Freestanding and Permselective Graphene Oxide Membranes Assembled at Liquid/Liquid Interface through Novel "Stitch Chemistry"

提案编号：1603264，PI：Zhu，Jiahua Title：Chemically Stitching Graphene Oxide Nanosheets into Separation Membranes化学缝合氧化石墨烯纳米片成分离膜化学、石油化工和生物工程行业迫切需要以低能耗从工艺流中净化水。此外，传统的基于聚合物和陶瓷的膜技术在生物燃料分离中具有显著的挑战。氧化石墨烯（GO，厚度小于1.0 nm的片状材料）已被探索作为在水分离中具有巨大潜力的膜材料。膜将由这种片材的层组成。拟议的研究将使用新的“缝合”分子作为工具，将GO片组装成具有所需微结构图案和层间距的膜。这些膜被设计成在广泛的分离实践中实现水的选择性渗透分离。这项研究的成果是提供一种可转移的独立膜处理技术，能够彻底改变生物燃料的分离效率，并大大提高水的净化能力。通过对研究生进行专业培训，制定研究生课程，促进STEM教育，以及参与针对大学预科生的重点推广活动，来解决教育方面的广泛影响。本研究的重点是在使用由液/液界面促进的聚合化学时，对氧化石墨烯片进入独立膜的界面传输、反应动力学和自组装现象的基本理解。在液/液界面处的自组装将通过使用新型缝合分子来实现，以影响GO膜的层与层的间距、膜表面的形成和孔通道的表面化学。该研究将使用生物燃料分离和水净化应用的例子来测试所得膜的选择性和渗透性。具体的研究目标是：1）了解GO片层在液/液界面上的传输行为和组装成膜现象; 2）利用GO基平面上的反应性基团来调节GO膜的孔结构和表面化学性质，从而影响膜的结构和化学功能;以及3）揭示以生物燃料选择性渗透分离和水净化应用为目标的GO膜的过程-结构-性能关系。这项技术的可转让性将使其能够立即推广到广泛的分离应用。

Proposal Number: 1603264, PI: Zhu, JiahuaTitle: Chemically Stitching Graphene Oxide Nanosheets into Separation Membranes Purifying water from processing streams with low energy consumption is urgently needed in the chemical, petrochemical and bioengineering industries. In addition, conventional polymer- and ceramic-based membrane technologies have significant challenges in biofuel separations. Graphene oxide (GO, a sheet material with a thickness less than 1.0 nm) has been explored as a membrane material with great potential in water separations. The membrane would consist of layers of this sheet material. The proposed research will use novel "stitch" molecules as a tool to assemble GO sheets into a membrane with desired microstructure pattern and layer spacing. These membranes are designed to achieve permselective separation of water in a broad range of separation practices. The outcome of this research is to offer a transferrable freestanding membrane processing technology that is capable to revolutionize biofuel separation efficiency, and greatly improve water purification capability. The educational broader impacts are addressed through professional training of graduate students, development of graduate curriculum and promoted STEM education and engagement in focused outreach activities to pre-college students. This research focuses on the fundamental understanding of interfacial transport, reaction kinetics, and self-assembly phenomena of graphene oxide sheets into freestanding membranes at using polymerization chemistry facilitated by a liquid/liquid interface. The self assembly at the liquid/liquid interface will be enabled with the use of novel stitching molecules to impact the layer to layer spacing of the GO membrane, the formation of the membrane surface, and the surface chemistry of the pore channels. The research will use examples of biofuel separation and water purification applications to test the selectivity and permeability of the resultant membranes. The specific research goals are to: 1) understand the transport behavior and assembly phenomena of GO sheets into membranes at the liquid/liquid interface; 2) tune GO membrane pore microstructure and surface chemistry properties using reactive groups in the GO basal planes to impact the membrane's structure and chemical function; and 3) reveal the process-structure-property relationships of GO membranes targeting permselective biofuel separation and water purification applications. The transferability of this technology will enable its immediate dissemination to a wide range of separation applications.