Hexagon AgNCs/PVP 结晶诱导阴极电化学发光增强 miRNA221 生物传感,Small

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Hexagon AgNCs/PVP 结晶诱导阴极电化学发光增强 miRNA221 生物传感
Small ( IF 13.0 ) Pub Date : 2022-12-30 , DOI: 10.1002/smll.202205607
Bin Wang _{1,

2} , Guangjie Wang ₃ , Jing Li ₄ , Xinling Liu ₁ , Nan Ni ₁ , Huilan Su ₁ , Mei Chen ₅ , Li Mao ₁

Affiliation

聚集诱导电化学发光 (AIECL) 有望成为合成高发光发射体和用于 ECL 分析的共反应物的有效策略，但是，合理控制电致发光强度仍然具有挑战性。低电导率和无定形分子构型是内在瓶颈。这项工作通过采用 Box-Behnken 设计的响应面计算模型来调节晶体聚集体，揭示了聚乙烯吡咯烷酮主链调节的银纳米晶 (AgNCs/PVP) 对近红外区域阴极 AIECL 特性的影响。电子顺磁共振波谱发现氢自由基（HO ^•_{) 主要的还原氧化 (RO) ECL 机制，AgNCs 在氧化石墨烯/过硫酸盐系统 (GO/S 2} O ₈²⁻ )中充当共反应加速器。_{理论计算和实验测量均证明，GO/S 2} O ₈²⁻中AgNCs 的ECL取决于原位电化学氧化Ag ⁺的浓度。结晶诱导增强型 ECL (CIECL) 的高效率源自 1) Ag ⁺加速 H2O ^•的有效电子转移，显着促进放射性跃迁，以及 2) 从 PVP 的富电子供体到电子的扭曲分子内电荷转移-Ag受体缺陷⁰限制非放射性跃迁。应用具有 CIECL 效应的 AgNCs/PVP 构建用于 miR-221 检测的超灵敏平台，检测限低于典型的 qPCR 方法7.47 × 10 ³ 拷贝 mL ^{-1 。}

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Hexagon AgNCs/PVP Crystallization Induced Cathode Electrochemiluminescence Enhancement for miRNA221 Biosensing

Aggredation-induced electrochemiluminescence (AIECL) promises an efficient strategy for synthesize highly luminescent emitter and co-reactant for ECL analysis, however, rational control of electrogenerated emission intensity is still challenging. The low electroconductivity and amorphous molecular configuration are intrinsic bottleneck. This work reveals the impact of polyvinyl pyrrolidone backbone regulated silver nanocrystallines (AgNCs/PVP) on the cathode AIECL properties in near infrared region, by employing the Box-Behnken designed response surface computation model to modulate crystal aggregates. Electron paramagnetic resonance spectroscopy discovered hydrogen radical (HO^•) dominant reductive-oxidative (R-O) ECL mechanism with AgNCs acting as the co-reaction accelerator in graphene oxide/persulfate system (GO/S₂O₈²⁻). Both theoretical calculation and experimental measurement testified that the ECL of AgNCs in GO/S₂O₈²⁻ dependent on the concentration of in situ electrochemical oxidized Ag⁺. The high efficiency of crystallization-induced enhanced ECL (CIECL) originates from 1) the effective electron transfer of Ag⁺ accelerated HO^• produce to notable promote radioactive transition, and 2) twisted intramolecular charge transfer from the electron-rich donor of PVP to electron-deficient receptor of Ag⁰ to restrict nonradioactive transition. The AgNCs/PVP with CIECL effect are applied to construct an ultrasensitive platform for miR-221 assay with a lower detection limit of 7.47 × 10³ copies mL⁻¹ than typical qPCR method.

更新日期：2022-12-30

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