Towards supramolecular chemistry with inorganic 2D nanomaterial building blocks

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Since the ground-breaking discovery that individual layers in graphite can be stably isolated to yield atomically thin graphene nanosheets, layered crystals have received enormous attention. In addition to graphite, a broad range of inorganic materials such as transition metal dichalcogenides or III-VI semiconductors are widely abundant in their layered form. As a process, delamination to individual nanosheets has had a transformative effect on materials science and technology by opening up exciting properties found in the two-dimensional (2D) exfoliated forms, not necessarily seen in their bulk counterparts. In addition, exfoliation creates materials with high aspect ratio and surface area. Recent years have seen significant progress to fundamentally study physical properties of a number of 2D materials. In addition, it was demonstrated that they can be exfoliated in liquids giving access to processing from solution which is beneficial for using these materials as building blocks in a broad range of potential applications from electronics to energy storage or electrocatalysis. However, up until now, the chemistry of the 2D materials is only little explored. In particular, wet chemical functionalization sequences to modify optical, electronic and surface properties are widely lacking. To fully exploit their potential, it will be necessary to fine-tune their properties.Within this proposal, a versatile and high throughput functionalization will be explored based on studying the noncovalent interaction of liquid exfoliated inorganic 2D materials with a broad range of organic molecules and polymers. The optical fingerprints of the nanomaterials which are highly sensitive to their chemical surrounding will be used to track interactions such as doping or photoinduced charge transfer. Based on this high throughput screening, suitable anchor groups for the functionalization with anionic, cationic or neutral functional moieties will be identified. This will give access to a broad range of 2D materials with tailored properties which can be processed from liquids by established techniques such as spin coating, drop casting or printing. In turn, this will allow for the fabrication of multicomponent inorganic/organic hybrid systems using supramolecular chemistry. Such systems are of great interest for both fundamental studies and various applications, as synergistic effects between different classes of nanomaterials can be exploited.