梯度掺杂界面功能化核壳结构氧化物制备及其担载Pt基催化剂的活性与稳定性研究

To resolve the key technical issues of high cost and durability absence in the commercialization of Proton Exchange Membrane Fuel Cells (PEMFCs), this project plans to work with the perspective on elevating the electrical transport of oxides support and enhancing the interaction between Pt nanoparticles and support materials via a brand new interfacial gradient functionalization Doping route. Based on the technique of Plasma Enhanced Chemical Vapor Deposition (PECVD), the novel core shell structured oxide (e.g. TiO2) with gradient doping concentration at interface support Pt catalysts are obtained through carbon, carbon/nitrogen, and transition metal assisted interfacial functionalization doping, which enhances its activity to maximal extent as well as the durability. Moreover, the intensive understanding in principle of activity enhancement in oxide support Pt catalyst with gradient core shell structure will provide the theoretical guidance for promoting the performance of catalyst and minimizing the usage of precious metal successively. And the research of this project will provide new strategy and technology for the performance improvement of PEMFCs catalyst, and promote the methodology of electrocatalysis and expand the research contents. The synthesis of novel core shell structured oxide support Pt catalysts will significantly elevate the commercialization step of PEMFCs system in terms of reduce usage of precious metal and cost. The approach of those catalysts is of great academic significance and practical value.

本项目针对阻碍质子交换膜燃料电池(PEMFC)商业化的成本高、寿命短等技术瓶颈，拟从界面功能化角度入手，提高氧化物载体界面电输运性能、增强Pt纳米粒子与氧化物载体界面之间的相互作用、改善功能化载体界面的助催化作用。通过基于等离子增强化学气相沉积方法实现高稳定性氧化物(TiO2等)界面梯度碳掺杂功能化、碳氮掺杂双功能化及过渡金属辅助的界面梯度共掺杂多功能化改性，制备具有改性元素掺杂浓度梯度分布的新型核壳结构氧化物为载体的Pt基催化剂。揭示梯度掺杂核壳结构氧化物担载Pt基催化剂活性与稳定性的增强机制，为提升催化性能、降低贵金属载量提供理论依据。本项目有望为PEMFC催化剂Pt载量的降低提供全新的策略与方法，促进电催化理论发展。新型梯度掺杂核壳结构氧化物载体担载Pt基催化剂的研制成功将加速PEMFC商业化进程、对延长PEMFC寿命、降低Pt载量具有重要的学术意义与显著的实际应用价值。

质子交换膜燃料电池(PEMFC)是一种绿色环保能源，然而其商业化仍受成本和寿命制约；其中催化剂运行中催化活性与稳定性是制约PEMFC商业化的关键因素之一。本项目针对阻碍质子交换膜燃料电池(PEMFC)商业化的成本高、寿命短等技术瓶颈，从界面功能化角度入手，提高氧化物载体界面电输运性能、增强Pt纳米粒子与氧化物载体界面之间的相互作用、改善功能化载体界面的助催化作用。在本项目中，已经通过基于等离子增强化学气相沉积方法实现高稳定性氧化物(TiO2等)界面梯度碳掺杂功能化、碳氮掺杂双功能化及过渡金属辅助的界面梯度共掺杂多功能化改性，制备了具有改性元素掺杂浓度梯度分布的新型核壳结构氧化物为载体的Pt基催化剂。揭示了梯度掺杂核壳结构氧化物担载Pt基催化剂活性与稳定性的增强机制，为提升催化性能、降低贵金属载量提供理论依据。本项目的研究结果为PEMFC催化剂Pt载量的降低提供全新的策略与方法，促进了电催化理论发展。新型梯度掺杂核壳结构氧化物载体担载Pt基催化剂的研制成功对加速PEMFC商业化进程、对延长PEMFC寿命、降低Pt载量具有重要的学术意义与显著的实际应用价值。截止目前，在国家基金的资助下，共发表核心以上科研论文86篇，其中SCI收录论文84篇，所发表SCI论文目前他引264次。申请国家发明专利18项。