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Water quality. Determination of Phenoxy carboxylic acids herbicide by High Performance Liquid Chromatography. Tandem Mass Spectrometry
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HJ 770-2015
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Standard similar to HJ 770-2015 HJ 511 HJ 945.3 HJ 780
Basic data Standard ID | HJ 770-2015 (HJ770-2015) | Description (Translated English) | Water quality. Determination of Phenoxy carboxylic acids herbicide by High Performance Liquid Chromatography. Tandem Mass Spectrometry | Sector / Industry | Environmental Protection Industry Standard | Word Count Estimation | 17,117 | Date of Issue | 2015-11-20 | Date of Implementation | 2015-12-15 | Quoted Standard | HJ/T 91; HJ/T 164 | Regulation (derived from) | Ministry of Environment Announcement 2015 No.73 | Issuing agency(ies) | Ministry of Ecology and Environment | Summary | This Standard specifies the determination of phenoxy acid herbicides in water by liquid chromatography /Tandem mass spectrometry. This Standard applies to surface water, groundwater and wastewater 2-methyl-4-chlorophenoxy acetic acid, 2, 4-dichlorophenoxyacetic acid, 2- (2-methyl-4-chlorophenoxy) propionic acid, 2- (2, 4-dichlorophenoxy) - propanoic acid (propionic acid or 2, 4), 2, 4, 5-trichlorophenoxyacetic acid, 2- (2, 4, 5-trimethyl chlorophenoxy) - propionic acid (2, 4, 5-T or propionic acid), 4- (2, 4-dichloro-phenoxy) - butyric acid and 4- (2-methyl-4-chlorophenoxy yl) butyric acid 8 kinds phenoxy acid herbicides determination. |
HJ 770-2015: Water quality. Determination of Phenoxy carboxylic acids herbicide by High Performance Liquid Chromatography. Tandem Mass Spectrometry ---This is a DRAFT version for illustration, not a final translation. Full copy of true-PDF in English version (including equations, symbols, images, flow-chart, tables, and figures etc.) will be manually/carefully translated upon your order.
Water quality.Determination of Phenoxy carboxylic acids herbicide by High Performance Liquid Chromatography.Tandem Mass Spectrometry
National Environmental Protection Standard of the People 's Republic of China
Water quality - Determination of phenoxy carboxylic acid herbicides
Liquid chromatography/tandem mass spectrometry
Water quality-Determination of Phenoxy carboxylic acids herbicide by
High Performance Liquid Chromatography-Tandem Mass
Spectrometry
2015-11-20 release
2015-12-15 implementation
Ministry of Environmental Protection released
Directory
Preface ..II
1 Scope of application
2 normative reference documents
3 Principle of the method
4 reagents and materials
5 instruments and equipment
6 samples
7 Analysis steps
8 Results calculation and presentation
9 precision and accuracy
Quality assurance and quality control
11 Waste treatment .9
Appendix A (normative appendix) method of detection limit and lower limit of determination
Appendix B (informative) method of precision and accuracy 11
Foreword
To implement the "Environmental Protection Law of the People's Republic of China" and "Water Pollution Prevention Law of the People's Republic of China" to protect the environment and protect the human body
Health, standard water phenoxy carboxylic acid herbicides monitoring methods, the development of this standard.
This standard specifies the determination of phenoxy carboxylic acid herbicides in water by liquid chromatography/tandem mass spectrometry.
This standard is the first release.
Appendix A is a normative appendix, Appendix B is an informative appendix.
This standard is organized by the Ministry of Environmental Protection Science and Technology Standards Division.
The main drafting unit of this standard. Jiangsu Province Environmental Monitoring Center.
The standard method of verification unit. Suzhou City Environmental Monitoring Center Station, Dalian Environmental Monitoring Center Station, Jiangsu Entry-Exit Inspection and Quarantine Bureau
Food Laboratory, Changzhou Environmental Monitoring Center, Jinan Environmental Monitoring Center, Shimadzu Enterprise Management (China) Co., Ltd. Shanghai Analysis
center.
The Environmental Protection Department of this standard approves on November 20,.2015.
This standard is implemented as of December 15,.2015.
This standard is explained by the Ministry of Environmental Protection.
Water quality - Determination of phenoxy carboxylic acid herbicides
Liquid chromatography/tandem mass spectrometry
Warning. Phenoxy carboxylic acid herbicides are toxic organic compounds, the experimental process of the use of organic solvents with strong volatility. Minute
Analysis of personnel in the experimental operation, should be in the fume hood operation; should be required to wear protective equipment, to avoid contact with skin and clothing.
1 Scope of application
This standard specifies the determination of phenoxy carboxylic acid herbicides in water by liquid chromatography/tandem mass spectrometry.
This standard applies to surface water, groundwater and waste water 2-methyl-4-chlorophenoxyacetic acid, 2,4-dichlorophenoxyacetic acid, 2- (2-methyl-
Chlorophenoxy) propionic acid, 2- (2,4-dichlorophenoxy) -propionic acid (or 2,4-propionic acid), 2,4,5-trichlorophenoxyacetic acid, 2- ( 2,4,5-trichloro
Phenoxy) -propionic acid (or 2,4,5-propionic acid), 4- (2,4-dichlorophenoxy) -butyric acid and 4- (2-methyl-4-chlorophenoxy ) Butyric acid
Determination of phenoxy carboxylic acid herbicides.
