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 (<30 min) and satisfy specific requirements to advance multilayered film technology3,4,18. This study showcases the feasibility, necessity and unlimited opportunities to transform laboratory nanoscience into nanotechnology through systems engineering of self-assembly.
| Original language | English |
|---|---|
| Pages (from-to) | 724-731 |
| Number of pages | 8 |
| Journal | Nature |
| Volume | 623 |
| Issue number | 7988 |
| DOIs | |
| State | Published - Nov 23 2023 |
Funding
This work was funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under contract DE-AC02-05CH11231 (Organic\u2013Inorganic Nanocomposites KC3104). E.V. was supported by the Department of Defense through the National Defense Science and Engineering Graduate (NDSEG) Fellowship Program. J.J. was supported by a National Science Foundation Graduate Research Fellowship under grant no. DGE 1752814. H.D. and X.T. acknowledge support from the Laboratory Directed Research and Development (LDRD) programme under contract no. DE-AC02-05CH11231. Membrane fabrication for VOC and water-permeability testing was supported by the Defense Threat Reduction Agency under contract no. HDTRA1-22-1-0005. Part of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory, the Advanced Photon Source operated by the Argonne National Laboratory, under contract no. DE-AC02-06CH11357, the Advanced Light Source and the Molecular Foundry operated by the Lawrence Berkeley National Laboratory under contract no. DE-AC02-05CH11231. We thank A. Minor for providing access to the nanoindentation measurements.\u00A0Q.Z. thanks R. Ziegler and D. P. Jensen Jr. for technical assistance. This work was funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under contract DE-AC02-05CH11231 (Organic\u2013Inorganic Nanocomposites KC3104). E.V. was supported by the Department of Defense through the National Defense Science and Engineering Graduate (NDSEG) Fellowship Program. J.J. was supported by a National Science Foundation Graduate Research Fellowship under grant no. DGE 1752814. H.D. and X.T. acknowledge support from the Laboratory Directed Research and Development (LDRD) programme under contract no. DE-AC02-05CH11231. Membrane fabrication for VOC and water-permeability testing was supported by the Defense Threat Reduction Agency under contract no. HDTRA1-22-1-0005. Part of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory, the Advanced Photon Source operated by the Argonne National Laboratory, under contract no. DE-AC02-06CH11357, the Advanced Light Source and the Molecular Foundry operated by the Lawrence Berkeley National Laboratory under contract no. DE-AC02-05CH11231. We thank A. Minor for providing access to the nanoindentation measurements. Q.Z. thanks R. Ziegler and D. P. Jensen Jr. for technical assistance.