A New Covalent Organic Framework of Dicyandiamide-Benzaldehyde Nanocatalytic Amplification SERS/RRS Aptamer Assay for Ultratrace Oxytetracycline with the Nanogold Indicator Reaction of Polyethylene Glycol 600
Abstract
:1. Introduction
2. Experimental
2.1. Instruments and Reagents
2.2. Preparation of the Highly Catalytic DdBd Nanosol
2.3. Procedure
3. Results and Discussion
3.1. Analytical Principles
3.2. Characterization of the Nanomaterials
3.3. RRS and SERS Spectra of the Catalytic Analysis System
3.4. Catalytic Enhancement Mechanism of COF
3.5. Optimal Conditions
3.6. Working Curve
3.7. Influence of Coexisting Substances
3.8. Sample Analysis
4. Discussion
5. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
Appendix A
Nano Catalytic System | Linear Range (nmol/L) | Linear Equation | Coefficient |
---|---|---|---|
lycol | 0.450–4.50 | ΔI370nm = 1.73 × 103 C − 67.4 | 0.9750 |
PEG200 | 0.225–1.575 | ΔI370nm = 5.54 × 103 C + 402.3 | 0.9208 |
PEG400 | 0.450–3.15 | ΔI370nm = 3.26 × 103 C + 383 | 0.9603 |
PEG600 | 0.225–1.58 | ΔI370nm = 6.67 × 103 C + 223 | 0.9952 |
PEG6000 | 0.225–1.58 | ΔI370nm = 2.79 × 103 C + 57.9 | 0.9590 |
PEG20000 | 0.225–1.58 | ΔI370nm = 5.11 × 103 C + 231.3 | 0.9301 |
Method | Principle | Linear Range | DL | Ref. |
---|---|---|---|---|
Fluorescence | The covalent attachment of DNA probes and MOF nanosheets enhances the affinity between the nanomaterials and DNA, and the interaction with OTC leads to a decrease in fluorescence. | 0.50–5.00 μg/L | 0.40 μg/L | [27] |
Apt electrochemical sensor | A portable aptamer sensor was constructed to detect oxytetracycline by using gold nanoparticles/carboxylated multi-walled carbon nanotubes @thionine-linked aptamer complementary chains as signal markers. | 10−13–10−5 g/mL | 3.1 × 10−14 g/mL | [28] |
Apt electrochemical sensor | The Ce-MOF@COF hybrid product shows high bioaffinity for OTC targeting aptamers, which further increases the detection effect of OTC detection. | 0.1–0.5 ng/mL | 17.4 fg/mL | [29] |
Ap light sensor | A LRET biosensor was developed, coupling the OTC aptamer to the photonanoparticle for OTC measurement. | 0.1–10 ng/ml | 0.054 ng/ml | [30] |
SERS | A nano-biosensor based on AuNPs was established, with stem-loop DNA modification as the SERS active substrate for OTC detection. | 4.60 × 10−2–4.6 × 102 fg/mL | 4.35 × 10−3 fg/mL | [31] |
SERS/RRS | According to a COF-catalyzed PEG600-HAuCl4-HCl reaction to generate AuNPs, SERS and RRS signals were generated, and combined with aptamers at the same time; a new SERS/RRS coupled dual-mode OTC detection method was developed. | 3.00 × 10−3–7.00 × 10−2 nmol/L | 9.0 × 10−4 nmol/L | This Method |
Coexisting Substances | Times | Relative Error (%) | Coexisting Substances | Times | Relative Error (%) |
---|---|---|---|---|---|
Na+ | 1000 | −2.4 | HCO3− | 500 | 2.4 |
Co2+ | 1000 | 4.5 | CH3COO− | 1000 | −2.1 |
Zn2+ | 500 | 3.3 | HPO42− | 500 | 6.1 |
K+ | 50 | 4.4 | H2PO4− | 10 | −5.3 |
Ca2+ | 1000 | 3.5 | P2O74− | 100 | 9.6 |
Mg2+ | 100 | −4.3 | CO32− | 500 | −7.5 |
Al3+ | 1000 | 5.2 | NAD | 100 | −5.3 |
Fe3+ | 500 | 3.1 | GTP | 1000 | −7.2 |
SO32− | 1000 | −6.4 | CTP | 1000 | −6.3 |
SO42− | 500 | −4.5 | UTP | 1000 | −4.1 |
PO43− | 1000 | −5.1 | ADP | 500 | −2.3 |
NO2− | 1000 | −3.1 | AMP | 100 | 6.8 |
penicillin sodium | 10 | 5.4 | tetracycline | 5 | 8.6 |
