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光化学触发的DNA微滴凝聚层自主振荡pH调制瞬态组装/拆卸

Photochemically Triggered and Autonomous Oscillatory pH-Modulated Transient Assembly/Disassembly of DNA Microdroplet Coacervates.

作者信息

Qin Yunlong, Sohn Yang Sung, Li Xiang, Nechushtai Rachel, Zhang Junji, Tian He, Willner Itamar

机构信息

The Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, 91904, Israel.

The Institute of Life Science, The Hebrew University of Jerusalem, Jerusalem, 91904, Israel.

出版信息

Angew Chem Int Ed Engl. 2025 Jan 15;64(3):e202415550. doi: 10.1002/anie.202415550. Epub 2024 Nov 9.

DOI:10.1002/anie.202415550
PMID:39378022
Abstract

The assembly of pH-responsive DNA-based, phase-separated microdroplets (MDs) coacervates, consisting of frameworks composed of Y-shaped nucleic acid modules crosslinked by pH-responsive strands, is introduced. The phase-separated MDs reveal dynamic pH-stimulated switchable or oscillatory transient depletion and reformation. In one system, a photoisomerizable merocyanine/spiropyran photoacid is used for the light-induced pH switchable modulation of the reaction medium between the values pH=6.0-4.4. The dynamic transient photochemically-induced switchable depletion/reformation of phase-separated MDs, follows the rhythm of pH changes in solution. In a second system, the Landolt oscillatory reaction mixture pH 7.5→4.2→7.5 is applied to stimulate the oscillatory depletion/reformation of the MDs. The autonomous dynamic oscillation of the assembly/disassembly of the MDs follows the oscillating pH rhythm of the reaction medium.

摘要

本文介绍了基于pH响应的DNA相分离微滴(MDs)凝聚物的组装,其由通过pH响应链交联的Y形核酸模块组成的框架构成。相分离的MDs显示出动态pH刺激的可切换或振荡瞬态耗尽和重构。在一个系统中,使用光异构化部花青/螺吡喃光酸对反应介质进行光诱导的pH值在6.0 - 4.4之间的可切换调制。相分离MDs的动态瞬态光化学诱导的可切换耗尽/重构遵循溶液中pH变化的节奏。在第二个系统中,应用Landolt振荡反应混合物pH 7.5→4.2→7.5来刺激MDs的振荡耗尽/重构。MDs组装/拆卸的自主动态振荡遵循反应介质的振荡pH节奏。

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J Am Chem Soc. 2025 May 14;147(19):16141-16153. doi: 10.1021/jacs.5c00637. Epub 2025 Apr 30.