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1.
J Am Chem Soc ; 146(5): 3323-3330, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38273768

RESUMO

In living organisms, precise control over the spatial and temporal distribution of molecules, including pheromones, is crucial. This level of control is equally important for the development of artificial active materials. In this study, we successfully controlled the distribution of small molecules in the system at nonequilibrium states by actively transporting them, even against the apparent concentration gradient, with high selectivity. As a demonstration, in the aqueous solution of acid orange (AO7) and TMC10COOH, we found that AO7 molecules can coassemble with transient anhydride (TMC10CO)2O to form larger assemblies in the presence of chemical fuel 1-ethyl-3-(3-(dimethylamino)propyl) carbodiimide hydrochloride (EDC). This led to a decrease in local free AO7 concentration and caused AO7 molecules from other locations in the solution to move toward the assemblies. Consequently, AO7 accumulates at the location where EDC was injected. By continuously injecting EDC, we could maintain a stable high value of the apparent AO7 concentration at the injection point. We also observed that this process which operated at nonequilibrium states exhibited high selectivity.

2.
Chem Sci ; 14(12): 3363-3369, 2023 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-36970082

RESUMO

Energy input plays a crucial role in the assembling of matter. In our present study, we utilize EDC as a chemical fuel to drive the molecular assembling of POR-COOH. POR-COOH will react with EDC to generate the intermediate POR-COOEDC first, which was well-solvated by solvent molecules. During the subsequent hydrolysis process, EDU and oversaturated POR-COOH molecules at high energy states will be formed and thus allowed the self-assembling of POR-COOH into 2D nanosheets. This chemical energy assisted assembling process could be performed not only under mild conditions with high spatial accuracy but also with high selectivity in complex environments.

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