Functional composites by programming entropy-driven nanosheet growth

Emma Vargo, Le Ma, He Li, Qingteng Zhang, Junpyo Kwon, Katherine M. Evans, Xiaochen Tang, Victoria L. Tovmasyan, Jasmine Jan, Ana C. Arias, Hugo Destaillats, Ivan Kuzmenko, Jan Ilavsky, Wei-Ren Chen, William Heller, Robert O. Ritchie, Yi Liu and Ting Xu ()
Additional contact information
Emma Vargo: University of California, Berkeley
Le Ma: University of California, Berkeley
He Li: Lawrence Berkeley National Laboratory
Qingteng Zhang: Argonne National Laboratory
Junpyo Kwon: Lawrence Berkeley National Laboratory
Katherine M. Evans: University of California, Berkeley
Xiaochen Tang: Lawrence Berkeley National Laboratory
Victoria L. Tovmasyan: University of California, Berkeley
Jasmine Jan: University of California, Berkeley
Ana C. Arias: University of California, Berkeley
Hugo Destaillats: Lawrence Berkeley National Laboratory
Ivan Kuzmenko: Argonne National Laboratory
Jan Ilavsky: Argonne National Laboratory
Wei-Ren Chen: Oak Ridge National Laboratory
William Heller: Oak Ridge National Laboratory
Robert O. Ritchie: University of California, Berkeley
Yi Liu: Lawrence Berkeley National Laboratory
Ting Xu: University of California, Berkeley

Nature, 2023, vol. 623, issue 7988, 724-731

Abstract: Abstract Nanomaterials must be systematically designed to be technologically viable1–5. Driven by optimizing intermolecular interactions, current designs are too rigid to plug in new chemical functionalities and cannot mitigate condition differences during integration6,7. Despite extensive optimization of building blocks and treatments, accessing nanostructures with the required feature sizes and chemistries is difficult. Programming their growth across the nano-to-macro hierarchy also remains challenging, if not impossible8–13. To address these limitations, we should shift to entropy-driven assemblies to gain design flexibility, as seen in high-entropy alloys, and program nanomaterial growth to kinetically match target feature sizes to the mobility of the system during processing14–17. Here, following a micro-then-nano growth sequence in ternary composite blends composed of block-copolymer-based supramolecules, small molecules and nanoparticles, we successfully fabricate high-performance barrier materials composed of more than 200 stacked nanosheets (125 nm sheet thickness) with a defect density less than 0.056 µm−2 and about 98% efficiency in controlling the defect type. Contrary to common perception, polymer-chain entanglements are advantageous to realize long-range order, accelerate the fabrication process (

Date: 2023
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DOI: 10.1038/s41586-023-06660-x

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