“流动化学”制备含锇、铑等贵金属多重键的多酸体系及催化性能研究

Uncovering the unique characters of continuous flow chemistry are the stepping stones to harnessing its power for technological innovation in inorganic materials for scientific applications. Compared to the traditional synthesis of polyoxometalate clusters under 'one-pot' solution processing conditions and hydrothermal (solvothermal, ionthermal) reaction, computer controlled continuous flow chemistry has its advantage to preciously control reaction rate, speed up and scale up the synthesis, deliver products with better yields etc. A general approach to the design and synthesis of noble metals-polyoxometalates composites is envisaged such that researchers can utilize a variety of building blocks to further understand the intrinsic characters of cluster assembly. The overall objectives of the proposed 4 year research program will be to: 1) construct continuous flow chemistry systems including linear, networked flow-reactor systems for the programmable assembly of the polyoxometalate clusters; 2) use the universal building block library within the flow chemistry system to synthesize new clusters containing noble metals, and unveil the formation mechanism of metal-metal multiple bonds; 3) explore the catalytic activity of POMs for alcohol oxidation / alkene epoxidation and water splitting, then set the stage for application of the materials with high catalytic activity.

"连续流动化学"是无机合成化学中一种极具发展潜力的科学手段, 与溶液合成、水热(溶剂热、离子热)合成方法相比, 计算机控制的"连续流动化学"具有可精确调控反应速度、缩短反应周期、优化并放大化学反应、提高产率的独特优势。 本项目旨在利用"连续流动化学"方法合成含锇、铑等贵金属的多酸复杂体系并研究体系的催化性能, 主要包括以下三个方面: 1) 发展"连续流动化学"手段(含串联型 / 网络型反应系统),建立具有自主知识产权的精确、高效、快速、智能的功能多酸化合物合成方法；2) 合成一系列贵金属-多酸复杂体系并侧重于金属-金属多重键的生成, 揭示多重键的形成机理并探索该体系的组装规律；3) 发掘该体系对于醇类 / 烯类底物的催化氧化性能和分解水的催化性能, 揭示结构与催化性能之间的内在联系，实现定向构筑功能性多酸材料的目标。