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This content will become publicly available on January 15, 2026

Title: Controlling the Spatiotemporal Self-Organization of Stimuli-Responsive Nanocrystals under Out-of-Equilibrium Conditions
Self-organization under out-of-equilibrium conditions is ubiquitous in natural systems for the generation of hierarchical solid-state patterns of complex structures with intricate properties. Efforts in applying this strategy to synthetic materials that mimic biological function have resulted in remarkable demonstrations of programmable self-healing and adaptive materials. However, the extension of these efforts to multifunctional stimuli-responsive solidstate materials across defined spatial distributions remains an unrealized technological opportunity. This paper describes the use of a nonequilibrium reaction−diffusion process to achieve the synthesis of a multifunctional stimuli-responsive electrically conductive metal−organic framework (cMOF) in a gelled medium with control over particle size and spatial periodicity on a macroscopic scale. Upon integration into chemiresistive devices, the resulting cMOF particles exhibit a size-dependent response toward hydrogen sulfide gas, as determined by their distinct surface-to-volume ratio, porosity, unique synthesis methodology, and unusual microcrystallite morphology compared to their counterparts obtained through bulk solution phase synthesis. Taken altogether, these achievements pave the way toward gaining access to functional nanomaterials with well-defined chemical composition, dimensions, and precisely tailored functions using far-from-equilibrium approaches.  more » « less
Award ID(s):
1945218 2125733
PAR ID:
10614543
Author(s) / Creator(s):
; ;
Publisher / Repository:
Journal of the American Chemical Society
Date Published:
Journal Name:
Journal of the American Chemical Society
Volume:
147
Issue:
2
ISSN:
0002-7863
Page Range / eLocation ID:
1584 to 1594
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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