Pt/层状双金属氧化物/石墨烯复合催化剂的研制及其对甲醇氧化的高效催化性能研究

Direct methanol fuel cell (DMFC) is a promising power source in portable devices and electronic products due to its high theoretical energy density, excellent environment-friendliness and easy transportation and storage. However, the practical application of DMFC is still limited by several problems, such as the poor catalytic activity and stability of anode catalysts. For the top priority issues of developing and optimizing hierarchical Pt based catalysts with more efficient and stable catalytic performance, we will adopt a novel approach based on surface functionalization, electrostatic-assembly and thermal treatment to synthesize Pt/layered double oxides-graphene (Pt/LDO-GN) composite catalyst. Then based on a trinity strategy of acid eching-pH supervision-electrochemical regulation, the orderly intercalated stacks, multilevel porosity and microelectronic structure of Pt can be finely tuned. To study the interaction between the micro-nano structure of Pt and its catalytic property, and methanol electrooxidation mechanism and reaction thermodynamics-kinetics specialties, characterization and analysis of the structure and electrocatalytic performance of the as-prepared catalyst, assistive with the theoretical simulation, will be progressively conducted. This project will be valuably instructive for the synthesis of highly efficient and stable catalyst and the development of high performance DMFC in terms of academic and applicable respects.

直接甲醇燃料电池（DMFC）由于具有能量密度高、环境友好、便于携带与储存等优点，因此在移动电源、便携式电子产品电源等领域具有广阔的应用前景，但阳极催化剂低的活性和稳定性等缺点阻碍了其实际应用。本项目围绕高效稳定多尺度Pt基催化剂的创制和优化这一核心和关键，提出基于表面功能化-静电组装-热处理的制备方法，制备结构新颖、性能优异的Pt/层状双金属氧化物-石墨烯插层结构复合催化剂材料；并基于不同程度酸蚀-pH调控-电化学调控三位一体的技术策略，调控该复合材料的有序化插层、多级孔道结构及Pt微观电子特性；通过对催化剂结构和电催化性能的表征，并结合理论模拟，揭示催化剂微纳结构与电化学性能的内在联系，阐明甲醇电氧化反应机理和电化学反应热、动力学特性。项目的实施将为指导新型高效稳定催化剂的合成、发展高性能直接甲醇燃料电池提供理论依据和技术支持，有重要的学术意义和应用价值。

直接甲醇燃料电池（DMFC）由于具有能量密度高、环境友好、便于携带安置等优点，受到了越来越广泛的关注，在移动电源、便携式电子产品等领域具有广阔的应用前景。目前，贵金属铂（Pt）是最常用的DMFC阳极催化剂，但由于Pt催化剂成本高，稳定性差，从而阻碍了DMFC的商业化发展。因此，开发出一种催化效率高、制备成本低、稳定性好的阳极催化剂是促进DMFC商业化发展的关键。以Pt为催化主体，引入第二种或者多种金属元素可以得到Pt基合金催化剂。合金催化剂的运用不仅降低了DMFC的制备成本，在一定程度上还表现出了较高的催化效率和良好的稳定性。赋予催化剂纳米颗粒载体，可以有效地促进纳米颗粒均匀负载，降低颗粒粒径，从而使得催化剂暴露更多的活性位点，进一步提高催化效率。基于以上设计思路及目标，本项目以Pt为催化主体，分别以钯（Pd）、镍（Ni）、石墨烯（GN）、镍铁层状双金属氢氧化物（Ni-Fe LDH）和镍铁氧化物（Ni-Fe LDO）为复合材料，采用多种方法构筑了一系列高效稳定复合催化剂。并通过多种实验方法，探讨了复合材料对催化剂催化效果的影响，揭示了复合材料与Pt之间的内在联系。