Electrochemical luminescence system for enhancing gold nanocluster based on double co-reactants
By using a water-soluble Zn2+ aggregation-induced dual co-reactant system with triethanolamine and borane-tert-butylamine complex as dual co-reactants, the electrochemiluminescence intensity and emission wavelength of gold nanoclusters were successfully improved, solving the problem of insufficient electrochemiluminescence intensity in existing technologies and broadening their application range.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2025-11-26
- Publication Date
- 2026-04-03
AI Technical Summary
In the existing technology, the electrochemiluminescence system of gold nanoclusters is mainly based on single co-reactant, while the research on dual co-reactant system is relatively limited, resulting in insufficient electrochemiluminescence intensity and restricting its application in the field of medical detection.
A water-soluble Zn2+ aggregation-induced dual co-reactant system was adopted, using triethanolamine and borane-tert-butylamine complex as dual co-reactants, to enhance the electrochemiluminescence of gold nanoclusters under buffer solution conditions, with a maximum emission wavelength greater than 850 nm.
Compared to single co-reactant systems, the electrochemiluminescence intensity was increased by 4-6 times, the emission wavelength was broadened to the near-infrared region, and the electrochemiluminescence application potential of gold nanoclusters was enhanced.
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Abstract
Description
Technical Field
[0001] This invention relates to an electrochemiluminescence system based on dual co-reactant-enhanced gold nanoclusters, belonging to the field of electrochemiluminescence technology. Background Technology
[0002] Since Bard's group first reported the electrochemiluminescence of Si nanoparticles in 2002 (Science 2002, 296, 1293), a series of advances have been made in the electrochemiluminescence of quantum dot-based nanomaterials, represented by II-VI quantum dots (Chem. Rev. 2014, 114, 11027). II-VI quantum dots often contain toxic elements, posing potential environmental and biological toxicity risks. The electrochemiluminescence of biocompatible metal nanoparticles such as gold, silver, and copper is attracting widespread attention. Gold nanoclusters-based ECL radiation systems, which achieve higher electrochemiluminescence efficiency, have also garnered significant interest. Yang et al. discovered that forming rigid conjugated structures on the surface of metal nanoclusters can significantly enhance the electrochemiluminescence of gold nanoclusters. The electrochemiluminescence of the prepared gold nanoclusters is located in the visible light region, with a maximum radiation wavelength of 532 nm (Angew. Chem. Int. Ed. 2019, 58, 6901). Traditional electrochemiluminescence systems are mainly based on single co-reactant structures, with very little research on dual co-reactant systems. The development of related methods and technologies is of significant academic value for enhancing the electrochemiluminescence intensity of gold nanoclusters and improving their application in medical detection, with broad application prospects. Summary of the Invention
[0003] To address the shortcomings of existing technologies, this invention provides an electrochemiluminescence system based on dual co-reactant-enhanced gold nanoclusters.
[0004] The electrochemiluminescence system of this invention uses water-soluble Zn 2+ Aggregation-induced dual co-reactant enhances gold nanoclusters as luminescent organisms. Triethanolamine and borane-tert-butylamine complexes serve as dual co-reactants, generating near-infrared electrochemiluminescence in the long-wavelength region under buffer solution conditions. This enhancement is 4-6 times greater than that of single co-reactant systems, with a maximum emission wavelength greater than 850 nm.
[0005] The technical solution of the present invention is as follows: An electrochemiluminescence system based on dual co-reactant enhanced gold nanoclusters, the luminescence system using water-soluble Zn 2+ Aggregation-induced dual co-reactant enhancement of gold nanoclusters as luminescent organisms, with triethanolamine and borane-tert-butylamine complex as dual co-reactants, produces near-infrared electrochemiluminescence in the long-wavelength region under buffer conditions, which is 4-6 times stronger than that of the single co-reactant system, and its maximum emission wavelength is greater than 850 nm.
[0006] According to a preferred embodiment of the present invention, water-soluble Zn 2+ Aggregation-induced dual co-reactant enhanced gold nanoclusters were prepared by the following method: (1) Add 11-mercaptoundecanoic acid and D-penicillamine to deionized water, then add H4AuCl4, and mix evenly by ultrasonication to obtain mixture a; (2) Add zinc acetate and borane-tert-butylamine complex to the mixture a in step (1) and mix evenly by ultrasonication to obtain mixture b; (3) Mixture b was stirred at room temperature to react. The resulting solution was purified by centrifugation with isopropanol, and the precipitate was water-soluble Zn. 2+ Aggregation-induced dual co-reactant enhances gold nanoclusters.
