氧化石墨烯混合基质渗透汽化膜传质机理和制备基础研究

Owing to its unique properites, graphene oxide as a potential material has attracted a great attention in the field of membrane researches. It is extremely important theoretical significance and scientific value for the scientific application of graphene oxide in pervaporation to research on the transport mechanism of graphene oxide mixed matrix membranes. In this research, transport behavior of organic compound and water in network channel of graphene oxide is invesitgaed. The research background is the dehydration of organic compound-water azeotropes, utlizing graphene oxide , polyetherimide, sulfonated polyethersulfone and polyvinyl alcohol as pervaporation membrane materials. The interfaction between surfacial functional groups (e.g. -OH、-COOH、-O-、C=O) and polymer materials is investigated to study micro-phase equilibrium and interface behaviour of the dispersion phase and continous phase (polymer). For water as the permeate, facilitated transport characteristics of surfacial active groups of GO and changes of network structure of membranes are investigated. The transport mechanism model of GO mixed matrix membranes for pervaporation is built by means of numerical solution of non - uniform field diffusion equation and computer molecular dynamics simulation. This will guide the design of membrane microstructure and fabrication of high-performance dehydration membranes. We believe that this study, if achieved, will contribute a lot to energy saving and emission reduction and the development of membrane science and technology in our country.

氧化石墨烯以其独特功能作为分离膜材料，已引起膜研究领域的极大关注。研究氧化石墨烯混合基质渗透汽化膜传质机理，对于氧化石墨烯在渗透汽化膜领域中的科学应用有着极其重要的理论意义和科学价值。本研究以含水恒沸体系脱水为研究背景，以氧化石墨烯、聚醚酰亚胺 、磺化聚醚砜 、聚乙烯醇等为渗透汽化膜材料，研究有机物小分子（醇、酯等）和水在氧化石墨烯的网络通道中的传质行为，探讨氧化石墨烯表面功能基团（-OH、-COOH、-O-、C=O）与聚合物膜材料之间的相互作用，研究氧化石墨烯分散相与聚合物连续相间的微相平衡，考察氧化石墨烯表面活性基团、网络通道结构变化对水的促进传递作用和水快速通道形成机制，借助于非均匀场扩散方程数值求解和分子动力学模拟，建立氧化石墨烯混合基质渗透汽化膜传质机理模型，用以指导膜微结构设计和高性能大通量渗透汽化脱水膜制备，为国家节能减排重大需求和促进膜科学技术发展做出贡献。

采用高纯鳞片石墨High purity flake graphite，制备了氧化石墨烯graphene oxide （GO）。应用石墨烯（GR）、GO、还原氧化石墨烯 reduced graphene oxide（rGO）、石墨烯纳米片graphene nanosheets（GNS），制备了GO/PVA混合基质膜、GR/PVA混合基质膜、GO改性PEI/SL复合膜、GO和ZIF-67同时改性PEI/SL复合膜、PA/GO-PMIA复合纳滤膜、GO改性PA/PMIA复合纳滤膜、rGO膜、GNS/PEG杂化膜。进行了FT-IR、SEM、XRD、CA、TGA、XPS、AFM膜结构表征，考察了GO、GR、ZIF-67、GNS等在PEI、PMIA、PVA等膜材料中的扩散过程。研究了制膜过程GO、GR、rGO、GNS含量、分散速度、反应时间、反应温度、刮膜速度等因素对膜结构和性能的影响，结合传质机理研究，制备出了系列性能优异的混合基质膜。将其应用于乙醇水体系渗透汽化脱水、盐水体系透水和分盐、染料水体系染料截留、汽油体系脱硫等，考察了GO、GR、rGO、GNS含量、膜材料种类等因素对膜传质性能的影响，研究了温度、压力、料液种类、料液浓度、运行时间等因素对膜分离性能的影响。取得了有理论意义和有应用前景的研究成果，为国家节能减排和促进膜科学技术发展做出了贡献。本研究课题培养出站博士后2名、毕业博士生1名。发表学术论文34篇，其中SCI收录18篇、国内核心期刊5篇、国际会议5篇、国内会议6篇。