纳米材料催化硼氢化物肼合物放氢反应的原位研究

项目名称： 纳米材料催化硼氢化物肼合物放氢反应的原位研究

项目编号： No.U1232120

项目类型： 联合基金项目

立项/批准年度： 2013

项目学科： 物理学II

项目作者： 吴国涛

作者单位： 中国科学院大连化学物理研究所

项目金额： 60万元

中文摘要： 金属硼氢化物肼合物是金属硼氢化物与肼复合形成的一类新的化合物。在此类化合物中，Hδ+和Hδ-共存，有利于氢气的释放。本申请拟利用上海同步辐射光源装置X射线衍射线站和X射线吸收线站对这些新化合物进行结构测定和通过原位反应实验研究纳米材料催化放氢反应机理。通过理论计算与实验结果相结合的方式，进一步了解金属氨硼烷和肼的相互作用以及催化反应中过渡态、中间体、反应路径和反应产物，旨在获得反应过程的热力学和动力学数据。全面了解催化剂形貌、成分、含量、制备条件和结构对催化反应活性的影响,为金属硼氢化物肼合物成为实用的储氢材料提供理论依据。

中文关键词： 硼氢化物肼合物；X射线衍射；X射线吸收；纳米材料；催化

英文摘要： Borohydride hydrazinates are a series of new compounds, which are formed through the coordination of hydrazine, a kind of bidentate ligand, with metal cations in borohydrides. For this kind of materials, Hδ+ and Hδ– co-exist in a single phase, expectedly facilitating the dehydrogenation of borohydride hydrazinates.This study aims at solving the crystal structures of borohydride hydrazinates and investigating the mechanism of the catalytic dehydrogenation of borohydride hydrazinates on transition metal nanomaterials. Synchrotron radiation powder X-ray diffraction (XRD) measurements, in-situ X-ray absorption fine structure (XAFS) and in-stiu XRD at Shanghai Facility (SSRF) are the effective experimental methods to get the necessary information. Combining first-principles calculations with experimental results, we could have an insight into the interaction between borohydride and hydrazine, transitional states of reactions on the surface of catalysts,intermediates, reaction paths and products during the catalytic dehydrogenation of borohydride hydrazinates. Through this research, it could be expected that thermodynamic and kinetic data of the catalytic dehydrogenation of borohydride hydrazinates could be obtained and that effects of shapes, compositions, contents, synthesis methods and microstructures of catalysts

英文关键词： borohydride hydrazinates；X-ray diffraction；X-ray absorption；nano-materials；catalysis