PDF(Pubmed)
Abstract：
Molecular logic gates are information processing devices that can respond to environmental signals and produce a readable output in response through Boolean logic operations. Molecules with these properties have been used to build smart sensors and therapeutic agents. In this work, dual enzyme-responsive molecular AND logic gate is developed with the intention to discriminate various combinations of enzyme level and/or activity. A resorufin-based sensor is substituted with self-immolative tyrosinase recognition site, 3-hydroxy benzyl group. The Hydroxyl group is protected with acetyl moiety which decreases the affinity of the enzyme. When both tyrosinase and esterase are present in the solution, the acetyl group is removed by the latter enzyme, allowing the former to recognise the ligand. Oxidation of the ligand by tyrosinase triggers self-immolative cleavage of the substitution, leading to almost 70 fold enhancement in fluorescence. When single enzyme is applied, there is no significant change in the emission intensity overall, an AND logic gate is constructed. Selectivity and Michaelis-Menten kinetics of the sensor is analysed. Smart molecular probes can contribute to the research on the development of biosensors that can discriminate diseases having characteristic combinations of enzyme activities.
摘要：
分子逻辑门是信息处理设备，可以响应环境信号，并通过布尔逻辑运算产生可读输出。具有这些性质的分子已被用于构建智能传感器和治疗剂。在这项工作中,开发了双酶响应分子与逻辑门，旨在区分酶水平和/或活性的各种组合。基于间苯二酚的传感器被自分解酪氨酸酶识别位点取代，3-羟基苄基。羟基被乙酰基部分保护,这降低了酶的亲和力。当溶液中同时存在酪氨酸酶和酯酶时，乙酰基被后一种酶去除，允许前者识别配体。酪氨酸酶对配体的氧化引发了取代的自我消融裂解，导致荧光增强近70倍。当应用单一酶时，整体发射强度没有显著变化，构造AND逻辑门。分析了传感器的选择性和米氏-Menten动力学。智能分子探针可以有助于研究生物传感器的开发，该生物传感器可以区分具有酶活性特征组合的疾病。
