二维原子晶体-半导体氧化物异质结的构筑及催化硼氢化物储氢机制的研究

In regard to the high adsorption/desorption temperature, sluggish dynamics of the hydrogen release from borohydrides, this project aims to construct heterojunctions between two-dimensional atomic crystal and semiconductor oxide. The active hydrogen spillover metal nanocatalysts will be further introduced. The formed composite will be utilized to catalyze the hydrogen absorption/desorption reactions of borohydrides. Through the reasonable design of the composition, engineering the heterojunction energy band, controlling the electron state of the heterjunctions, the catalytic activity is supposed to be effectively improved. The types of two-dimensional atomic crystals (such as graphene, and MoS2), metal oxide (TiO2, SiO2, and Co3O4) defects, the size of metal nanoparticles, structure the heterojunction composite will be examined to build the relationship between these factors and their catalytic properties. The catalytic performance of different composition, structure, morphology will be compared. Combined with the calculation of density functional theory, the microscopic catalytic nature of heterostructures will be revealed. The hydrogen atoms migration at the micro-interface and separation mechanism will be explained. The model between the catalytic performance and their structure and morphology will be established. The implementation of this project will provide useful guide and instruction for the development of efficient borohydride hydrogen storage system with cheap catalysts.

针对硼氢化物储氢材料吸放氢温度高，动力学缓慢等科学问题，本项目拟在二维原子晶体和半导体氧化物界面构筑异质结，并引入氢溢流活性金属粒子形成复合催化剂，对硼氢化物储氢材料进行有效催化。通过带隙匹配和能带工程设计，调控异质结的带宽及电子赋存状态，以期能够有效提高异质结的综合催化性能。探索二维原子晶体的种类（如石墨烯、MoS2等）、氧化物（如TiO2、SiO2、Co3O4等）的缺陷、金属纳米粒子的尺寸、复合材料的能带结构等与其催化性能之间的对应关系。通过不同组成、结构、形貌的异质结催化性能比较，并结合密度泛函理论计算，研究二维原子晶体异质结催化硼氢化物的作用原理和微观本质；揭示氢原子在微观界面的迁移和分离机制；建立催化性能与其组成、结构、形貌之间的构效关系模型。本项目的实施将为开发基于硼氢化物与廉价催化剂的高效储氢体系奠定理论基础和实验依据。

本项目以二维原子晶体和半导体氧化物界面构筑了异质结，并引入氢溢流活性金属粒子Ru等形成复合催化剂，对NaBH4储氢材料实现了有效催化。通过带隙匹配和能带工程设计，调控了异质结的带宽及电子赋存状态，有效提高了异质结的综合催化性能。探索了二维原子晶体的种类、氧化物的缺陷、金属纳米粒子的尺寸、复合材料的能带结构等与其催化性能之间的对应关系。通过不同组成、结构、形貌的异质结催化性能比较，并结合密度泛函理论计算，研究了二维原子晶体异质结催化硼氢化物的作用原理和微观本质，揭示了氢原子在微观界面的迁移和分离机制。本项目的成功实施将为开发基于硼氢化物与廉价催化剂的高效储氢体系奠定理论基础和实验依据。