[0007] This invention is based on Zn 2+ Aggregation-induced reduction of Au was achieved through the online reduction of 11-mercaptoundecanoic acid and D-penicillamine, which acted as short / long chain dual stabilizers. + The principle and method were used to successfully prepare Zn 2+ Aggregation-induced dual co-reactant enhances gold nanoclusters.
[0008] According to the present invention, preferably, in step (1), the molar ratio of H4AuCl4 to 11-mercaptoundecanoic acid is 10000:(1-5), and more preferably, the molar ratio of H4AuCl4 to 11-mercaptoundecanoic acid is 10000:1.
[0009] According to the present invention, preferably, in step (1), the molar ratio of H4AuCl4 to D-penicillamine is 500:(1-5), and more preferably, the molar ratio of H4AuCl4 to D-penicillamine is 500:2.
[0010] According to the present invention, preferably, in step (1), the concentration of H4AuCl4 in mixture a is 80-120 mM, the concentration of 11-mercaptoundecanoic acid is 4-8 μM, and the concentration of D-penicillamine is 5-10 μM.
[0011] According to the present invention, preferably, in step (2), the molar ratio of zinc acetate to H4AuCl4 in step (1) is (1-5):10000, and more preferably, the molar ratio of zinc acetate to H4AuCl4 in step (1) is 1:10526.
[0012] According to the present invention, preferably, in step (2), the molar ratio of the borane-tert-butylamine complex to H4AuCl4 is (1-5):1000, and more preferably, the molar ratio of the borane-tert-butylamine complex to H4AuCl4 is 1:1000.
[0013] According to the present invention, preferably, in step (2), the concentration of zinc acetate in mixture b is 0.2-1 μM, and the concentration of the borane-tert-butylamine complex is 1-10 μM.
[0014] According to the present invention, preferably, in step (3), the stirring time is 12-36 hours, and more preferably, the stirring time is 24 hours.
[0015] According to a preferred embodiment of the present invention, water-soluble Zn 2+ Aggregation-induced dual co-reactant enhanced gold nanoclusters were prepared by the following method: 1) Add the ligands D-penicillamine and 11-mercaptoundecanoic acid to 3.2 mL of deionized water to make the concentration of D-penicillamine 6.25 μM and the concentration of 11-mercaptoundecanoic acid 6.25 μM. Then, add 100 μL of HAuCl4·H2O to the above solution to make the concentration of HAuCl4·H2O 100 mM. Adjust the pH to 3.0 with stirring to obtain a mixed solution. 2) The borane-tert-butylamine complex and zinc acetate were added dropwise to the mixture from step 1), bringing the concentration of the borane-tert-butylamine complex to 7.5 μM and the concentration of zinc acetate to 0.425 μM. The mixture was stirred at 1500 rpm / min for one day. After adding the reducing agent, the color of the reaction solution changed from colorless to brown; the resulting solution contained Zn 2+ -DPA / MUA@AuNCs were precipitated with isopropanol, and excess ligands were removed by centrifugation. Then, the solid sample was dissolved in ultrapure water to obtain a 2 mg / mL gold nanocluster solution for later use.
[0016] Zn prepared by this invention 2+ Solid samples of -DPA / MUA@AuNCs can be safely stored in a refrigerator for more than one month.
[0017] According to a preferred embodiment of the present invention, in the electrochemiluminescence system, water-soluble Zn 2+ The concentration of aggregation-inducing dual co-reactant to enhance gold nanoclusters is 1-5 mg / mL.
[0018] According to a preferred embodiment of the present invention, the concentration of the dual co-reactant in the electrochemiluminescence system is 8-25 mM.
[0019] According to a preferred embodiment of the present invention, the molar concentration of triethanolamine in the electrochemiluminescence system is 4-10 mM.
[0020] According to a preferred embodiment of the present invention, the molar concentration of the borane-tert-butylamine complex in the electrochemiluminescence system is 4-15 mM.
