Abstract
Polymer dots (Pdots) have become a type of attractive illuminant for electrochemiluminescence (ECL). However, the low ECL efficiency severely limits their practicability. Here, we design a dual intramolecular resonance energy transfer (RET) mechanism with newly synthesized triple-component Pdots to achieve great ECL enhancement. This mechanism efficiently shortens the path of energy transmission, thus greatly promoting the ECL amplification by 380 and 31 times compared to systems with no and single RET, and results in a relative ECL efficiency of 23.1% (vs. 1mM Ru(bpy)32+). Using metal-organic frameworks to carry the triple-component Pdots, a highly luminescent probe is proposed. By integrating the probe with target-mediated enzymatic circulation amplification and DNA arrays, a highly sensitive ECL imaging method is designed for simultaneous visual analysis of two kinds of proteins, mucin 1 and human epidermal growth factor receptor 2, on living cells, which exhibited linear ranges of 1 pg mL-1 to 5 ng mL-1 and 5 pg mL-1 to 10 ng mL-1 with limits of detection of 1 pg mL-1 and 5 pg mL-1, respectively. The proposed strategy showed promising application in bioanalysis.
Highlights
IntroductionOwing to their good biocompatibility, low cellular toxicity, easy functionalization, high photostability, and size/surface-trap controlled luminescence, polymer dots (Pdots) have been widely applied as promising uorescent bioprobes in single particle tracing, biosensing and cellular labeling.[1,2,3,4,5,6] The electrochemiluminescence (ECL) of Pdots has attracted considerable attention due to their tunable optical and electrochemical properties.[7,8,9,10] the ECL application of Pdots, especially in ECL imaging that requires a higher luminescence intensity, is still a great challenge due to their relatively lower ECL efficiency and/or higher ECL potential than general inorganic emitters.[11,12]
To achieve excellent ECL performance, this work further screened optimal types of the acceptor and an appropriate ratio of D/A for the preparation of polymer dots (Pdots), and designed a dual resonance energy transfer (RET) (D1–A1/D2–A2) mechanism to overcome the bottleneck of Pdots in ECL efficiency
P4 was composed of more A1/D2 and less A2 compared to P1 and acted as the model of incomplete dual ECL–RET
Summary
Owing to their good biocompatibility, low cellular toxicity, easy functionalization, high photostability, and size/surface-trap controlled luminescence, polymer dots (Pdots) have been widely applied as promising uorescent bioprobes in single particle tracing, biosensing and cellular labeling.[1,2,3,4,5,6] The electrochemiluminescence (ECL) of Pdots has attracted considerable attention due to their tunable optical and electrochemical properties.[7,8,9,10] the ECL application of Pdots, especially in ECL imaging that requires a higher luminescence intensity, is still a great challenge due to their relatively lower ECL efficiency and/or higher ECL potential than general inorganic emitters.[11,12] Inspired by these results, in our previous work we synthesized two kinds of three-component Pdots with the same AIE-active moiety but different D–A structures containing carbazole and uorene, respectively, and proved the stronger electrondonating ability of the carbazole moiety with a lower ECL onset potential and higher intensity of ECL emission.[18] To achieve excellent ECL performance, this work further screened optimal types of the acceptor and an appropriate ratio of D/A for the preparation of Pdots, and designed a dual resonance energy transfer (RET) (D1–A1/D2–A2) mechanism to overcome the bottleneck of Pdots in ECL efficiency. The excellent performance of the proposed method indicates the promising application of the dual RET mechanism along with the triple-component Pdots in bioanalysis
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