Bio-Enhanced Degradation Strategies for Fluoroquinolones in the Sewage Sludge Composting Stage: Molecular Modification and Resistance Gene Regulation
Abstract
:1. Introduction
2. Materials and Methods
2.1. Source of FQs and Biodegradation Enzymes in Sewage Sludge Composting Stage
2.2. Characterization of FQs Molecular Biodegradability in Sewage Sludge Composting Stage—Molecular Docking Method
2.3. Characterization of the Combined Biodegradability of Thermophilic Bacteria of FQs Sewage Sludge Composting Stage—Entropy Weight Method and Index Normalization Method
2.4. Construction of 3D-QSAR Models of FQs Biodegradability for Single and Combined Thermophilic Bacteria—CoMFA Method
2.5. Optimization of External Environmental Conditions for Combined Biodegradability Improvement of FQs Sewage Sludge Composting Stage under Multiple Scenarios
2.5.1. Characterization of Key Proteins Affecting the Combined Biodegradability of FQs Sewage Sludge Composting Stage—Protein–Protein Docking
2.5.2. Screening of External Environmental Conditions Affecting the Combined Biodegradability of FQs Sewage Sludge Composting Stage and Setting of Degradation Scenarios
2.5.3. Optimization of External Environmental Conditions for Combined Biodegradability Improvement of FQ Sewage Sludge Composting Stage—MD Simulation
3. Results and Discussion
3.1. Quantitative Analysis of Combined Biodegradation Levels of Single Thermophilic Bacteria and Thermophilic Group to FQs in Sewage Sludge Composting Stage
3.2. Construction and Evaluation of the Biodegradability 3D-QSAR Models of FQs by Thermophilic Bacteria in Sewage Sludge Composting Stage
3.3. Molecular Modification of FQs with Improved Biodegradation and Prediction of Relevant Properties for FQ Derivatives
3.3.1. Determination of Modified Sites and Groups for FQs with High Combined Biodegradability Based on the Contour Maps
3.3.2. Evaluation of Biodegradability, Environmental Friendliness, and Functionality of MOX Derivatives
3.4. Regulation of External Environmental Conditions to Enhance the Combined Biodegradation of FQs by the Thermophilic Group in Sewage Sludge Composting Stage
3.4.1. Effectiveness Validation of External Environmental Conditions to Enhance the Combined Biodegradation of FQs by Thermophilic Group
3.4.2. Identification of Interactions between the External Environmental Conditions for Enhancing the Combined Biodegradation of FQs by Thermophilic Group
3.5. Regulatory Measures to Enhance the Ability of FQs Antibiotics to Inhibit Expression of Bacterial Resistance in Agricultural Soils
3.5.1. Characterization of the Ability of FQs Antibiotics to Inhibit the Expression of Bacterial Resistance
3.5.2. A Survey on Background Values of Nutrients in Agricultural Soils Based on the Sampling Method
3.5.3. Validation of Field Measures to Strengthen FQs Antibiotics to Inhibit Bacterial Resistance Expression
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Scenarios | Group | OM | POS | WV | CA | AP | UR | NTA | MS |
---|---|---|---|---|---|---|---|---|---|
Scenarios 1–4 | 0 | 0 | 0 | 0 | 0 | 0 | 0 | 0 | 0 |
1 | 1 | 0 | 0 | 0 | 0 | 0 | 0 | 0 | |
2 | 0 | 1 | 0 | 0 | 0 | 0 | 0 | 0 | |
3 | 0 | 0 | 1 | 0 | 0 | 0 | 0 | 0 | |
4 | 0 | 0 | 0 | 1 | 0 | 0 | 0 | 0 | |
5 | 0 | 0 | 0 | 0 | 1 | 0 | 0 | 0 | |
6 | 0 | 0 | 0 | 0 | 0 | 1 | 0 | 0 | |
7 | 0 | 0 | 0 | 0 | 0 | 0 | 1 | 0 | |
8 | 0 | 0 | 0 | 0 | 0 | 0 | 0 | 1 |
