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有机催化剂的化学信号激活能够控制软材料的形成。

Chemical signal activation of an organocatalyst enables control over soft material formation.

作者信息

Trausel Fanny, Maity Chandan, Poolman Jos M, Kouwenberg D S J, Versluis Frank, van Esch Jan H, Eelkema Rienk

机构信息

Department of Chemical Engineering, Delft University of Technology, van der Maasweg 9, Delft, 2629, HZ, The Netherlands.

出版信息

Nat Commun. 2017 Oct 12;8(1):879. doi: 10.1038/s41467-017-00998-3.

Abstract

Cells can react to their environment by changing the activity of enzymes in response to specific chemical signals. Artificial catalysts capable of being activated by chemical signals are rare, but of interest for creating autonomously responsive materials. We present an organocatalyst that is activated by a chemical signal, enabling temporal control over reaction rates and the formation of materials. Using self-immolative chemistry, we design a deactivated aniline organocatalyst that is activated by the chemical signal hydrogen peroxide and catalyses hydrazone formation. Upon activation of the catalyst, the rate of hydrazone formation increases 10-fold almost instantly. The responsive organocatalyst enables temporal control over the formation of gels featuring hydrazone bonds. The generic design should enable the use of a large range of triggers and organocatalysts, and appears a promising method for the introduction of signal response in materials, constituting a first step towards achieving communication between artificial chemical systems.Enzymes regulated by chemical signals are common in biology, but few such artificial catalysts exist. Here, the authors design an aniline catalyst that, when activated by a chemical trigger, catalyses formation of hydrazone-based gels, demonstrating signal response in a soft material.

摘要

细胞能够通过改变酶的活性来响应特定化学信号,从而对其环境做出反应。能够被化学信号激活的人工催化剂很少见,但对于制造自主响应材料而言却很有意义。我们展示了一种能被化学信号激活的有机催化剂,它能实现对反应速率和材料形成的时间控制。利用自牺牲化学,我们设计了一种失活的苯胺有机催化剂,它能被化学信号过氧化氢激活,并催化腙的形成。催化剂一旦被激活,腙的形成速率几乎瞬间增加10倍。这种响应性有机催化剂能够对具有腙键的凝胶的形成进行时间控制。这种通用设计应能使人们使用多种触发因素和有机催化剂,并且似乎是一种在材料中引入信号响应的很有前景的方法,是朝着实现人工化学系统之间通信迈出的第一步。受化学信号调节的酶在生物学中很常见,但这类人工催化剂却很少。在此,作者设计了一种苯胺催化剂,当被化学触发因素激活时,它能催化基于腙的凝胶的形成,证明了在软材料中的信号响应。

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