仿生三元共涂覆构筑高通量纳滤膜研究

Nanofiltration (NF) membrane has gained rapid development in recent years, especially for the significant strategic applications such as environmental protection, biopharmacy, and etc. The corresponding high-flux NF membranes have received more and more attention. For the first time, a ternary bionic coating system (composing of polyphenols, amino molecules, and metal ions) is disclosed to fabricate the high-flux NF membranes. Therein, polyphenols could react with amino molecules via Michael addition/Schiff base reaction, also could chelate with metal ions. The aforementioned competition reactions occurred in the co-deposition procedures could tune the surface chemistry of porous membranes to obtain NF membranes with both high flux and selectivity. The characterization on the permeate flux and rejection could illustrate the influences of incubation conditions (concentrations, mass ratios, incubation time, etc.) of ternary bionic coating system on the membrane performance. Meanwhile, the systematic physicochemical characterization could reveal the mechanism underlying the performance improvement of as-prepared membranes, and the separation conditions and optimized performance of the as-prepared NF membranes on the dye and antibiotic separation will be explored. In addition, the anti-fouling properties of novel nanofiltration membrane will be investigated. We believe this study will generate great impact on promoting the rapid development of membrane separation and technology theoretically and practically, and demonstrate the significant scientific and practical potential.

面向环保、生物制药等领域应用的高通量纳滤膜日益受到重视。本项目率先设计多酚类物质、氨基化物质、金属离子仿生三元体系共涂覆构筑高通量纳滤膜，利用多酚类物质与氨基化物质发生迈克尔加成/席夫碱反应以及金属离子与多酚类物质/氨基化物质作用进行仿生三元共涂覆，在共涂覆过程中通过仿生三元体系竞争反应调控多孔膜表面性能从而获得兼具高通量和高选择性的纳滤分离膜。进行渗透通量、截留率等测试阐明仿生三元共涂覆体系的配比、浓度、反应时间等条件对纳滤膜分离性能的影响规律，确定优化工艺条件。同时，通过系统的物理化学表征揭示仿生三元共涂覆构筑纳滤膜的改性机理及性能提升机制，并进一步探索新型纳滤膜抗污染性能、对染料及抗生素的分离条件及优化效果，为膜分离技术的迅速发展提供理论与实践基础，具有积极的科学意义和潜在的实用价值。

依赖传质速率差异进行物料分离的膜分离技术不仅能缓解世界范围内的水资源短缺问题，还能为工业上有机溶剂的处理和回收利用提供前沿的技术方法。本项目旨在采用将仿生材料与传统方法相结合的策略在多孔基膜上进行可调控界面反应来制备从水体系分离到有机溶剂体系分离的纳滤膜，最终获得在水及有机溶剂双体系环境下都兼具高通量、优异稳定性的新型纳滤膜。.本项目利用仿生材料并借鉴自然界竞争驱动进化机制提出仿生界面竞争涂覆策略获得高通量水处理用纳滤膜。依据第一过渡系金属离子可通过杂化轨道接受电子与多酚物质和氨基物质形成较强的配位键原理，结合多酚类物质能与氨基化物质发生迈克尔加成/席夫碱反应生成共价键，通过涂覆溶液体系中共价键与配位键间的竞争反应在多孔基膜上形成均匀的超薄（~33 nm）三元反应涂层。系统研究了仿生三元共涂覆过程中，反应物浓度、配比、反应时间等对复合纳滤膜选择层结构的影响规律及涂覆机理，所制备的pDA/PEI/Co2+复合纳滤膜性在实现100%截留刚果红（CR）和溴百里香酚蓝（BTB）染料的同时膜通量达到104 L m-2 h-1 bar-1 和 114 L m-2 h-1 bar-1的高值，比传统商用纳滤膜通量提高一个数量级，并具有优异的长期稳定性。.本项目成果发表SCI论文共52篇，获得授权国家发明专利3项，培养硕士生4名，博士生2名。获2021年黑龙江省自然科学二等奖（第一）1项。