高分子膜燃料电池高效电催化剂设计和制备
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摘要
高分子膜燃料电池,作为一种清洁、可再生能源,受到能源部门、科学界广泛关注。但是,氧气电还原和有机小分子电氧化(如甲醇、甲酸)均是动力学缓慢的电催化反应,导致阴阳极需要高载量电催化剂—Pt/C。为此,设计、制备高效电催化剂不仅可以降低Pt使用量,而且可加速燃料电池商业化。催化剂主要由载体和纳米粒子组成,合理地选择载体和调控纳米粒子组成、结构等因素,均可明显提升催化活性。石墨烯是一种具有潜力的载体材料,为进一步提升其助催化性能,分别采取杂离子掺杂、表面包覆、表面造孔等改性方法,显著提升催化剂催化甲醇氧化和氧气还原活性。同时,发现部分非铂催化剂(如钯金和碳基催化剂)的催化氧还原反应活性和稳定性已经接近甚至优于商业化Pt/C催化剂。另一方面,清晰的电催化反应路径和电催化剂结构演变机制有助于设计电催化剂,提出铂单层结构演化模型以及新的铂金催化甲酸氧化机理—铂促进金表面吸附甲酸分子的C-H键断裂。
As a clean and renewable power source, polymeric membrane fuel cells have provoked extensive attention. However, oxygen reduction and organic small molecule oxidation which are highly irreversible reaction necessity high loading of Pt and severely impede the application of fuel cells. Therefore, design and fabrication of electrocatalyst with high performance is necessary. Design of support and tuning the composition and structure of nanoparticles greatly enhance the electrocatalytic activity. Graphene is a promising materials as support. The many method, such as doping, cladding, have been proposed to increase performance. In the meanwhile, Pd-based, carbon-based materials exhibited similar performance and stability as that of commercial Pt/C. On the other hand, clear reaction pathway and evolution formulation of structure of electrocatalyst are also important for engineering nanostructure with outstanding activity. Here, a new formic acid oxidation mechanism on Pt-Au system and structure evolution of Pt monolayer on Pd have been proposed.
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