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Electrochemical luminescence method taking covalent organic framework as coreactant and application of arsenite radical detection

A covalent organic framework, co-reactant technology, applied in chemiluminescence/bioluminescence, electrochemical variables of materials, analysis by chemical reaction of materials, etc. , human health hazards, etc., to achieve the effect of good application prospects

Active Publication Date: 2020-11-06
NANCHANG UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0003] Ruthenium terpyridine (Ru(bpy) 3 2+ ) and terphenylpyridine iridium (Ir(ppy) 3 ) is a commonly used ECL luminescent reagent, and their commonly used co-reactants mainly include tripropylamine, triethylamine, triethanolamine, etc., but these amine co-reactants are volatile, highly toxic, and harmful to human health
However, there is no research report on COF as an ECL co-reactant

Method used

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  • Electrochemical luminescence method taking covalent organic framework as coreactant and application of arsenite radical detection
  • Electrochemical luminescence method taking covalent organic framework as coreactant and application of arsenite radical detection
  • Electrochemical luminescence method taking covalent organic framework as coreactant and application of arsenite radical detection

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Experimental program
Comparison scheme
Effect test

Embodiment 1

[0028] Preparation and Characterization of Tp-Bpy COF

[0029] Preparation of Tp-Bpy COF: first add trialdehyde phloroglucinol (Tp) and 5,5'-diamino-2,2'-bipyridine (Bpy) into a glass tube, then add 1,4-diox Alkanes, 1.0mL mesitylene and 6M acetic acid solution, the mixed solution was quickly frozen in a liquid nitrogen bath, and at the same time, the glass tube was evacuated and flame-sealed, and the sealed glass tube was placed in an oven at 120°C for 3 days. The product was washed with anhydrous tetrahydrofuran, and the obtained brown-red product was dried at 100°C for 24 hours to prepare a pyridine-containing covalent organic framework Tp-Bpy COF.

[0030] figure 1 A is the powder X-ray diffraction pattern (PXRD) of Tp-Bpy COF, Tp-Bpy COF has a strong diffraction peak at 3.6°, which is attributed to the reflection of the (100) crystal plane, at 7.2° and 26.9° The diffraction peaks were attributed to the (200) and (002) crystal planes of Tp-Bpy COF, respectively, indicati...

Embodiment 2

[0032] Coreactant effect of Tp-Bpy COF

[0033] The glassy carbon electrode was sequentially polished with 1.0, 0.3 and 0.05 μm alumina suspensions, and then ultrasonically cleaned in 0.1M nitric acid, absolute ethanol and ultrapure water for 1 minute, and the electrode surface was dried with nitrogen. 10μL 0.5mg mL -1 The mixed solution of Tp-Bpy COF and 0.002% chitosan (CS) was coated on the clean surface of GCE. 29 The single-stranded DNA was reacted in PBS (20mM pH 7.4) buffer solution for 12h, and the (AC) 29 Modified to the surface of the electrode by amide reaction, after cleaning the electrode with ultrapure water, soak the prepared electrode in a solution containing 100nM (GT) 29 Single-stranded DNA in PBS (20mM pH 7.4) buffer solution, reacted at 37°C for 30min, (GT) 29 Connected to the electrode by DNA complementary hybridization reaction, the prepared (GT) 29 / (AC) 29 / Tp-Bpy COF / GCE, the schematic diagram of the electrode modification process and the detectio...

Embodiment 3

[0037] Construction and characterization of ECL sensors

[0038] The construction process of the ECL sensor was characterized by cyclic voltammetry (CV) and alternating current impedance spectroscopy (EIS). Depend on Figure 4 A can be seen in [Fe(CN) 6 ] 3- / 4- In solution, GCE has an obvious redox peak (curve a); the peak current on Tp-Bpy COF / GCE is obviously weakened (curve b); due to (AC) 29 Single-stranded DNA has a negatively charged phosphate backbone, (AC) 29 The current on / Tp-BpyCOF / GCE further decreases (curve c); when (GT) 29 When connected to the electrode surface by DNA hybridization, the peak current is further reduced (curve d); (GT) 29 / (AC) 29 / Tp-Bpy COF / GCE in Ru(bpy) 3 2+ After reacting in the solution for 30min, because Ru(bpy) 3 2+ Positively charged, the peak current of the electrode increases slightly (curve e); when there is 10ppb As(III), the peak current of the electrode is significantly enhanced (curve f), which is due to As(III) and (GT)...

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Abstract

The invention discloses an electrochemical luminescence method taking a covalent organic framework as a coreactant and application of arsenite radical detection, which belong to the technical field ofelectrochemiluminescence sensing. The surface of a glassy carbon electrode is coated with a mixed solution of a covalent organic framework Tp-Bpy COF and chitosan; (AC)29 is assembled to the surfaceof an electrode through an amide reaction, and (GT)29 is connected to the electrode through DNA complementary hybridization to prepare a (GT)29 / (AC)29 / Tp-Bpy COF modified electrode which has a strongcathode ECL signal in Ir(bpy)3. When Ru(bpy)3<2+> is embedded into (GT)29 / (AC)29 double chains through electrostatic interaction, ECL of Ru(bpy)3<2+> is enhanced, and ECL of Ir(bpy)3 is weakened. WhenAs(III) is present, the ECL signal of Ir(ppy)3 is enhanced, and the ECL signal of Ru(bpy)3<2+> is reduced; the ratio of the ECL signals of Ir(ppy)3 and Ru(bpy)3<2+> and the concentration of As(III) have a linear relationship; and an ECL method based on a Tp-Bpy COF co-reactant effect and an ECL-RET effect between Ru(bpy)3<2+> and Ir(ppy)3 is constructed, and is used for ultra-sensitive detectionof As(III).

Description

technical field [0001] The invention relates to an electrochemiluminescence method using a covalent organic framework as a co-reactant and an arsenite detection application, belonging to the technical field of electrochemiluminescence sensing. Background technique [0002] Arsenic is widely distributed in nature, and inorganic arsenic is a kind of carcinogenic and highly toxic substance, which can cause lung cancer and skin cancer. Arsenic poisoning mainly comes from polluted drinking water, so it is of great significance to develop detection methods for arsenic in complex environmental water samples. In recent years, arsenite As(III) has been detected by a variety of methods, including inductively coupled plasma mass spectrometry, fluorescence, Raman scattering, electrochemical, colorimetry, and electrochemiluminescence (ECL), etc. Among them, ECL has the characteristics of high sensitivity, wide linear range, low background signal and low cost, and has outstanding advanta...

Claims

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Application Information

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IPC IPC(8): G01N27/30G01N21/76
CPCG01N21/76G01N27/308
Inventor 梁汝萍曹姝萍邱建丁
Owner NANCHANG UNIV
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