富勒烯插层氧化石墨烯超薄纳滤膜的制备及结构调控研究

High performance nanofiltration membranes are very important for membrane separation processes, and greatly demanded in the water purification, energy and environment fields. However, it is still a big challenge to fabricate the GO-based nanofiltration membranes with high permeation flux and precise pore size. Currently, the GO-based nanofiltration membranes usually have low permeation fluxes, especially in which the interlayer spacing in the GO nanosheets is difficult to control precisely. Meanwhile, the size of GO nanosheets must be bigger than the pore size of supports for the membrane prepared by filtration. Here we present a novel approach to fabricate the ultrathin GO nanofiltration membranes by using the sacrificial layer of nickel hydroxide nanosheets, in which sandwich-type nanosheets of GO and fullerenes C60 are stacked into the laminar membranes. The intercalation of C60 precisely modulate the interlayer spacing of GO membranes. The fabricated membranes should have the high flux and precise pore size with narrow distribution. This work will study on the preparation of nano-size GO nanosheets, synthesis of amino grafted C60 molecules, fabrication and characterizations of the C60 intercalated GO nanofiltration membranes, regulatory mechanism of d-space of GO nanosheets, and structure-related performance of the membranes. Furthermore, effects of C60 content, grafting groups, and size of GO nanosheets on structure and separation performances of the as-fabricated membrane will be studied. This work will produce new insights into the design and fabrication of GO-based nanofiltration membranes with high flux for water purification, environmental remediation, and others fields.

面向水净化、能源和环境等领域对高性能纳滤膜的重大需求、针对氧化石墨烯（GO）纳滤膜的通量低、孔径难精确控制、GO纳米片尺寸较大的难题，提出氢氧化镍纳米片牺牲层在制备大孔基膜上富勒烯（C60）插层GO超薄纳滤膜的成膜原理，构建具有“砖墙”结构的大通量、孔径精确控制的GO纳滤膜。重点开展：1）小尺寸GO纳米片的制备和C60的氨基功能化；2）基于“砖墙”构架结构的作用原理、以GO纳米片为“砖”、氨基功能化C60分子为“粘结剂”经缩合反应构建结构稳定的C60插层GO超薄纳滤膜，研究成膜原理及制膜工艺；3）C60调控GO膜层间距的作用机理，GO尺寸对膜结构和性能的影响规律。获得的成膜原理、GO膜层间距的作用机理及GO纳滤膜的构-效关系，可为高性能二维纳米材料纳滤膜的研究提供新思路和理论指导，具有重要的科学意义；制备的大通量、孔径分布窄的纳滤膜，可为水净化等领域提供高性能纳滤膜，具有良好的应用价值。

面向水净化、能源和环境等领域对高性能纳滤膜的重大需求、针对氧化石墨烯（GO）纳滤膜的通量低、孔径难精确控制、GO纳米片尺寸较大的难题，项目在前期研究工作基础上，提出了氢氧化镍纳米片牺牲层在大孔基膜上制备富勒烯（C60）插层GO超薄纳滤膜的成膜原理，构建了具有“砖墙”结构的大通量、孔径精确控制的GO纳滤膜，揭示了C60调控GO膜层间距的作用机理、GO尺寸对膜结构和性能的影响规律。在C60插层GO纳滤膜研究的基础上，开发了Ni(OH)2纳米片插层模板法和壳聚糖高分子链插层交联法，均实现了对GO膜层间距的有效调控，获得了通量高、尺寸选择性好高性能GO纳滤膜。获得的成膜原理、GO膜层间距的作用机理及GO纳滤膜的构-效关系，可为高性能二维纳米材料纳滤膜的研究提供新思路和理论指导，具有重要的科学意义。.受启发于上述GO纳滤膜的研究，针对界面聚合聚酰胺纳滤膜通量较小的问题，从聚合方法出发开发了全新的醛-氨界面聚合法制备疏松纳滤膜、从降低过滤阻力出发开发了超薄磺化介孔中间层和支撑层法制备高通量聚酰胺纳滤，获得了3种具有良好应用前景的高通量聚酰胺纳滤膜。针对可化学接枝中空纤维基膜缺乏的问题，开发了2种易接枝功能化的中空纤维基膜材料，并由此获得高通量的中空纤维超滤基膜及高通量表面接枝中空纤维纳滤复合膜。可为水净化等领域提供高性能纳滤膜，具有良好的应用价值。.研究结果申请国家发明专利2件，在J. Membr. Sci.（6篇）、Chem. Eng. J.、AIChE J.、Chem. Eng. Sci.学术期刊上发表SCI收录论文11篇，培养博士生2人、硕士生9人。