[0021] According to a preferred embodiment of the present invention, in the electrochemiluminescence system, the buffer solution is one of the following: phosphate buffer solution, carbonate buffer solution, borate buffer solution, acetate buffer solution, hepes buffer solution, and tris-HCl buffer solution.
[0022] According to a preferred embodiment of the present invention, in the electrochemiluminescence system, the buffer solution is a phosphate buffer solution with a concentration of 0.1-0.5M and a pH value of 5-10.
[0023] The construction method of the electrochemiluminescence system based on dual co-reactant enhanced gold nanoclusters described above includes the following steps: Water-soluble Zn 2+ Aggregation-induced dual co-reactant-enhanced gold nanoclusters were used as luminescent agents, and triethanolamine and borane-tert-butylamine complexes were used as dual co-reactants. In the presence of buffer solution, a dual co-reactant-type electrochemiluminescence system was formed. A three-electrode system and cyclic voltammetry were used to drive the electrochemiluminescence radiation of a dual co-reactant electrochemiluminescence system.
[0024] Technical features and advantages of the present invention: 1. This invention is based on Zn 2+ Aggregation-induced reduction of Au was achieved through the online reduction of 11-mercaptoundecanoic acid and D-penicillamine, which acted as short / long chain dual stabilizers. + The principle and method were used to successfully prepare Zn 2+ Aggregation-induced dual co-reactant enhancement of gold nanoclusters. The resulting gold nanoclusters exhibit good stability. When triethanolamine or borane-tert-butylamine complex is used as a single co-reactant, the electrochemiluminescence signal is weak. However, when triethanolamine and borane-tert-butylamine complex are used as dual co-reactants, the electrochemiluminescence intensity is increased by approximately 4.7 times, and near-infrared electrochemiluminescence with a maximum radiation wavelength greater than 850 nm is generated.
[0025] 2. The electrochemiluminescence system of the present invention generates electrochemiluminescence radiation in the near-infrared region in an aqueous system. Compared with the single co-reactant electrochemiluminescence system, its electrochemiluminescence radiation is enhanced by 4.7 times, and its maximum radiation wavelength is greater than 800 nanometers. This broadens the types of dual co-reactant systems, promotes the application of gold nanoclusters to enhance electrochemiluminescence, and the steps are simple, the conditions are mild, and the operation is safe. Attached Figure Description
[0026] Figure 1 Zn prepared in Example 1 2+ Aggregation-induced dual co-reactant enhances fluorescence excitation and emission of gold nanoclusters, UV spectrum.
[0027] Figure 2 Zn prepared in Example 1 2+High-resolution electron microscopy image of aggregation-induced dual co-reactant-enhanced gold nanoclusters.
[0028] Figure 3 This is a potential-electrochemiluminescence intensity diagram for different electrochemiluminescence systems.
[0029] Figure 4 Electrochemiluminescence spectra of different electrochemiluminescence systems.
[0030] Figure 5 This is a potential-electrochemiluminescence intensity diagram of the electrochemiluminescence system in Comparative Example 3. Detailed Implementation
[0031] The present invention is further illustrated by the following examples, but is not limited thereto.
[0032] The fluorescence spectra of the gold nanoclusters described in the examples were obtained using an F-4700 fluorescence spectrophotometer. The ultraviolet-visible absorption spectra were obtained using an Agilent Cary 60 UV-Vis spectrophotometer. Electrochemiluminescence spectra were acquired using the GCFG-A electrochemiluminescence spectroscopy acquisition system developed by Shandong Guochen Biotechnology Co., Ltd. The potential window used was 0 ~ 1.6 V, and the scan rate was 50 mV / s.
[0033] Example 1 Water-soluble Zn 2+ Preparation of aggregation-induced dual co-reactant enhanced gold nanoclusters: 1) Add the ligands D-penicillamine and 11-mercaptoundecanoic acid to 3.2 mL of deionized water to make the concentration of D-penicillamine 6.25 μM and the concentration of 11-mercaptoundecanoic acid 6.25 μM. Then, add 100 μL of HAuCl4·H2O to the above solution to make the concentration of HAuCl4·H2O 100 mM. Adjust the pH to 3.0 with stirring to obtain a mixed solution. 2) The borane-tert-butylamine complex and zinc acetate were added dropwise to the mixture from step 1), bringing the concentration of the borane-tert-butylamine complex to 7.5 μM and the concentration of zinc acetate to 0.425 μM. The mixture was stirred at 1500 rpm / min for one day. After adding the reducing agent, the color of the reaction solution changed from colorless to brown; the resulting solution contained Zn 2+ -DPA / MUA@AuNCs were precipitated with isopropanol and centrifuged to remove excess ligands.
