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Abstract
Mass transport through graphene is receiving increasing attention due to the potential for molecular sieving. Experimental studies are mostly limited to the translocation of protons, ions, and water molecules, and results for larger molecules through graphene are rare. Here, we perform controlled radical polymerization with surface-anchored self-assembled initiator monolayer in a monomer solution with single-layer graphene separating the initiator from the monomer. We demonstrate that neutral monomers are able to pass through the graphene (via native defects) and increase the graphene defects ratio (Raman ID/IG) from ca. 0.09 to 0.22. The translocations of anionic and cationic monomers through graphene are significantly slower due to chemical interactions of monomers with the graphene defects. Interestingly, if micropatterned initiator-monolayers are used, the translocations of anionic monomers apparently cut the graphene sheet into congruent microscopic structures. The varied interactions between monomers and graphene defects are further investigated by quantum molecular dynamics simulations.
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; Dianat, Arezoo 4 ; Liu, Xiaoling 5 ; Xiao, Peng 6 ; Amin, Ihsan 7 ; Gutierrez, Rafael 4 ; Chen, Tao 6 ; Zschech, Ehrenfried 8 ; Cuniberti, Gianaurelio 9 ; Jordan, Rainer 1 1 Chair of Macromolecular Chemistry, Faculty of Chemistry and Food Chemistry, School of Science, Technische Universität Dresden, Dresden, Germany; Center for Advancing Electronics Dresden, Technische Universität Dresden, Dresden, Germany
2 Institute for Materials Science and Max Bergmann Center of Biomaterials, Technische Universität Dresden, Dresden, Germany; Fraunhofer Institute for Ceramic Technologies and Systems (IKTS), Dresden, Germany
3 Institute for Materials Science and Max Bergmann Center of Biomaterials, Technische Universität Dresden, Dresden, Germany; Max Planck Institute for the Physics of Complex Systems, Dresden, Germany
4 Institute for Materials Science and Max Bergmann Center of Biomaterials, Technische Universität Dresden, Dresden, Germany
5 Leibniz-Institut für Polymerforschung Dresden e.V., Dresden, Germany
6 Key Laboratory of Marine Materials and Related Technologies, Zhejiang Key Laboratory of Marine Materials and Protective Technologies, Ningbo Institute of Material Technology and Engineering, Chinese Academy of Sciences, Ningbo, China
7 Chair of Macromolecular Chemistry, Faculty of Chemistry and Food Chemistry, School of Science, Technische Universität Dresden, Dresden, Germany; Junior Research Group Biosensing Surfaces, Leibniz Institute for Plasma Science and Technology, INP Greifswald e.V., Greifswald, Germany
8 Center for Advancing Electronics Dresden, Technische Universität Dresden, Dresden, Germany; Fraunhofer Institute for Ceramic Technologies and Systems (IKTS), Dresden, Germany
9 Center for Advancing Electronics Dresden, Technische Universität Dresden, Dresden, Germany; Institute for Materials Science and Max Bergmann Center of Biomaterials, Technische Universität Dresden, Dresden, Germany; Dresden Center for Computational Materials Science, Technische Universität Dresden, Dresden, Germany