Coexisting Substances | Times | Relative Error (%) | Coexisting Substances | Times | Relative Error (%) |
---|---|---|---|---|---|
Na+ | 1000 | −5.9 | HCO3− | 100 | −1.8 |
Co2+ | 1000 | 5.9 | CH3COO− | 1000 | −7.1 |
Zn2+ | 10 | −3.5 | HPO42− | 500 | 5.4 |
K+ | 100 | −5.3 | H2PO4− | 1000 | −0.6 |
Ca2+ | 500 | −3.4 | P2O74− | 500 | −6.1 |
Mg2+ | 1000 | −6.7 | CO32− | 100 | −3.5 |
Al3+ | 50 | 2.8 | Thr | 1000 | −4.7 |
Fe3+ | 1000 | 4.2 | Lys | 1000 | 1.1 |
SO32− | 1000 | 2.8 | His | 500 | 6.1 |
SO42− | 10 | −9.5 | Trp | 100 | 2.8 |
PO43− | 1000 | 1.7 | Ala | 1000 | 4.3 |
NO2− | 1000 | −6.9 | Gly | 10 | −5.7 |
ofloxacin | 5 | 6.7 | tetracycline | 5 | 7.1 |
Sample | Single Value (×10−3 nmol/L) | Average (×10−3 nmol/L) | Added (×10−3 nmol/L) | Found (×10−3 nmol/L) | Recovery (%) | RSD (%) | Content (μg/kg) | AAS (μg/kg) |
---|---|---|---|---|---|---|---|---|
1 | 5.45, 5.36, 5.73, 5.01, 5.36 | 5.38 | 6.70 | 11.88 | 96.3 | 4.78 | 2.04 | |
13.0 | 18.79 | 107.6 | 2.20 | |||||
20.0 | 25.52 | 102.6 | ||||||
2 | 7.04, 6.73, 6.96 7.23, 7.18 | 7.03 | 6.70 | 13.42 | 95.6 | 2.82 | 2.67 | |
13.0 | 20.39 | 105.1 | 2.44 | |||||
20.0 | 27.10 | 101.1 | ||||||
3 | 8.49, 8.47, 8.34 8.61, 8.73 | 8.53 | 6.70 | 15.16 | 99.2 | 1.73 | 3.24 | |
13.0 | 21.42 | 98.7 | 3.46 | |||||
20.0 | 28.17 | 95.8 | ||||||
4 | 7.82, 7.83, 7.65 7.93, 7.74 | 7.79 | 6.70 | 14.05 | 94.3 | 1.35 | 2.96 | |
13.0 | 20.93 | 101.8 | 3.12 | |||||
20.0 | 28.17 | 104.9 |
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Reductant | Linear Range (×10−3 nmol/L) | Linear Equation | Coefficient | DL (×10−3 nmol/L) |
---|---|---|---|---|
EG | 13.0–53.0 6.70–33.0 | ΔIRRS = 2.54 × 103 COTC + 11.9 ISERS = 1.44 × 104 COTC − 92.5 | 0.9853 0.9797 | 8.7 7.2 |
PEG200 | 6.70–46.7 6.70–53.0 | ΔIRRS = 7.30 × 103 COTC + 13.9 ISERS = 2.50 × 104 COTC + 59.4 | 0.9721 0.9932 | 3.3 2.2 |
PEG400 | 13.0–60.0 6.70–60.0 | ΔIRRS = 2.99 × 103 COTC − 8.10 ISERS = 4.00 × 104 COTC + 308 | 0.9715 0.9292 | 5.0 5.0 |
PEG600 | 3.00–60.0 3.00–70.0 | ΔIRRS = 9.33 × 103 COTC + 33.9 ISERS = 4.58 × 104 COTC + 181 | 0.9902 0.9872 | 1.1 0.9 |
PEG6000 | 6.70–57.0 3.30–33.0 | ΔIRRS = 7.76 × 103 COTC + 0.400 ISERS = 2.93 × 104 COTC − 0.800 | 0.9748 0.9899 | 2.9 2.6 |
PEG20000 | 6.70–50.0 6.70–43.0 | IRRS = 6.19 × 103 COTC + 18.2 ISERS = 171 × 104 COTC − 13.9 | 0.9905 0.9801 | 3.2 3.8 |
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Liang, A.; Zhi, S.; Liu, Q.; Li, C.; Jiang, Z. A New Covalent Organic Framework of Dicyandiamide-Benzaldehyde Nanocatalytic Amplification SERS/RRS Aptamer Assay for Ultratrace Oxytetracycline with the Nanogold Indicator Reaction of Polyethylene Glycol 600. Biosensors 2021, 11, 458. https://doi.org/10.3390/bios11110458
Liang A, Zhi S, Liu Q, Li C, Jiang Z. A New Covalent Organic Framework of Dicyandiamide-Benzaldehyde Nanocatalytic Amplification SERS/RRS Aptamer Assay for Ultratrace Oxytetracycline with the Nanogold Indicator Reaction of Polyethylene Glycol 600. Biosensors. 2021; 11(11):458. https://doi.org/10.3390/bios11110458
Chicago/Turabian StyleLiang, Aihui, Shengfu Zhi, Qiwen Liu, Chongning Li, and Zhiliang Jiang. 2021. "A New Covalent Organic Framework of Dicyandiamide-Benzaldehyde Nanocatalytic Amplification SERS/RRS Aptamer Assay for Ultratrace Oxytetracycline with the Nanogold Indicator Reaction of Polyethylene Glycol 600" Biosensors 11, no. 11: 458. https://doi.org/10.3390/bios11110458