[0034] Example 2 An electrochemiluminescence system based on dual co-reactant enhanced gold nanoclusters, wherein the luminescence system uses water-soluble Zn from Example 1 2+Aggregation-induced dual co-reactant enhancement of gold nanoclusters as the luminescent agent, triethanolamine and borane-tert-butylamine complex as the dual co-reactant, and phosphate buffer solution as the buffer solution, produces near-infrared electrochemiluminescence in the long-wavelength region; in the electrochemiluminescence system, water-soluble Zn 2+ The concentration of the aggregation-inducing dual co-reactant-enhanced gold nanoclusters was 2 mg / mL, the molar concentration of triethanolamine was 10 mM, the molar concentration of the borane-tert-butylamine complex was 10 mM, the concentration of the phosphate buffer solution was 0.1 M, and the pH value of the phosphate buffer solution was 7.4.
[0035] Example 3 An electrochemiluminescence system based on dual co-reactant enhanced gold nanoclusters, wherein the luminescence system uses water-soluble Zn from Example 1 2+ Aggregation-induced dual co-reactant enhancement of gold nanoclusters as the luminescent agent, triethanolamine and borane-tert-butylamine complex as the dual co-reactant, and phosphate buffer solution as the buffer solution, produces near-infrared electrochemiluminescence in the long-wavelength region; in the electrochemiluminescence system, water-soluble Zn 2+ The concentration of the aggregation-inducing dual co-reactant-enhanced gold nanoclusters was 3 mg / mL, the molar concentration of triethanolamine was 8 mM, the molar concentration of the borane-tert-butylamine complex was 12 mM, the concentration of the phosphate buffer solution was 0.3 M, and the pH value of the phosphate buffer solution was 7.4.
[0036] Example 4 An electrochemiluminescence system based on dual co-reactant enhanced gold nanoclusters, wherein the luminescence system uses water-soluble Zn from Example 1 2+ Aggregation-induced dual co-reactant enhancement of gold nanoclusters as the luminescent agent, triethanolamine and borane-tert-butylamine complex as the dual co-reactant, and phosphate buffer solution as the buffer solution, produces near-infrared electrochemiluminescence in the long-wavelength region; in the electrochemiluminescence system, water-soluble Zn 2+ The concentration of the aggregation-inducing dual co-reactant-enhanced gold nanoclusters was 5 mg / mL, the molar concentration of triethanolamine was 12 mM, the molar concentration of the borane-tert-butylamine complex was 10 mM, the concentration of the phosphate buffer solution was 0.5 M, and the pH of the phosphate buffer solution was 7.4.
[0037] Experimental Example 1 1. Water-soluble Zn collected in Example 1 2+ Aggregation-induced dual co-reactant enhanced gold nanoclusters were re-dissolved in ultrapure water to prepare a 2 mg / mL solution. The optical properties of the gold nanoclusters were characterized, and the UV and fluorescence spectra of the gold nanoclusters are shown in the figure. Figure 1 .from Figure 1 It can be seen from the water-soluble Zn 2+The maximum emission fluorescence of the aggregation-induced dual co-reactant-enhanced gold nanoclusters is located in the near-infrared region, at 747 and 816 nm, with maximum excitation wavelengths at 440 and 450 nm, respectively. There is a distinct surface plasmon resonance peak in the ultraviolet region at 590 nm.
[0038] 2. Zn collected in Example 1 2+ Aggregation-induced dual co-reactant enhanced precipitation of gold nanoclusters into powder was performed. The powder was then dropped onto a copper grid with a 1 mg / mL solution prepared from ultrapure water to characterize the morphology of the gold nanoclusters. High-resolution transmission electron microscopy of the gold nanoclusters was observed. Figure 2 .from Figure 2 It can be seen from Zn 2+ Aggregation-induced dual-ligand stabilized gold nanoclusters were 3 nm spherical particles.
