基于纳米多孔材料的二氧化碳原位催化转化

碳减排作为一项影响国计民生的重大问题，已经引起了全世界的广泛关注。人们开发出一系列基于化学吸收法、物理吸附法的碳捕捉方法，并相应地研究了对二氧化碳的地下封存技术。然而，这些方法都不能从根本上解决大量二氧化碳的出路问题。金属有机骨架材料是一类由金属氧簇和有机配体聚合而成的新型纳米多孔材料。此类材料具有高比表面积、可功能化等优点，但是目前为止还没有利用该类材料直接催化转化二氧化碳的研究。同时，在真实工业废气排放的复杂环境中，此类材料的捕捉与催化性能研究也是一项空白。在本项目中，我们将通过对金属氧簇构造单元的研究来设计、合成新型具有催化活性金属有机骨架材料，同时系统性地研究有机配体及其官能团对于捕捉和催化反应的影响。进而通过合成后修饰的手段，引入其它复杂催化活性中心，进一步提高相应二氧化碳催化反应的选择性与转化率。最终实现对二氧化碳捕捉、储存与催化转化一体化系统的研究和建立。

Carbon emmision control is one of the most critical issue in the world and has drawn much attention lately. Many carbon capture techniques had been developed based upon chemical absorption and physical adsorption.Meanwhile carbon sequestration storage is established where carbon dioxide is designed to stored in some geological formations. Apparently such methods may not fundamentally solve the challenge. Metal-organic frameworks are a new class of nanoporous materials constructed from metal clusters and organic linkers.Although these materials had shown high surface area, high functionality, no work had been done using them as heterogeneous catalysts to convert carbon dioxide thus captured. Moreover investigation of their capture and catalytic performance under industrial gas emission condition is required. Hereby, in this proposal, we will design and synthesize novel catalytical-active MOFs by altering metal clusters and changing various organic linkers. Also different active centers will be introduced into MOFs via post-synthetic modification to further improve their capture selectivity and conversion efficiency. Ultimately, a system of carbon capture, storage and catalytic conversion will be studied and established.