No. | LibDock Scores (Å) | No. | LibDock Scores (Å) | ||||
---|---|---|---|---|---|---|---|
1GKQ | 1OB0 | 5M0K | 1GKQ | 1OB0 | 5M0K | ||
DIF | 84.12 | 75.48 | 140.10 | GRE | 112.04 | 96.52 | 131.73 |
ENR | 100.78 | 86.76 | 134.64 | ORB | 109.02 | 73.32 | 123.93 |
NOR | 104.68 | 72.91 | 112.09 | SIT | 113.51 | 44.62 | 116.03 |
LOM | 101.81 | 77.37 | 102.15 | TEM | 101.77 | 66.88 | 128.92 |
OFL | 98.41 | 78.28 | 116.92 | D1 | 97.29 | 65.18 | 117.57 |
PEF | 99.23 | 79.78 | 116.54 | D12 | 103.11 | 62.64 | 121.15 |
FLE | 99.72 | 79.14 | 119.69 | D13 | 110.35 | 72.08 | 140.83 |
CIP | 104.38 | 70.57 | 121.27 | D14 | 108.14 | 72.45 | 126.07 |
BAL | 93.22 | 70.74 | 112.77 | D16 | 111.53 | 70.42 | 118.88 |
MAR | 95.34 | 71.23 | 112.43 | D28 | 105.93 | 68.43 | 119.98 |
PIP | 98.32 | 80.33 | 115.43 | D29 | 106.31 | 72.58 | 93.84 |
CIN | 82.01 | 77.73 | 106.75 | D32 | 109.95 | 66.48 | 123.98 |
ENO | 105.20 | 69.22 | 116.45 | D36 | 108.31 | 71.45 | 111.83 |
DAN | 113.74 | 74.73 | 117.32 | D37 | 109.31 | 77.10 | 124.29 |
GAT | 93.02 | 54.82 | 104.21 | F1 | 101.62 | 83.50 | 118.65 |
LEV | 98.41 | 78.28 | 116.92 | F2 | 111.46 | 77.43 | 111.20 |
RUF | 82.48 | 77.59 | 102.54 | F3 | 61.76 | 72.02 | 56.16 |
PAZ | 95.01 | 79.25 | 123.49 | F4 | 91.93 | 76.03 | 91.83 |
NAD | 108.43 | 81.41 | 112.09 | F5 | 99.71 | 65.73 | 113.26 |
MOX | 83.16 | 69.91 | 83.47 | F6 | 113.41 | 81.72 | 105.99 |
SPA | 114.87 | 72.45 | 121.10 | Gat-29 | 116.29 | 72.32 | 130.15 |
SAR | 88.81 | 75.82 | 135.60 | Gat-30 | 117.05 | 77.81 | 129.55 |
AMI | 97.24 | 73.04 | 105.85 | Gat-31 | 91.29 | 63.80 | 117.09 |
BES | 82.54 | 59.00 | 119.14 | Gat-33 | 106.93 | 80.69 | 125.73 |
CLI | 109.08 | 69.81 | 115.70 |
No. | CV | No. | CV | No. | CV | No. | CV |
---|---|---|---|---|---|---|---|
1 | 5.857 | 14 | 6.205 | 27 | 6.185 | F1 | 6.154 |
2 | 6.792 | 15 | 4.129 | 28 | 4.882 | F2 | 6.027 |
3 | 5.605 | 16 | 5.752 | 29 | 5.800 | F3 | 2.050 |
4 | 5.351 | 17 | 4.630 | D1 | 5.177 | F4 | 4.571 |
5 | 5.752 | 18 | 5.881 | D12 | 5.413 | F5 | 5.149 |
6 | 5.834 | 19 | 6.108 | D13 | 6.747 | F6 | 6.110 |
7 | 5.931 | 20 | 3.696 | D14 | 6.185 | Gat-29 | 6.629 |
8 | 5.801 | 21 | 6.278 | D16 | 5.990 | Gat-30 | 6.871 |
9 | 5.095 | 22 | 5.902 | D28 | 5.727 | Gat-31 | 4.872 |
10 | 5.186 | 23 | 5.116 | D29 | 5.045 | Gat-33 | 6.475 |
11 | 5.785 | 24 | 4.401 | D32 | 5.933 | ||
12 | 4.758 | 25 | 5.764 | D36 | 5.675 | ||
13 | 5.615 | 26 | 7.541 | D37 | 6.367 |
Compounds | Substituent Groups | Predicted CV | Change Range (%) | Predicted 1GKQ | Change Range (%) | Predicted 1OB0 | Change Range (%) | Predicted 5M0K | Change Range (%) |
---|---|---|---|---|---|---|---|---|---|
Moxifloxacin | - | 3.696 | - | 1.920 | - | 1.845 | - | 1.922 | - |
Derivative-1 | 1-NO | 3.823 | 3.44 | 2.049 | 6.72 | 1.873 | 1.52 | 2.062 | 7.28 |
Derivative-2 | 1-COOH | 3.712 | 0.43 | 2.048 | 6.67 | 1.880 | 1.90 | 2.066 | 7.49 |
Derivative-3 | 2-CH3 | 4.079 | 10.36 | 2.051 | 6.82 | 1.891 | 2.49 | 2.058 | 7.08 |
Derivative-4 | 2-C2H5 | 4.315 | 16.75 | 2.049 | 6.72 | 1.889 | 2.38 | 2.073 | 7.86 |
Derivative-5 | 2-C3H7 | 4.592 | 24.24 | 2.049 | 6.72 | 1.887 | 2.28 | 2.093 | 8.90 |
Derivative-6 | 2-C4H9 | 4.592 | 24.24 | 2.049 | 6.72 | 1.885 | 2.17 | 2.100 | 9.26 |
Derivative-7 | 2-C5H11 | 4.623 | 25.08 | 2.049 | 6.72 | 1.883 | 2.06 | 2.106 | 9.57 |
Derivative-8 | 2-C=C | 4.144 | 12.12 | 2.050 | 6.77 | 1.885 | 2.17 | 2.070 | 7.70 |