[0039] 3. Electrochemiluminescence assay: A glassy carbon electrode was used as the working electrode, an Ag / AgCl electrode as the reference electrode, and a Pt wire as the counter electrode. A gold nanocluster modified electrode was prepared by drop-coating 10 μL of 2 mg / mL gold nanocluster solution onto the surface of the working electrode and then drying it. The test solution was a 0.1 M phosphate buffer solution (pH 7.4) containing 10 mM triethanolamine and 10 mM borane-tert-butylamine complex. The collected electrochemiluminescence spectra were integrated spectra of all ECL radiation.
[0040] Zn collected in Example 1 2+ The potential-electrochemiluminescence intensity diagram of aggregation-induced dual co-reactant enhanced gold nanoclusters (dotted line with dashes) is shown in [reference needed]. Figure 3 It can be seen that Zn 2+ The electrochemiluminescence signal of the aggregation-induced dual-ligand stabilized gold nanoclusters was approximately 4.7 times stronger than that of the single-co-reactant electrochemiluminescence system.
[0041] 4. Zn collected in Example 1 2+ The electrochemical spectroscopy of the aggregation-induced dual co-reactant-enhanced gold nanoclusters (dotted lines) is shown in [reference needed]. Figure 4 It can be seen that Zn 2+ Aggregation-induced dual co-reactant enhanced the electrochemiluminescence signal of gold nanoclusters in the near-infrared region, exceeding 850 nm, with a signal enhancement of approximately 4.7 times.
[0042] Comparative Example 1 The system is based on a single co-reactant gold nanoclusters electrochemiluminescence system, which uses water-soluble Zn from Example 1. 2+ Aggregation-induced dual co-reactant-enhanced gold nanoclusters as luminescent organisms, triethanolamine as reactant, and phosphate buffer solution as buffer solution, produce near-infrared electrochemiluminescence in the long-wavelength region.
[0043] Electrochemiluminescence assays were performed using a glassy carbon electrode as the working electrode, an Ag / AgCl electrode as the reference electrode, and a Pt wire as the counter electrode. The gold nanocluster-modified electrode was prepared by drop-coating 10 μL of 2 mg / mL gold nanocluster solution onto the surface of the working electrode and allowing it to dry. The test solution was a 0.1 M phosphate buffer solution (pH 7.4) containing 10 mM triethanolamine. The collected electrochemiluminescence spectra were integrated spectra of all ECL radiations.
[0044] Its electrochemiluminescence intensity diagram is shown below Figure 3 (Dash line), see electrochemiluminescence spectrum. Figure 4 (Dash line) Its electrochemiluminescence intensity is far less than that of the dual co-reactant electrochemiluminescence system.
[0045] Comparative Example 2 The system is based on a single co-reactant gold nanoclusters electrochemiluminescence system, which uses water-soluble Zn from Example 1. 2+ Aggregation-induced dual co-reactant enhances gold nanoclusters as luminescent organisms, with borane-tert-butylamine complex as reactant and phosphate buffer solution as buffer, generating near-infrared electrochemiluminescence in the long-wavelength region.
[0046] Electrochemiluminescence assays were performed using a glassy carbon electrode as the working electrode, an Ag / AgCl electrode as the reference electrode, and a Pt wire as the counter electrode. The gold nanocluster-modified electrode was prepared by drop-coating a 10 μL 2 mg / mL gold nanocluster solution onto the surface of the working electrode and allowing it to dry. The test solution was a 0.1 M phosphate buffer solution (pH 7.4) containing a 10 mM borane-tert-butylamine complex. The collected electrochemiluminescence spectra were integrated spectra of all ECL radiations.
[0047] Its electrochemiluminescence intensity diagram is shown below Figure 3 (Dotted lines), see electrochemiluminescence spectrum. Figure 4 (Dotted line) Its electrochemiluminescence intensity is far less than that of the dual co-reactant electrochemiluminescence system.
