Department of Pharmacy and Department of Radiology (The First Affiliated Hospital), Shantou University Medical College, Shantou, 515041, China.
Department of Pharmacy and Department of Radiology (The First Affiliated Hospital), Shantou University Medical College, Shantou, 515041, China.
Biosens Bioelectron. 2022 Nov 15;216:114622. doi: 10.1016/j.bios.2022.114622. Epub 2022 Aug 9.
To develop various biosensors, several 2D nanomaterials adsorb DNA probes (aptamers) via π-π stacking interactions. However, interference from DNA displacement by external non-targeted ligands has precluded their practical applications for specific detection and imaging at high protein concentrations. Metal coordination is an attractive strategy for biomolecular crosslinking and functional molecular self-assembly. Herein, a robust 2D biosensor nanoplatform was developed to enhance DNA adsorption and affinity using Mn-modified black phosphorus nanosheets (BPNS@Mn) via metal coordination. The Mn can simultaneously coordinate with the lone pair electrons (π bonds) of the BPNS and nucleotide bases to provide binding sites for DNA nucleobases on the BPNS surface, which greatly enhances the stability of the inner BPNS and improves DNA adsorption and affinity. The DNA adsorption mechanism of BPNS@Mn was also characterized, and is extensively discussed. Without any further modification, this BPNS@Mn/DNA biosensor specifically detected single-stranded DNA (linear range: 10-200 nM, detection limit: 5.76 nM) and thrombin (linear range: 20-180 nM, detection limit: 2.39 nM) in 100 nM bovine serum albumin solution. The nonspecific ligands in the environment did not affect the detection performance of the robust biosensor. In addition, the expression levels of microRNA-21 can be imaged and analyzed in living cells using this biosensor, which is consistent with the results of the polymerase chain reaction. This study highlights the potential of metal coordination in surface modification and provides new opportunities for biomedical applications of 2D nanomaterials with superior DNA-adsorption capacity, facilitating the development of biosensor design and nucleic acid/drug delivery.
为了开发各种生物传感器，几种二维纳米材料通过π-π 堆积相互作用吸附 DNA 探针（适配体）。然而，由于外部非靶向配体的 DNA 置换干扰，它们在高蛋白质浓度下的特定检测和成像中的实际应用受到了限制。金属配位是生物分子交联和功能分子自组装的一种有吸引力的策略。在此，通过金属配位，使用 Mn 修饰的黑磷纳米片（BPNS@Mn）开发了一种强大的二维生物传感器纳米平台，以增强 DNA 的吸附和亲和力。Mn 可以同时与 BPNS 的孤对电子（π 键）和核苷酸碱基配位，为 BPNS 表面上的 DNA 核苷酸碱基提供结合位点，这极大地增强了内 BPNS 的稳定性，并提高了 DNA 的吸附和亲和力。还对 BPNS@Mn 的 DNA 吸附机制进行了表征，并进行了广泛的讨论。无需进一步修饰，这种 BPNS@Mn/DNA 生物传感器可特异性检测单链 DNA（线性范围：10-200 nM，检测限：5.76 nM）和凝血酶（线性范围：20-180 nM，检测限：2.39 nM）在 100 nM 牛血清白蛋白溶液中。环境中的非特异性配体不会影响稳健生物传感器的检测性能。此外，还可以使用该生物传感器对活细胞中的 microRNA-21 表达水平进行成像和分析，这与聚合酶链反应的结果一致。这项研究强调了金属配位在表面修饰中的潜力，并为具有优异 DNA 吸附能力的二维纳米材料的生物医学应用提供了新的机会，促进了生物传感器设计和核酸/药物输送的发展。
