分子限域对Ni-Zn有序合金结构的可控诱导及丙烷脱氢性能强化机制研究

本项目针对丙烷脱氢高温反应条件下C-H选择性活化转化难以控制和催化剂活性组分易烧结团聚的难题，基于金属Ni良好的C-H键活化能力以及Zn原子结构调控的灵活性，以负载型非贵金属Ni-Zn金属间化合物催化剂为创新研究对象，另辟蹊径地提出以异核双金属络合物为前驱体的水热合成法诱导产生Ni-Zn键的设想，系统开展含高度有序Ni-Zn键负载型催化剂的方法设计和精准合成，并揭示其在C-H键活化转化中的强化作用机制，以期通过原子/分子水平的精细调控，实现大幅度提升丙烷脱氢丙烯选择性和催化剂稳定性。通过项目研究，解决“异核双金属络合物组成结构及催化剂前驱体转变条件协同控制”及“Ni-Zn键合方式和键合程度对C-H键活化转化方式的影响机制”两个关键科学问题。形成一套非贵金属有序合金催化材料的可控制备和精准调控技术，获得一类具有应用潜力的丙烷脱氢新型Ni基催化剂。

Aiming at the challenges of selective conversion of C-H and easy sintering of active components of catalyst under high temperature reaction conditions, this project focus on a new way to construct Ni-Zn intermetallic catalyst for propane dehydrogenation. Basing on the excellent C-H activation ability of Ni and the flexibility of Zn atomic structure control, a hydrothermal synthesis method using hetero-nuclear bimetallic complex as a precursor is taken to induce the formation of Ni-Zn bonds. Systematically studying its mechanism in the activation and conversion of C-H bond at the atomic/molecular level, in order to achieve a significant enhancement of the selectivity and stability for propane dehydrogenation. Through the research, two critical scientific problems should be solved: (1) the synergistic controlling of composition and its structure transformation of hetero-nuclear bimetallic complexes; (2) the influence of type and degree of Ni-Zn bonds on electronic and geometric effect among Ni sites and catalytic performance. The implementation of this project will develop a controllable preparation and precise regulation technologies for supported ordered alloy catalysts, and a new type of promising Ni-based catalyst for propane dehydrogenation can be obtained.