Photoelectrochemical sensor based on AuNPs@WO₃@TpPa-1-COF for quantification of DNA methylation levels

作者全名："Liu, Huamin; Li, Chenghong; Wang, Lina; Fang, Lichao; Huang, Hui; Deng, Jun; Hu, Yue; Li, Mimi; Ran, Xiaoping; Li, Lulu; Zheng, Junsong"

作者地址："[Liu, Huamin; Li, Chenghong; Wang, Lina; Fang, Lichao; Huang, Hui; Deng, Jun; Ran, Xiaoping; Li, Lulu; Zheng, Junsong] Army Med Univ, Coll Med Lab Sci, Dept Clin & Mil Lab Med, Chongqing 400038, Peoples R China; [Hu, Yue; Li, Mimi] Chongqing Med Univ, Emergency Dept, Affiliated Hosp, Chongqing 400010, Peoples R China"

通信作者："Zheng, JS (通讯作者)，Army Med Univ, Coll Med Lab Sci, Dept Clin & Mil Lab Med, Chongqing 400038, Peoples R China."

来源：MICROCHIMICA ACTA

ESI学科分类：CHEMISTRY

WOS号：WOS:001173206100003

JCR分区：Q1

影响因子：5.7

年份：2024

卷号：191

期号：3

开始页：　

结束页：　

文献类型：Article

关键词：5-Methylcytosine; Photoactive material; P-N-type quenching; Photoelectochemical biosensor

摘要："A ""signal-off"" photoelectrochemical (PEC) sensing platform has been designed for the ultrasensitive detection of DNA methylation levels and multiple methylated sites. The platform employs tungsten trioxide and TpPa-1-COF loaded by gold nanoparticle (AuNPs@WO3@TpPa-1-COF) composite material as the photoactive component and p-type reduced graphene (rGO) as an efficient quencher. The PEC signal of AuNPs@WO3@TpPa-1-COF composite is effectively quenched in the presence of p-type rGO, because p-type rGO can compete with AuNPs@WO3@TpPa-1-COF to deplete light energy and electron donors. In addition, a hybrid strand reaction (HCR) amplification strategy fixes more target DNA and then combines with rGO-modified anti-5-methylcytosine antibody to facilitate ultrasensitive DNA methylation detection. Under optimal conditions, DNA methylation can be measured within a linear concentration range of 10(-14) to 10(-8) M, with an exceptionally low detection limit of 0.19 fM (S/N = 3). At the same time, the platform can conduct quantitative determination of multi-site methylation, with the linear equation triangle I = 44.19LogA + 61.43, and the maximum number of methylation sites is 5. The sensor demonstrates high sensitivity, excellent selectivity, and satisfactory stability. Furthermore, the proposed signal-off PEC strategy was successfully employed to detect DNA methylation in spiked human serum samples, with recoveries ranging from 93.17 to 107.28% and relative standard deviation (RSD) ranging from 1.15 to 5.49%."

基金机构："National Natural Science Foundation of China [82272430, 81873982, 82003109]; Special Project of Scientific and Technological Innovation Capability Improvement of the Army Military Medical University [2022XQN04, 2021XQN03]; Special Support from the Chongqing Postdoctoral Research Project [2021XM1018]"

基金资助正文："Financial support for this work was provided by the National Natural Science Foundation of China (No. 82272430, No. 81873982, and No. 82003109), Special Project of Scientific and Technological Innovation Capability Improvement of the Army Military Medical University (No. 2022XQN04 and No. 2021XQN03), and Special Support from the Chongqing Postdoctoral Research Project (No. 2021XM1018)."