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Conductive Covalent Organic Frameworks with Conductivity- and Pre-Reduction-Enhanced Electrochemiluminescence for Ultrasensitive Biosensor Construction
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-02-14 , DOI: 10.1021/acs.analchem.1c05436 Jin-Ling Zhang 1 , Li-Ying Yao 1 , Yang Yang 1 , Wen-Bin Liang 1 , Ruo Yuan 1 , Dong-Rong Xiao 1
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-02-14 , DOI: 10.1021/acs.analchem.1c05436 Jin-Ling Zhang 1 , Li-Ying Yao 1 , Yang Yang 1 , Wen-Bin Liang 1 , Ruo Yuan 1 , Dong-Rong Xiao 1
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Covalent organic frameworks (COFs) have attracted widespread attention in the electrochemiluminescence (ECL) field owing to their high load capacity of ECL luminophores and porous structures, but their ECL performance is still limited by the intrinsic poor conductivity (generally <10–8 S m–1). To address this shortcoming, we used 2,3,6,7,10,11-hexaaminotriphenylene (HATP) and 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) to synthesize a conductive COF (HHTP-HATP-COF, conductivity = 3.11 × 10–4 S m–1). Compared with HATP, HHTP, and low-conductive HHTP-DABZ-COF, HHTP-HATP-COF exhibited superior ECL performance, not only because HHTP-HATP-COF possessed massive ECL luminophores but also because its conductive porous framework accelerated charge transport in the whole framework and improved the utilization ratio of ECL luminophores. More interestingly, the ECL intensity of the HHTP-HATP-COF/S2O82– system was further improved after pre-reduction electrolysis due to the accumulation of HHTP-HATP-COF cation radicals. The experimental results showed that the ECL intensity of the HHTP-HATP-COF/S2O82– system after pre-reduction was about 1.64-, 3.96-, 6.88-, and 8.09-fold higher than those of HHTP-HATP-COF/S2O82–, HHTP-DABZ-COF/S2O82–, HHTP/S2O82–, and HATP/S2O82– systems, respectively. Considering the superior ECL property of the HHTP-HATP-COF/S2O82– system after pre-reduction, it was used as a high-efficient ECL beacon together with an aptamer/protein proximity binding-induced three-dimensional bipedal DNA walker to construct an ultrasensitive biosensor for thrombin detection, which displayed broad linearity (100 aM to 1 nM) with a detection limit of 62.1 aM. Overall, the work offered effective ways to increase ECL performance by the enhancement of conductivity and by the pre-reduction, proposing new ideas to design high-efficiency COF-based ECL materials and endowing conductive COFs with ECL biosensor application for the first time.
中文翻译：
用于超灵敏生物传感器构建的具有电导率和预还原增强电化学发光的导电共价有机框架
共价有机框架 (COF) 因其对 ECL 发光体和多孔结构的高负载能力而在电化学发光 (ECL) 领域引起了广泛关注，但其 ECL 性能仍受限于固有的低电导率（通常 <10 –8 S m –1 )。为了解决这个缺点，我们使用 2,3,6,7,10,11-六氨基苯并苯 (HATP) 和 2,3,6,7,10,11-六羟基苯并苯 (HHTP) 合成了导电 COF (HHTP-HATP- COF，电导率 = 3.11 × 10 –4 S m –1）。与 HATP、HHTP 和低导电性 HHTP-DABZ-COF 相比，HHTP-HATP-COF 表现出优异的 ECL 性能，这不仅是因为 HHTP-HATP-COF 拥有大量的 ECL 发光体，而且还因为其导电多孔框架加速了电荷传输。整个框架并提高了 ECL 发光体的利用率。更有趣的是，由于 HHTP-HATP-COF 阳离子自由基的积累，在预还原电解后，HHTP-HATP-COF/S 2 O 8 2-体系的 ECL 强度进一步提高。实验结果表明，预还原后HHTP-HATP-COF/S 2 O 8 2-体系的ECL强度分别比HHTP-HATP-高1.64-、3.96-、6.88-和8.09-倍。 COF/S2 O 8 2–、HHTP-DABZ-COF/S 2 O 8 2–、HHTP/S 2 O 8 2–和 HATP/S 2 O 8 2–系统。考虑到 HHTP-HATP-COF/S 2 O 8 2优越的 ECL 特性——在预还原后的系统中，它被用作高效的 ECL 信标，与适体/蛋白质邻近结合诱导的三维双足 DNA walker 一起构建了用于凝血酶检测的超灵敏生物传感器，其表现出广泛的线性（100 aM 至 1 nM)，检测限为 62.1 aM。总体而言，这项工作提供了通过提高电导率和预还原来提高 ECL 性能的有效途径，为设计基于 COF 的高效 ECL 材料提出了新思路，并首次赋予导电 COF 以 ECL 生物传感器应用。
更新日期：2022-02-14
中文翻译：
用于超灵敏生物传感器构建的具有电导率和预还原增强电化学发光的导电共价有机框架
共价有机框架 (COF) 因其对 ECL 发光体和多孔结构的高负载能力而在电化学发光 (ECL) 领域引起了广泛关注，但其 ECL 性能仍受限于固有的低电导率（通常 <10 –8 S m –1 )。为了解决这个缺点，我们使用 2,3,6,7,10,11-六氨基苯并苯 (HATP) 和 2,3,6,7,10,11-六羟基苯并苯 (HHTP) 合成了导电 COF (HHTP-HATP- COF，电导率 = 3.11 × 10 –4 S m –1）。与 HATP、HHTP 和低导电性 HHTP-DABZ-COF 相比，HHTP-HATP-COF 表现出优异的 ECL 性能，这不仅是因为 HHTP-HATP-COF 拥有大量的 ECL 发光体，而且还因为其导电多孔框架加速了电荷传输。整个框架并提高了 ECL 发光体的利用率。更有趣的是，由于 HHTP-HATP-COF 阳离子自由基的积累，在预还原电解后，HHTP-HATP-COF/S 2 O 8 2-体系的 ECL 强度进一步提高。实验结果表明，预还原后HHTP-HATP-COF/S 2 O 8 2-体系的ECL强度分别比HHTP-HATP-高1.64-、3.96-、6.88-和8.09-倍。 COF/S2 O 8 2–、HHTP-DABZ-COF/S 2 O 8 2–、HHTP/S 2 O 8 2–和 HATP/S 2 O 8 2–系统。考虑到 HHTP-HATP-COF/S 2 O 8 2优越的 ECL 特性——在预还原后的系统中，它被用作高效的 ECL 信标，与适体/蛋白质邻近结合诱导的三维双足 DNA walker 一起构建了用于凝血酶检测的超灵敏生物传感器，其表现出广泛的线性（100 aM 至 1 nM)，检测限为 62.1 aM。总体而言，这项工作提供了通过提高电导率和预还原来提高 ECL 性能的有效途径，为设计基于 COF 的高效 ECL 材料提出了新思路，并首次赋予导电 COF 以 ECL 生物传感器应用。
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