Transmembrane signal transduction by cofactor transport.
Transmembrane signal transduction by cofactor transport.
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DOI：
10.1039/d1sc03910e
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发表时间：
2021-09-29
期刊：
影响因子：
8.4
通讯作者：
Hunter CA
中科院分区：
文献类型：
--
作者：
Kocsis I;Ding Y;Williams NH;Hunter CA
生物系统中的信息处理和细胞信号传导依赖于通过脂质双层膜传递化学信号，但能够实现这一过程的合成系统的例子很少。已经开发了一种合成换能器，其响应于向外部囊泡溶液中加入金属离子而触发脂囊泡内酯底物的催化水解。在囊泡的内部隔室中产生的输出信号通过将金属离子辅因子结合到换能器上的头基以形成催化活性复合物来产生。信号转导的机制是基于跨双分子层的金属离子辅因子的传输的换能器，和系统可以可逆地切换之间的开和关状态，分别通过添加镉（II）和乙二胺四羧酸输入信号。换能器还配备有酰肼部分，其允许通过与醛的共价缀合来调节活性。共轭与糖衍生物废除活动，因为所得的腙是太极性的双分子层，而共轭与吡啶衍生物增加活动。耦合传输与催化提供了一个简单的机制，产生复杂的系统使用简单的组件。合成的转换器将外部添加的金属离子辅因子运输穿过囊泡的脂质双层膜，以触发内室中酯水解的催化。信号转导活性受腙形成的调节。
Information processing and cell signalling in biological systems relies on passing chemical signals across lipid bilayer membranes, but examples of synthetic systems that can achieve this process are rare. A synthetic transducer has been developed that triggers catalytic hydrolysis of an ester substrate inside lipid vesicles in response to addition of metal ions to the external vesicle solution. The output signal generated in the internal compartment of the vesicles is produced by binding of a metal ion cofactor to a head group on the transducer to form a catalytically competent complex. The mechanism of signal transduction is based on transport of the metal ion cofactor across the bilayer by the transducer, and the system can be reversibly switched between on and off states by adding cadmium(ii) and ethylene diamine tetracarboxylic acid input signals respectively. The transducer is also equipped with a hydrazide moiety, which allows modulation of activity through covalent conjugation with aldehydes. Conjugation with a sugar derivative abolished activity, because the resulting hydrazone is too polar to cross the bilayer, whereas conjugation with a pyridine derivative increased activity. Coupling transport with catalysis provides a straightforward mechanism for generating complex systems using simple components. Synthetic transducers transport externally added metal ion cofactors across the lipid bilayer membrane of vesicles to trigger catalysis of ester hydrolysis in the inner compartment. Signal transduction activity is modulated by hydrazone formation.
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