摘要
用2,5-二(2-甲氧基-乙氧基)对苯二甲酰肼(BMTH)和1,3,5-三甲氧基-2,4,6-三甲酰基苯(TpOMe)缩聚,基于界面聚合法,在多孔三氧化二铝(AAO)基底上制备出一种二维共价有机骨架(COF)膜TpOMe-BMTH,并研究了所得膜材料对锂、镁离子的分离性能。结果显示,TpOMe-BMTH/AAO膜具有高的结晶性和良好的稳定性,并表现出优异的金属离子选择性,在LiCl(0.1 mol·L^(-1))和MgCl_(2)(0.1 mol·L^(-1))组成的二元混合离子体系中,对Li^(+)/Mg^(2+)的分离因子高达258。基于密度泛函理论的平面波赝势方法计算表明,材料孔道中的富氧低聚醚链对Li^(+)和Mg^(2+)的结合能分别为-282.69和-13.46 kJ·mol^(-1),使材料表现出强的亲锂特性,促进了Li^(+)沿着COF膜的一维孔道进行吸附扩散,最终实现锂、镁离子的高效分离。
The two⁃dimensional covalent organic framework(COF)membrane material TpOMe⁃BMTH was prepared on the anodic aluminum oxide(AAO)substrate with 2,5⁃di⁃(2⁃methoxy⁃methoxy⁃ethoxy)⁃phenylmethylhydrazide(BMTH)and 2,4,6⁃trimethoxy⁃1,3,5⁃benzenetricarbaldehyde(TpOMe)condensation based on interfacial polymeriza⁃tion.The separation properties of the obtained membrane material for lithium and magnesium ions were investigat⁃ed.Results showed that the TpOMe⁃BMTH/AAO membranes possessed high crystallization,good stability,and excellent metal ion selectivity,with a separation factor of up to 258 for Li^(+)/Mg^(2+)in a binary salt system consisting of LiCl(0.1 mol·L^(-1))and MgCl2(0.1 mol·L^(-1)).The plane wave pseudopotential method calculation based on the densi⁃ty functional theory showed that the binding energy of the oxygen⁃rich oligoether chains in the material pore for Li^(+)and Mg^(2+)was-282.69 or-13.46 kJ·mol^(-1).This result means that the obtained membrane has stronger lithium⁃philic properties and promotes Li^(+)adsorption diffusion along the one⁃dimensional pore of the COF membrane,finally enabling the efficient separation of lithium and magnesium ions.
作者
谢文典
隆月华
谢健阳
邢丽群
佘世雄
杨燕
黄智昊
XIE Wendian;LONG Yuehua;XIE Jianyang;XING Liqun;SHE Shixiong;YANG Yan;HUANG Zhihao(College of Chemical Engineering,Qinghai University,Xining 810016,China;Department of Materials Science and Engineering,City University of Hong Kong,Hong Kong 999077,China;School of Materials Science and Engineering,Harbin Institute of Technology,Harbin 150006,China)
出处
《无机化学学报》
SCIE
CAS
CSCD
北大核心
2024年第8期1528-1536,共9页
Chinese Journal of Inorganic Chemistry
基金
青海省自然科学基金(No.2020-ZJ-742)
国家自然科学基金(No.214610211)
青海省“昆仑英才·高端创新创业人才”项目资助。
关键词
共价有机骨架
薄膜
离子分离
covalent organic framework
membrane
ion separation
