohol of cathode materials.

研究对氧还原具有高催化活性、高稳定性、且耐醇的非贵金属阴极催化材料是实现直接甲醇燃料电池(DMFC)商业应用的关键技术之一。本项目提出以尖晶石型AB2O4代替Pt，以g-C3N4代替C，采用电沉积技术和溶液法，制备一维有序g-C3N4/AB2O4纳米管阵列和NiCo2O4/g-C3N4/AB2O4三明治阵列复合材料。通过对g-C3N4及AB2O4实现结构、组成和形态的理性设计与可控制备，可以充分利用类石墨相氮化碳(g-C3N4) 及尖晶石型NiCo2O4两者本身活性反应位点多和耐醇稳定性高等性能优势，从而深入研究g-C3N4与AB2O4之间的ORR协同催化机制，旨在实现缩短电子传输路径，使ORR按4e-途径进行，提高其电催化效率。以期最终实现催化活性高、稳定性好、成本低廉的耐醇完全代替Pt类贵金属的电催化材料的设计及制备目标，为遴选高效、稳定且耐醇新型阴极材料提供理论依据与技术支撑。

直接甲醇燃料电池被广泛认为是下一代储能设备的一个有前途的候选。为实际应用配置高效的直接甲醇燃料电池，制备高效、廉价的阴极氧还原电催化剂是一个紧迫的问题。本项目提出来一种通用的策略增强阴极氧还原性能—尖晶石纳米复合材料，主要研究内容：研究了不同尖晶石材料、碳基材料复合、离子掺杂、碳基材料改性等对复合阴极催化剂氧还原性能的影响规律。最终实现了这几类电极材料的可控制备、性能优化与储能器件组装，促进了尖晶石复合纳米材料在能源储存领域的应用。