担载型低/非贵金属纳米催化材料的制备及其在硼肼制氢上的应用

Hydrazine borane (N2H4BH3) is now a novel and promising hydrogen storage/generation material. The key point and bid hurdel for the practical application of hydrazine borane is serching for the highly selective and activitive, low-cost, and long-time stable catalysts to insure the contronable hydrogn generation from hydrazine borane at mild condition. Based on the molecular structure and physical/chemical properties of hydrazine borane, this project will focus on design and synthesis of supported low/none noble metal containing nanocatalysts with different cmopositions, architectures, lattice planes and supporters through various novel methods for preparition of nanomaterial.The well synegetic effects of metallic active sites to sites and active sites to supporters may has the potential to greatly increase the catalytic properties and lower the costs of catalysts. All the prepared catalysts will be applied on the dehydrogenation of hydrazine borane, and the catalystic activities, selectives, recycling stabilities, as well as the mechanism of the reactions will be comprehensively and thoroughly studied. The success of this project will provide the experimental basis for the practical application of hydrazine borane as hydrogen storage/generation material, and also supply the scientific theories for the development of novel and "clean" energy.

硼肼（N2H4B3）是一种新型的极具应用前景的储氢/制氢材料。寻求高选择性、高活性、低成本、长寿命的催化材料以保障硼肼在温和条件下高效可控地释放氢气，是推动该储氢/制氢体系实用化进程的关键和难点。本项目针对硼肼分子结构与其物理化学性质的特点，采用不同的纳米制备新方法，设计并合成具有不同组分、结构、晶面、载体的低/非贵金属纳米担载型催化材料。充分发挥金属活性组分间以及活性组分与载体间的协同作用，以期提高催化材料的性能及降低催化剂的成本。研究所合成催化剂的活性、选择性及循环稳定性，探讨其催化反应机理，为促进硼肼储氢/制氢的实际应用提供可靠的实验依据，同时为新型清洁能源的开发研究奠定科学的理论基础。

储氢是氢经济中的核心技术，是制约氢燃料电池车大规模商业化的瓶颈之一。开发低廉高性能金属催化剂，是解决储氢材料放氢选择性差，动力学缓慢问题的关键。项目对储氢用金属催化材料进行了深入的研究，主要研究成果为： 1)设计并制备了高效硼肼与水合肼制氢用非贵金属催化材料；2）揭示了甲酸催化放氢中单金属催化材料Pd 活性低的制约因素，通过合金化及表面压应变等降低了纳米Pd 的表面能/吸附能，大幅提升其常温常压下的催化活性，建立了普适性的设计新策略，并实现了Pd 的部分替代；2）提出了高活性电催化合成氨催化材料设计及材料筛选原则，通过构建富含低配位原子的催化表面，将没有活性的块体Au 变成了常温常压水溶液条件下性能优异的电催化氮气还原合成氨的催化材料。研究结果发表于国际著名期刊，如Advanced Materials, Energy & Environmental Science, Advanced Functional Materials等；培养研究生6人，博士后1人；其中2人获得吉林省优秀博士学位论文，1人获得吉林省优秀硕士论文；负责人以第一发明人获授权专利2项，申请专利4项；负责人受邀在第十六届金属-氢体系国际研讨会（MH2018）和中国材料大会2018等国内外重要学术会议做特邀报告，积极参与国际合作与交流。