Fu Yu, Wu Yue, Zeng Jiahui, Wang Shanshan, Li Xiaoyu, Zhang Wenxiang, Ma Heping
School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, 710049, China.
Chemistry. 2023 Nov 24;29(66):e202302462. doi: 10.1002/chem.202302462. Epub 2023 Oct 12.
Efficient and inherently safe NH storage and separation are of significant importance for the chemical industry. Herein, we proposed zwitterionic COF as a porous host to disperse LiCl for highly efficient NH storage and separation with record adsorption capacity. The equivalently cationic and anionic groups in the channels of zwitterionic COF could act as two separated sites to facilitate the dispersion of LiCl, hence the optimal composite exhibits a high capture capacity of 44.98 mmol/g at 25 °C and 1 bar, far exceeding other existing porous materials. Notably, the adsorption capacity is completely reversible and the efficient separation of NH from NH /CO /N mixture is achieved through breakthrough experiments. DFT calculation combined with XPS and Li NMR experimental results give insight into the interaction between zwitterionic COF and LiCl. This work extends possibilities for the development of efficient adsorbents for NH storage and separation.
高效且本质安全的氨储存和分离对化学工业至关重要。在此,我们提出两性离子共价有机框架作为多孔主体来分散LiCl,以实现高效的氨储存和分离,其吸附容量创纪录。两性离子共价有机框架通道中当量的阳离子和阴离子基团可作为两个分离的位点来促进LiCl的分散,因此该最佳复合材料在25 °C和1 bar下表现出44.98 mmol/g的高捕获容量,远超其他现有多孔材料。值得注意的是,吸附容量完全可逆,并且通过突破实验实现了从NH₃/N₂/CO₂混合物中高效分离氨。密度泛函理论计算结合X射线光电子能谱和锂核磁共振实验结果深入了解了两性离子共价有机框架与LiCl之间的相互作用。这项工作拓展了开发用于氨储存和分离的高效吸附剂的可能性。