Journal
SCIENCE ADVANCES
Volume 6, Issue 33, Pages -Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.abb5976
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Funding
- German Research Foundation (DFG)
- Ministry of Science, Research and the Arts (MWK) of Baden-Wuerttemberg (DFG) [KA 1295/21-1]
- EU Graphene Flagship
- DFG [CRC 1279, 426572620, SFB-1415, 417590517]
- ERC [819698, 852909, 639233]
- EU Graphene Flagship [785219]
- COORNET [SPP 1928]
- CONJUGATION [706082]
- German Science Council, Center for Advancing Electronics Dresden (cfaed) [EXC1056, OR 349/1]
- Alexander von Humboldt Foundation
- German Excellence Initiative via the Cluster of Excellence cfaed [EXC 1056]
- EU Framework Programme for Research and Innovation HORIZON 2020 [730872]
- Cluster of Excellence e-conversion
- National Natural Science Foundation of China [51873236, 51833011]
- Youth 1000 Talent Program of China
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Two-dimensional (2D) polymers, hold great promise in the rational materials design tailored for next-generation applications. However, little is known about the grain boundaries in 2D polymers, not to mention their formation mechanisms and potential influences on the material's functionalities. Using aberration-corrected high-resolution transmission electron microscopy, we present a direct observation of the grain boundaries in a layer-stacked 2D polyimine with a resolution of 2.3 angstrom, shedding light on their formation mechanisms. We found that the polyimine growth followed a birth-and-spread mechanism. Antiphase boundaries implemented a self-correction to the missing-linker and missing-node defects, and tilt boundaries were formed via grain coalescence. Notably, we identified grain boundary reconstructions featuring closed rings at tilt boundaries. Quantum mechanical calculations revealed that boundary reconstruction is energetically allowed and can be generalized into different 2D polymer systems. We envisage that these results may open up the opportunity for future investigations on defect-property correlations in 2D polymers.
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