[0048] Comparative Example 3 To compare the electrochemiluminescence signals of different co-reactants, the electrochemiluminescence assay used a glassy carbon electrode as the working electrode, an Ag / AgCl electrode as the reference electrode, and a Pt wire as the counter electrode. A gold nanocluster-modified electrode was prepared by drop-coating a 10 μL (2 mg / mL) gold nanocluster solution onto the working electrode surface and allowing it to dry. The test solutions were 0.1 M phosphate buffer solutions containing 10 mM borane-tert-butylamine complex and 10 mM triethanolamine (dotted line), 10 mM sodium cyanoborohydride and 10 mM triethanolamine (solid line), 10 mM borane-ammonia complex and 10 mM triethanolamine (dotted line), and 10 mM hydrazine hydrate and 10 mM triethanolamine (dotted line). The electrochemiluminescence intensity diagrams are shown below. Figure 5 , Figure 5 It can be seen that the electrochemiluminescence signal of the dual co-reactant system with the addition of the reducing agent of the present invention is significantly enhanced compared with that of the single co-reactant system, and the signal of the dual co-reactant system with tert-butylammonoborane and triethanolamine is enhanced.
Claims
1. An electrochemiluminescence system based on dual co-reactant enhanced gold nanoclusters, wherein the luminescence system uses water-soluble Zn 2+ Aggregation-induced dual co-reactant enhancement of gold nanoclusters as luminescent organisms, with triethanolamine and borane-tert-butylamine complex as dual co-reactants, produces near-infrared electrochemiluminescence in the long-wavelength region under buffer conditions, which is 4-6 times stronger than that of the single co-reactant system, and its maximum emission wavelength is greater than 850 nm.
2. The electrochemiluminescence system according to claim 1, characterized in that, Water-soluble Zn 2+ Aggregation-induced dual co-reactant enhanced gold nanoclusters were prepared by the following method: (1) Add 11-mercaptoundecanoic acid and D-penicillamine to deionized water, then add H4AuCl4, and mix evenly by ultrasonication to obtain mixture a; (2) Add zinc acetate and borane-tert-butylamine complex to the mixture a in step (1) and mix evenly by ultrasonication to obtain mixture b; (3) Mixture b was stirred at room temperature to react. The resulting solution was purified by centrifugation with isopropanol, and the precipitate was water-soluble Zn. 2+ Aggregation-induced dual co-reactant enhances gold nanoclusters.
3. The electrochemiluminescence system according to claim 2, characterized in that, In step (1), the molar ratio of H4AuCl4 to 11-mercaptoundecanoic acid is 10000:(1-5), and the molar ratio of H4AuCl4 to D-penicillamine is 500:(1-5).
4. The electrochemiluminescence system according to claim 2, characterized in that, In step (1), the concentration of H4AuCl4 in mixture a is 80-120 mM, the concentration of 11-mercaptoundecanoic acid is 4-8 μM, and the concentration of D-penicillamine is 5-10 μM.
5. The electrochemiluminescence system according to claim 2, characterized in that, In step (2), the molar ratio of zinc acetate to H4AuCl4 in step (1) is (1-5):10000, and the molar ratio of borane-tert-butylamine complex to H4AuCl4 is (1-5):1000.
6. The electrochemiluminescence system according to claim 2, characterized in that, In step (2), the concentration of zinc acetate in mixture b is 0.2-1 μM, and the concentration of borane-tert-butylamine complex is 1-10 μM. In step (3), the stirring time is 12-36 hours.
7. The electrochemiluminescence system according to claim 1, characterized in that, In electrochemiluminescence systems, water-soluble Zn 2+ The concentration of aggregation-inducing dual co-reactant to enhance gold nanoclusters is 1-5 mg / mL.
8. The electrochemiluminescence system according to claim 1, characterized in that, In the electrochemiluminescence system, the concentration of the dual co-reactant is 8-25 mM, the molar concentration of triethanolamine is 4-10 mM, and the molar concentration of the borane-tert-butylamine complex is 4-15 mM.
9. The electrochemiluminescence system according to claim 1, characterized in that, In the electrochemiluminescence system, the buffer solution is a phosphate buffer solution with a concentration of 0.1-0.5M and a pH value of 5-10.
10. The method for constructing the electrochemiluminescence system based on dual co-reactant enhanced gold nanoclusters as described in claim 1, comprising the following steps: Water-soluble Zn 2+ Aggregation-induced dual co-reactant-enhanced gold nanoclusters were used as luminescent agents, and triethanolamine and borane-tert-butylamine complexes were used as dual co-reactants. In the presence of buffer solution, a dual co-reactant-type electrochemiluminescence system was formed. A three-electrode system and cyclic voltammetry were used to drive the electrochemiluminescence radiation of a dual co-reactant electrochemiluminescence system.