Shear Stress-Responsive Polymersome Nanoreactors Inspired by the Marine Bioluminescence of Dinoflagellates.

Shear Stress-Responsive Polymersome Nanoreactors Inspired by the Marine Bioluminescence of Dinoflagellates.
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DOI:
10.1002/anie.202010099
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发表时间:
2021-01-11
期刊:
Angewandte Chemie (International ed. in English)
影响因子:
--
通讯作者:
Bruns N
Bruns N
中科院分区:
其他
文献类型:
--
作者:
Rifaie-Graham O;Galensowske NFB;Dean C;Pollard J;Balog S;Gouveia MG;Chami M;Vian A;Amstad E;Lattuada M;Bruns N

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一些被称为甲藻的海洋浮游生物会随着周围海水的运动而发光,导致一种被称为乳白色海洋或海洋闪光的现象。基本的概念,剪应力诱导的生物催化反应室的渗透性,转移到聚合物为基础的纳米反应器。两亲性嵌段共聚物在其疏水嵌段中携带核碱基,自组装成聚合体。通过在流动中或在聚合物分散体的湍流混合期间发生的剪切力,囊泡的膜可以在不透水和半透水状态之间瞬时切换。当施加机械力时,疏水小叶中的碱基对分离,暴露出它们的氢键基序,从而使膜不那么疏水,对水溶性化合物更具渗透性。该极性开关用于根据需要释放聚合体的有效载荷,并激活聚合体内部的生物催化反应。当施加剪切力时,在其膜上具有核碱基对的聚合体对底物变得瞬时渗透。这些力响应型聚合体允许通过囊泡分散体的湍流混合来开启酶反应,这在比色反应和化学发光反应以及水凝胶的固化中得到了证明。
Some marine plankton called dinoflagellates emit light in response to the movement of surrounding water, resulting in a phenomenon called milky seas or sea sparkle. The underlying concept, a shear‐stress induced permeabilisation of biocatalytic reaction compartments, is transferred to polymer‐based nanoreactors. Amphiphilic block copolymers that carry nucleobases in their hydrophobic block are self‐assembled into polymersomes. The membrane of the vesicles can be transiently switched between an impermeable and a semipermeable state by shear forces occurring in flow or during turbulent mixing of polymersome dispersions. Nucleobase pairs in the hydrophobic leaflet separate when mechanical force is applied, exposing their hydrogen bonding motifs and therefore making the membrane less hydrophobic and more permeable for water soluble compounds. This polarity switch is used to release payload of the polymersomes on demand, and to activate biocatalytic reactions in the interior of the polymersomes. Polymersomes with nucleobase pairs in their membrane become transiently permeable for substrates when shear forces are applied. These force‐responsive polymersomes allow to switch on enzymatic reactions by turbulent mixing of vesicle dispersions, which is demonstrated with colorimetric and chemoluminescent reactions, as well as the curing of hydrogels.
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