Derivative-9 | 2-CH2NH2 | 4.088 | 10.61 | 2.050 | 6.77 | 1.890 | 2.44 | 2.064 | 7.39 |
Derivative-10 | 2-NH2 | 4.454 | 20.51 | 2.047 | 6.61 | 1.896 | 2.76 | 2.048 | 6.56 |
No. | Genotoxicity | Bioaccumulation | Photodegradability | |||
---|---|---|---|---|---|---|
Predicted | Change Range (%) | Predicted | Change Range (%) | Predicted | Change Range (%) | |
MOX | 8.869 | 0.950 | 1.975 | |||
Derivative-1 | 7.978 | −10.05 | 0.211 | −77.79 | 0.965 | −51.14 |
Derivative-2 | 8.163 | −7.96 | 0.541 | −43.05 | 0.921 | −53.37 |
Derivative-3 | 8.389 | −5.41 | 1.147 | 20.74 | 1.07 | −45.82 |
Derivative-4 | 8.343 | −5.93 | 1.258 | 32.42 | 1.094 | −44.61 |
Derivative-5 | 8.437 | −4.87 | 1.497 | 57.58 | 1.117 | −43.44 |
Derivative-6 | 8.537 | −3.74 | 1.547 | 62.84 | 1.153 | −41.62 |
Derivative-7 | 8.467 | −4.53 | 1.643 | 72.95 | 1.156 | −41.47 |
Derivative-8 | 8.373 | −5.59 | 1.102 | 16.00 | 1.068 | −45.92 |
Derivative-9 | 8.549 | −3.61 | 0.912 | −4.00 | −0.582 | −129.47 |
Derivative-10 | 8.808 | −0.69 | 0.453 | −52.32 | −0.219 | −111.09 |
Area | No. | Coordinate | Nutrient Content (g/kg) | |||
---|---|---|---|---|---|---|
E (°) | N (°) | C | N | P | ||
I | 1 | 125.60 | 50.15 | 1.33 | 0.85 | 2.17 |
2 | 125.62 | 48.46 | 0.87 | 0.56 | 1.27 | |
3 | 125.56 | 46.64 | 0.43 | 0.24 | 0.84 | |
4 | 125.45 | 45.23 | 0.68 | 0.58 | 0.99 | |
II | 5 | 120.20 | 40.41 | 0.96 | 0.53 | 1.23 |
6 | 122.95 | 42.00 | 0.76 | 0.49 | 1.14 | |
7 | 124.79 | 41.33 | 0.37 | 0.24 | 0.57 | |
8 | 121.44 | 38.91 | 0.96 | 0.53 | 1.23 | |
III | 9 | 125.97 | 41.94 | 2.13 | 0.49 | 1.14 |
10 | 120.07 | 43.63 | 1.42 | 0.88 | 1.36 | |
11 | 127.55 | 42.82 | 1.23 | 0.72 | 0.99 | |
12 | 130.71 | 44.47 | 2.13 | 1.15 | 2.17 | |
Average value | 1.11 | 0.61 | 1.26 | |||
Addition of Nutrient Elements | 2 | 1 | 2 |
FQs | Nutrient Elements | Field Measures | Binding Energy | Change Range | ||||
---|---|---|---|---|---|---|---|---|
C | N | P | Organic Fertilizer Application | Straw Returning | Plowing | |||
MOX | 2 | 1 | 2 | - | - | - | −49.445 | - |
Derivative-10 | - | - | - | −73.608 | 48.87% | |||
0 | 0 | 0 | −73.608 | - | ||||
1 | 0 | 0 | −85.565 | 16.24% | ||||
0 | 1 | 0 | −78.515 | 6.67% | ||||
0 | 0 | 1 | −93.523 | 27.06% | ||||
1 | 1 | 0 | −95.529 | 29.78% | ||||
1 | 0 | 1 | −87.956 | 19.49% | ||||
0 | 1 | 1 | −85.619 | 16.32% | ||||
1 | 1 | 1 | −104.013 | 41.31% |
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Jin, X.; Zhao, Y.; Ren, Z.; Wang, P.; Li, Y. Bio-Enhanced Degradation Strategies for Fluoroquinolones in the Sewage Sludge Composting Stage: Molecular Modification and Resistance Gene Regulation. Int. J. Environ. Res. Public Health 2022, 19, 7766. https://doi.org/10.3390/ijerph19137766
Jin X, Zhao Y, Ren Z, Wang P, Li Y. Bio-Enhanced Degradation Strategies for Fluoroquinolones in the Sewage Sludge Composting Stage: Molecular Modification and Resistance Gene Regulation. International Journal of Environmental Research and Public Health. 2022; 19(13):7766. https://doi.org/10.3390/ijerph19137766
Chicago/Turabian StyleJin, Xingyan, Yuanyuan Zhao, Zhixing Ren, Panpan Wang, and Yu Li. 2022. "Bio-Enhanced Degradation Strategies for Fluoroquinolones in the Sewage Sludge Composting Stage: Molecular Modification and Resistance Gene Regulation" International Journal of Environmental Research and Public Health 19, no. 13: 7766. https://doi.org/10.3390/ijerph19137766