大气压冷等离子体-乙醇协同制备钯基甲酸脱氢催化剂及其机理研究

开发高活性、高稳定性的钯基甲酸脱氢催化剂，对于加速直接甲酸燃料电池商业化进程，以及氢能的存储利用具有重要意义。前期研究表明，采用大气压冷等离子体，以乙醇为氢源，在乙醇产生氢活性物种还原和碳残留物种空间限域效应共同作用下，可制备小粒径、高分散，且具有优异性能的负载型Pd催化剂，但对其制备机制认识较为模糊。本项目拟采用大气压冷等离子体，以安全且易于存储和运输的乙醇为氢活性物种来源，开展大气压冷等离子体-乙醇协同制备钯基甲酸脱氢催化剂及其机理研究工作。通过系统实验研究，建立大气压冷等离子体制备钯基催化剂结构调控规律，并探明催化剂构效关系。通过发射光谱原位诊断研究，傅里叶变换红外光谱和质谱等在线分析技术，以及其他离线分析技术，揭示大气压冷等离子体-乙醇协同制备机理。基于钯基催化剂冷等离子体制备结构调控规律，构效关系及制备机理认识，为高性能钯基甲酸脱氢催化剂的设计和制备提供坚实的理论和实验基础。

Preparation of supported Pd-based catalysts with high activity and stability for formic acid dehydrogenation is of great significance for accelerating commercialization of direct formic acid fuel cell and the storage and utilization of hydrogen energy. Previous results showed that high performance supported Pd catalysts with smaller size and high dispersion of metallic Pd nanopaticles can be obtained under the influence of the active hydrogen species and the space-limiting effect of ethanol in atmospheric-pressure cold plasma. However, understanding of the preparation mechanism is still in obscure. In this project, atmospheric-pressure cold plasma will be adopted by using the active hydrogen species formed by ethanol, which is easy and safe to store and transport, to prepare Pd-based catalysts for formic acid dehydrogenation by the synergy of atmospheric-pressure cold plasma and ethanol and its mechanism will be disclosed. The structure regulation law and of Pd-based catalysts prepared by atmospheric pressure cold plasma will be established by systematic experimental study, and structure-property relationship of the catalysts will be demonstrated. The preparation mechanism will be disclosed by in-situ optical emission spectroscopy, on-line analytical techniques such as Fourier transform infrared spectroscopy and mass spectroscopy, and other off-line analytical techniques. Based on the understanding of structure regulation law of Pd-based catalysts by cold plasma, structure-property relationship and preparation mechanism, this will provide solid theoretical and experimental foundation for designing and preparation of high-performance Pd-based catalysts for formic acid dehydrogenation.