Key Laboratory for Large-Format Battery Materials and System, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering , Huazhong University of Science and Technology , Wuhan , 430074 , P. R. China.
State Key Laboratory of Digital Manufacturing Equipment and Technology , Huazhong University of Science and Technology , Wuhan 430074 , P. R. China.
Anal Chem. 2019 Mar 19;91(6):3912-3920. doi: 10.1021/acs.analchem.8b04685. Epub 2019 Feb 22.
The precise monitoring of HS has aroused immense research interest in the biological and biomedical fields since it is exposed as a third endogenous gasotransmitter. Hence, there is an urgent requisite to explore an ultrasensitive and economical HS detection system. Herein, we report a simple strategy to configure an extremely sensitive electrochemical sensor with a 2D nanosheet-shaped layered double hydroxide (LDH) wrapped carbon nanotubes (CNTs) nanohybrid (CNTs@LDH), where a series of CNTs@CuMn-LDH nanohybrids with varied amounts of LDH nanosheets grafted on a conductive CNTs backbone has been synthesized via a facile coprecipitation approach. Taking advantage of the unique core-shell structure, the integrated electrochemically active CuMn-LDH nanosheets on the conductive CNTs scaffold, the maximum interfacial collaboration, and the superior specific surface area with a plethora of surface active sites and ultrathin LDH layers, the as-prepared CNTs@CuMn-LDH nanoarchitectures have exhibited superb electrocatalytic activity toward HS oxidation. Under the optimum conditions, the electrochemical sensor based on the CNTs@CuMn-LDH nanohybrid shows remarkable sensing performances for HS determination in terms of a wide linear range and a low detection limit of 0.3 nM (S/N = 3), high selectivity, reproducibility, and durability. With marvelous efficiency achieved, the proposed sensing platform has been practically used in in situ detection of abiotic HS efflux produced by sulfate reducing bacteria and real-time in vitro tracking of HS concentrations from live cells after being excreted by a stimulator which in turn might serve as early diseases diagnosis. Thus, our core-shell hybrid nanoarchitectures fabricated via structural integration strategy will open new horizons in material synthesis, biosensing systems, and clinical chemistry.
精确监测 HS 作为第三种内源性气体递质的出现，在生物和生物医学领域引起了极大的研究兴趣。因此，迫切需要探索一种超灵敏和经济的 HS 检测系统。在此，我们报告了一种简单的策略，通过一种简便的共沉淀方法，配置具有二维纳米片状层状双氢氧化物 (LDH) 包裹的碳纳米管 (CNT) 纳米杂化物 (CNTs@LDH) 的极其灵敏的电化学传感器。在此，通过一种简便的共沉淀方法，合成了一系列具有不同数量 LDH 纳米片接枝在导电 CNT 骨架上的 CNT@CuMn-LDH 纳米杂化物。利用独特的核壳结构、集成在导电 CNT 支架上的电化学活性 CuMn-LDH 纳米片、最大的界面协同作用以及具有丰富表面活性位点和超薄 LDH 层的卓越比表面积，所制备的 CNT@CuMn-LDH 纳米结构对 HS 氧化表现出出色的电催化活性。在最佳条件下，基于 CNT@CuMn-LDH 纳米杂化物的电化学传感器对 HS 测定表现出显著的传感性能，具有宽线性范围和低检测限为 0.3 nM（S/N = 3）、高选择性、重现性和耐用性。所提出的传感平台具有卓越的效率，已实际用于原位检测硫酸盐还原菌产生的非生物 HS 流出物，并实时跟踪刺激物排出后活细胞中 HS 浓度，这反过来可能作为早期疾病诊断。因此，我们通过结构集成策略制备的核壳杂化纳米结构将为材料合成、生物传感系统和临床化学开辟新的视野。
