Free-standing homochiral 2D monolayers by exfoliation of molecular crystals

Jinqiao Dong, Lingmei Liu, Chunxia Tan, Qisong Xu, Jiachen Zhang, Zhiwei Qiao, Dandan Chu, Yan Liu, Qun Zhang, Jianwen Jiang, Yu Han (), Anthony P. Davis () and Yong Cui ()
Additional contact information
Jinqiao Dong: Shanghai Jiao Tong University
Lingmei Liu: Chongqing University
Chunxia Tan: Shanghai Jiao Tong University
Qisong Xu: National University of Singapore
Jiachen Zhang: University of Science and Technology of China
Zhiwei Qiao: National University of Singapore
Dandan Chu: Shanghai Jiao Tong University
Yan Liu: Shanghai Jiao Tong University
Qun Zhang: University of Science and Technology of China
Jianwen Jiang: National University of Singapore
Yu Han: Advanced Membranes and Porous Materials Center, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology (KAUST)
Anthony P. Davis: University of Bristol
Yong Cui: Shanghai Jiao Tong University

Nature, 2022, vol. 602, issue 7898, 606-611

Abstract: Abstract Two-dimensional materials with monolayer thickness and extreme aspect ratios are sought for their high surface areas and unusual physicochemical properties1. Liquid exfoliation is a straightforward and scalable means of accessing such materials2, but has been restricted to sheets maintained by strong covalent, coordination or ionic interactions3–10. The exfoliation of molecular crystals, in which repeat units are held together by weak non-covalent bonding, could generate a greatly expanded range of two-dimensional crystalline materials with diverse surfaces and structural features. However, at first sight, these weak forces would seem incapable of supporting such intrinsically fragile morphologies. Against this expectation, we show here that crystals composed of discrete supramolecular coordination complexes can be exfoliated by sonication to give free-standing monolayers approximately 2.3 nanometres thick with aspect ratios up to approximately 2,500:1, sustained purely by apolar intermolecular interactions. These nanosheets are characterized by atomic force microscopy and high-resolution transmission electron microscopy, confirming their crystallinity. The monolayers possess complex chiral surfaces derived partly from individual supramolecular coordination complex components but also from interactions with neighbours. In this respect, they represent a distinct type of material in which molecular components are all equally exposed to their environment, as if in solution, yet with properties arising from cooperation between molecules, because of crystallinity. This unusual nature is reflected in the molecular recognition properties of the materials, which bind carbohydrates with strongly enhanced enantiodiscrimination relative to individual molecules or bulk three-dimensional crystals.

Date: 2022
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DOI: 10.1038/s41586-022-04407-8

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