Han Qian, Shi Xueran, Cao Yingbo, Gu Tiance, Shen Yizhong, Wang Jing
School of Pharmacy, Key Laboratory of Innovative Drug Development and Evaluation, Hebei Medical University, Shijiazhuang 050017, Hebei, China.
Engineering Research Center of Bio-Process, Ministry of Education, School of Food & Biological Engineering, Hefei University of Technology, Hefei 230009, China.
Anal Chem. 2025 Jul 15;97(27):14584-14593. doi: 10.1021/acs.analchem.5c02016. Epub 2025 Jun 30.
Gel-type electrochemiluminescence (ECL) active materials have attracted attention in sensing applications, where solid-state flexible and robust-response gels are required. Herein, we report a 5,10,15,20-tetrakis(4-sulfonatophenyl) porphyrin-decorated sodium alginate hydrogel (TPPS-SA hydrogel) as a new-generation ECL cathode luminophore. TPPS-SA hydrogel was synthesized by a facile hydrogen bond interaction. Different from the ECL instability of raw water-soluble TPPS, the ECL emission of the TPPS-SA hydrogel with a space-confined effect gave constantly stable signals with peroxy-disulfate (SO) as an efficient coreactant. Furthermore, to address the inherent high electrical impedance of the SA hydrogel, carboxyl-functionalized multiwalled carbon nanotubes (MWCNTs-COOH) served as the conductive scaffold to significantly enhance the ECL performance of the TPPS-SA hydrogel. Targeting insufficient detection sensitivity of antibiotic resistance genes (ARGs), we developed a highly selective and sensitive ECL sensing platform to detect ARGs using MWCNTs-COOH-assisted TPPS-SA hydrogels as signal probes coupled with DNA walking machines for target amplification. The proposed ECL sensor demonstrated a low limit of detection (0.42 pM) and excellent selectivity, providing a reliable paradigm for the application of porphyrin-based hydrogels in ECL sensing analysis.
凝胶型电化学发光(ECL)活性材料在传感应用中受到关注,这类应用需要固态柔性且响应稳健的凝胶。在此,我们报道一种5,10,15,20-四(4-磺酸苯基)卟啉修饰的海藻酸钠水凝胶(TPPS-SA水凝胶)作为新一代ECL阴极发光体。TPPS-SA水凝胶通过简便的氢键相互作用合成。与原始水溶性TPPS的ECL不稳定性不同,具有空间限制效应的TPPS-SA水凝胶以过二硫酸盐(SO)作为有效共反应剂时能给出持续稳定的信号。此外,为解决SA水凝胶固有的高电阻抗问题,羧基功能化多壁碳纳米管(MWCNTs-COOH)用作导电支架以显著增强TPPS-SA水凝胶的ECL性能。针对抗生素抗性基因(ARGs)检测灵敏度不足的问题,我们开发了一种高选择性和灵敏的ECL传感平台,使用MWCNTs-COOH辅助的TPPS-SA水凝胶作为信号探针并结合DNA步行机进行目标放大来检测ARGs。所提出的ECL传感器展示出低检测限(0.42 pM)和优异的选择性,为基于卟啉的水凝胶在ECL传感分析中的应用提供了可靠范例。