| 王 存,张瑶瑶,张玉乾,许韶菡,龚涛,文容,廖宇航,杨怡萌,任彦荣.化学通报,2025,88(9):983-991. |
| 镧系铈配合物信号探针合成及microRNA-21高灵敏传感检测 |
| Synthesis of lanthanide cerium complex signal probe and detection of microRNA-21 with high sensitivity |
| 投稿时间：2025-03-16 修订日期：2025-06-06 |
| DOI： |
| 中文关键词: 铈双配体配合物 生物传感器 MicroRNA-21 催化发夹自组装 |
| 英文关键词:Cerium double ligand complex Biosensor MicroRNA-21 Catalytic hairpin assembly |
| 基金项目:国家自然科学基金项目(22204010)、重庆市自然科学基金研究项目(CSTB2022NSCQ-MSX1015)、重庆市教育委员会科学技术研究 重点项目(KJZD-K202501601)、重庆市博士后研究项目特别资助( 2022CQBSHTB3005)、重庆市自然科学基金创新发展联合基金 (CSTB2023NSCQ-LZX0171)和重庆市大学生创新训练计划立项项目(S202414388010)资助 |
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| 中文摘要: |
| 本文以2,2":6",2"-三联吡啶-4-羧酸（Hmctpy）和硫瑾（Thi）为有机配体，镧系Ce3+为金属配位中心，通过水热法合成了系列铈双配体配位化合物（Ce-dCOPs）电化学信号探针。电化学活性Thi分子直接以配体的形式结合到Ce-dCOPs中，避免了检测过程中信号分子的脱落，极大的提高了传感器的稳定性。此外，在一定电压扫描过程中，Ce3+会转化成Ce4+，Ce3+/Ce4+对Thi具有高效的催化活性，因此避免了检测底液中添加底物，减少了外界的干扰，增加了检测的准确。紧接着，原位将纳米金包裹到Ce-dCOP（AuNPs@Ce-dCOP）表面，克服配合物导电性差的缺点。最后，以AuNPs@Ce-dCOP为信号探针，催化发夹自组装（CHA）信号放大策略，本文成功构建了用于乳腺癌标志物microRNA-21（miRNA-21）高灵敏检测的生物传感器。在100.0 amol·L-1～1.0 nmol·L-1的浓度范围内，miRNA-21的检测限低至86.1 amol·L-1（S/N = 3）。实际样品血清中miRNA-21的回收率在99.96%～106.00%之间，表明本研究既为肿瘤标志物的检测提供了一个简单、有效的检测方法，也为电化学信号探针的合成提供了思路。 |
| 英文摘要: |
| In this paper, a series of cerium double-ligand coordination compounds (Ce-dCOPs) electrochemical signal probes have been synthesized by hydrothermal method using 2,2":6",2"–terpyridine-4-carboxylic acid (Hmctpy) and thionine (Thi) as organic ligands and lanthanide Ce3+ as metal coordination center. The electrochemically active Thi molecules are directly bound to the Ce-dCOPs in the form of ligands, which avoids the shedding of signal molecules during the detection process and significantly improves the stability of the sensor. In addition, Ce3+ will be converted into Ce4+ during a certain voltage scanning process, and Ce3+/Ce4+ has efficient catalytic activity on Thi, so the addition of substrates in the detection substrate is avoided, the external interference is reduced, and the detection accuracy is increased. Subsequently, gold nanoparticles were coated on the surface of Ce-dCOP (AuNPs@Ce-dCOP) in situ to overcome the poor electrical conductivity of the complex. Finally, using AuNPs@Ce-dCOP as the signal probe and catalytic hairpin assembly (CHA) signal amplification strategy, a biosensor for highly sensitive detection of breast cancer marker microRNA-21 (miRNA-21) was successfully constructed. In the concentration range of 100.0 amol·L-1 to 1.0 nmol·L-1, the detection limit of miRNA-21 was as low as 86.1 amol·L-1 (S/N = 3). The recovery rates of miRNA-21 in actual serum samples were 99.96%-106.00%, indicating that this study not only provides a simple, effective and accurate detection method for the detection of tumor markers, but also provides ideas for the synthesis of electrochemical signal probes. |
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