金属有机骨架材料开发及绿色能源净化与绿色化学催化应用

The developing of a material is interesting in worldwide research, especially material related for energy and environment. Metal-Organic Frameworks (MOFs) are one of material which their outstanding properties (large surface and tunable pore design) has allowed us to manufacture powerful and efficient devices for a wide variety of tasks, making function materials important to our daily life such as energy and environment. Including with the crisis energy source and environmental concern due to the prodigious increasing of population in the world, have driving force us to search and find new renewable energy source and friendly with environment. Biogas which produce from waste, could answer in several problem before because of their consist of methane (CH4) within can using as energy and carbondioxide (CO2) with can convert to several fine chemical. However, the powerful and efficient of biogas performance have through the future technological process which integrated/relative to material field. In this project we will focus on the development of novel MOF materials via multi-metal, mixed ligands and nano-composite synthesis MOFs which it use for adsorbent in biogas upgrading (bio-methane for energy) and also can apply for any separation process of CO2 mixture. Furthermore, those MOFs will apply as catalyst for biogas reforming (CO2 dry reforming from CH4 to synthesis gas of H2, CO) and CO2 carboxylation of theminal alkynes to acid compound which these catalysts could also work in several reaction of carboxylation of CO2. The most attractive of this project is simple method but powerful innovative of new material for multi-function or application (adsorbent and catalyst). It is to be expected that a better knowledge of this fundamentals could lead to new and improved materials to the commercial potential in future. We also hopefully aim to contribute to the Chinese society and more specific to the Chinese economy.

当今世界重视材料的开发，尤其是能源和环境材料。金属有机骨架材料（metal organic frameworks, MOFs）是近年所开发出的性能杰出的材料之一，我们能利用其极大比表面积和可调孔道等特性创造出各种性能优异和高效的材料及器件，其中包括与生活息息相关的能源与环境功能材料。随着人口增长，日益严峻的能源和环境问题驱使着我们去开发新的可再生洁净能源。沼气，由废弃有机成分物质产生，其主要成分甲烷和二氧化碳，前者可以作为能源直接使用，而后者可以催化转化为精细化工品。本项目的研究将围绕这两点展开。其一，开发新型MOFs材料吸附分离二氧化碳升级沼气得到生物甲烷作为能源；其二，将MOFs与高效催化剂复合进行1）沼气重整，即二氧化碳/甲烷干重整合成氢气和一氧化碳，2）对二氧化碳羧化催化合成精细化工品。本项目重点从经济性和实用性对MOFs材料进行开发研究，相信在不久的将来这些新型

本项目旨在设计和合成一种基于金属有机骨架（MOFS）的新型材料，该材料主要用于吸附分离和催化。研究了利用已开发材料（MOFs）对二氧化碳进行吸附净化或升级为净化CH4（CO2/CH4分离）。由于二氧化碳是副产物，且是目前造成气候变暖的主要原因之一，因此接下来利用已开发的MOFs作为催化剂的主要任务是CO2利用或将二氧化碳转化为精细化工产品。该项目合成的MOFs结构设计是基于金属簇、有机连接体、复合材料或改性策略，以开发出一种新的MOF材料。并发明了一种更环保或低能耗（如室温法合成）或最快的途径（如喷雾干燥制备法）的合成方法。同时，研究了合成路线对已开发的MOFs的结构和性能的影响。随后，利用已开发的材料作为非均相催化剂，并将二氧化碳转化为精细化学品或升级化学产品(二氧化碳利用)。以二氧化碳为C1碳源，利用MOFS为催化剂，合成了一种羧酸和碳酸盐化合物。MOFs在其应用中的主要缺点是其化学和热性能的稳定性。选择稳定度高的MOFs，是简单的选择，但并不限于此。利用热分解法使其转变为碳材料是提高该材料稳定性的另一种选择。此外，在最佳条件下的热分解可以提供有利于催化等特殊应用是的纳米金属或金属氧化物，因此，在一定条件下，利用已开发的MOF在掺杂多孔碳中进行热分解，从而得到了纳米金属颗粒，并将其作为一种强的非均相催化剂用于CO2转化反应和电化学反应。合成的MOF不仅限于此反应，而且还应用于新颖多样的催化剂反应，如均聚反应、聚合反应、酯化反应、诺伦加尔缩合反应等。