Institute for Advanced Interdisciplinary Research, University of Jinan , Jinan, Shandong 250022, P. R. China.
School of Chemistry and Chemical Engineering, University of Jinan , Jinan, Shandong 250022, P. R. China.
ACS Appl Mater Interfaces. 2017 Nov 1;9(43):37839-37847. doi: 10.1021/acsami.7b12338. Epub 2017 Oct 17.
In this work, a chemiluminescence-driven collapsible greeting card-like photoelectrochemical lab-on-paper device (GPECD) with hollow channel was demonstrated, in which target-triggering cascade DNA amplification strategy was ingeniously introduced. The GPECD had the functions of reagents storage and signal collection, and the change of configuration could control fluidic path, reaction time and alterations in electrical connectivity. In addition, three-dimentional reduced graphene oxide affixed Au flower was in situ grown on paper cellulose fiber for achieving excellent conductivity and biocompatibility. The cascade DNA amplification strategy referred to the cyclic formation of target analog chain and its trigger action to hybridization chain reaction (HCR), leading to the formation of numerous hemin/G-quadruplex DNA mimic enzyme with the presence of hemin. Subjected to the catalysis of hemin/G-quadruplex, the strong chemiluminiscence of luminol-HO system was obtained, which then was used as internal light source to excite photoactive materials realizing the simplification of instrument. In this analyzing process, thrombin served as proof-of-concept, and the concentration of target was converted into the DNA signal output by the specific recognition of aptamer-protein and target analog chain recycling. The target analog chain was produced in quantity with the presence of target, which further triggered abundant HCR and introduced hemin/G-quadruplex into the system. The photocurrent signal was obtained after the nitrogen-doped carbon dots sensitized ZnO was stimulated by chemiluminescence. The proposed GPECD exhibited excellent specificity and sensitivity toward thrombin with a detection limit of 16.7 fM. This judiciously engineered GPECD paved a luciferous way for detecting other protein with trace amounts in bioanalysis and clinical biomedicine.
在这项工作中,展示了一种基于化学发光的可折叠贺卡式纸基光电化学实验室装置(GPECD),其中巧妙地引入了目标触发级联 DNA 扩增策略。GPECD 具有试剂储存和信号收集功能,其结构变化可以控制流体路径、反应时间和电连接的变化。此外,三维还原氧化石墨烯附着的 Au 花在纸纤维素纤维上原位生长,以实现优异的导电性和生物相容性。级联 DNA 扩增策略是指目标类似物链的循环形成及其对杂交链式反应(HCR)的触发作用,导致在血红素存在的情况下形成大量血红素/G-四链体 DNA 模拟酶。在血红素/G-四链体的催化下,获得了强化学发光的鲁米诺-HO 体系,然后将其用作内部光源来激发光活性材料,实现仪器的简化。在这个分析过程中,凝血酶被用作概念验证,目标的浓度通过适体-蛋白质和目标类似物链循环的特异性识别转化为 DNA 信号输出。存在目标时会大量产生目标类似物链,进一步触发大量 HCR,并将血红素/G-四链体引入系统。氮掺杂碳点敏化 ZnO 受到化学发光刺激后,获得光电流信号。所提出的 GPECD 对凝血酶表现出优异的特异性和灵敏度,检测限低至 16.7 fM。这种巧妙设计的 GPECD 为在生物分析和临床生物医学中检测其他痕量蛋白质铺平了道路。