When the injection volume is 10 μl, the detection limit of the method is 0.3 μg/L ~ 0.5 μg/L, and the detection limit is 1.2 μg/L ~ 2.0
Μg/L, see Appendix A.
When the volume of the sample was 100 ml, the volume of the volume was 1.0 ml after concentration and the volume of the sample was 10 μl.
Limited to 0.006 μg/L to 0.009 μg/L, with a lower limit of 0.024 μg/L to 0.036 μg/L, as described in Appendix A.
2 normative reference documents
The contents of this standard refer to the terms of the following documents. For undated references, the valid version applies to this standard.
Technical specification for surface water and wastewater monitoring
Technical specification for groundwater environmental monitoring
3 Principle of the method
The phenoxy carboxylic acid herbicides in water were enriched by direct injection or solid phase extraction and separated by liquid chromatography/tandem mass spectrometry. according to
Retention time and characteristic ion peak characterization, internal standard method quantification.
4 reagents and materials
Unless otherwise stated, analytical analytical reagents and experimental water are used in accordance with national standards.
4.1 standard solution
4.1.1 Phenoxy carboxylic acid herbicide standard stock solution. ρ = 100 μg/ml.
Can be directly purchased certified standard solution can also be prepared with standard materials. The stock solution is stored in the dark at 0 ° C to 4 ° C or referenced to the manufacturer
product manual. Use should be restored to room temperature, and shake.
4.1.2 phenoxy carboxylic acid herbicides standard use of liquid. ρ = 10.0 μg/ml (reference concentration).
The standard stock solution (4.1.1) of the phenoxy carboxylic acid compound is diluted with acetonitrile (4.2) as required. Standard use of liquid at 4 ℃ cold, avoid
Light preservation, shelf life of two months. Use should be restored to room temperature, and shake.
4.1.3 Internal standard stock solution. ρ = 100 μg/ml.
The internal standard is 2,4-dichlorophenoxyacetic acid-13C6, can be directly purchased certified standard solution can also be prepared with the standard material. The stock solution is at zero
℃ ~ 4 ℃ Keep away from light or refer to the manufacturer's product description. Use should be restored to room temperature, and shake.
4.1.4 Internal standard liquid. ρ = 10.0 μg/ml (reference concentration).
The internal standard stock solution (4.1.3) was diluted with acetonitrile (4.2) as needed. Internal standard use of liquid at 0 ℃ ~ 4 ℃ dark preservation, shelf life
Two months. Use should be restored to room temperature, and shake.
4.2 acetonitrile (CH3CN). pesticide residues.
4.3 methanol (CH3OH). pesticide residues.
4.4 Methanol/water mixed solution. 1 4.
4.5 acetonitrile/water mixed solution. 1 4.
4.6 Ammonium acetate solution. C (CH3COONH4) = 0.002 mol/L.
Weigh 0.077 g of ammonium acetate in 500 ml of experimental water and 0.22 μm filter (4.13).
4.7 Sulfuric acid (H2SO4). ρ (H2SO4) = 1.84 g/ml.
4.8 Sodium hydroxide (NaOH).
4.9 Sulfuric acid solution. 1 1.
Measure 50 ml of concentrated sulfuric acid (4.7) and slowly add to 50 ml of water.
4.10 Sodium hydroxide solution. ρ (NaOH) = 0.4 g/ml.
Weigh 40 g of sodium hydroxide (4.8) in water and set to 100 ml.
4.11 solid phase extraction column. filler for the divinyl benzene and N-vinyl pyrrolidone copolymer (HLB) or the same column efficiency of the extraction column, specifications for the 6
Ml/500 mg.
4.12 Nitrogen. Purity ≥99.99%.
4.13 Filtration. 0.22 μm Teflon or other material equivalent filter.
5 instruments and equipment
5.1 solid phase extraction device. automatic or manual, flow rate can be adjusted.
5.2 Concentration device. KD concentrator or nitrogen blowing concentrator and other equipment equivalent performance.
5.3 Liquid Chromatography/Tandem Mass Spectrometer. Equipped with electrospray ionization source (ESI).
5.4 Column. C18 or equivalent reversed-phase high performance liquid chromatography column with reference specifications of 100 mm × 2.1 mm, 1.7 μm.
5.5 Microinjectors. 10 μl, 50 μl, 100 μl, 250 μl.
5.6 Common laboratory equipment and equipment.
6 samples
6.1 sample collection
Samples were collected with reference to the relevant provisions of HJ/T 91 and HJ/T 164.
Fresh water was collected with a pre-washed clean and dry milled brown glass bottle (250 ml).
6.2 Sample storage
Collected water samples 0 ℃ ~ 4 ℃ dark preservation, 3 days analysis is completed.
6.3 Preparation of the sample
6.3.1 Direct injection method
Mix 1.0 ml of water, add the internal standard solution 5.0 μl (4.1.4), mix and filter through the 0.22 μm filter (4.13), placed in the sample
Bottle, to be tested.
6.3.2 Solid phase extraction method
The solid phase extraction column (4.11) was activated with 10 ml of methanol (4.3) and 10 ml of experimental water to ensure the stigma infiltration. Measure 100
Ml water sample, using a sulfuric acid solution (4.9) or sodium hydroxide solution (4.10) to adjust the pH to neutral water, water samples below 10 ml/min
(About 3 to 4 drops/second) flow rate through the column. The volume of the waste water sample can be appropriately reduced according to the actual situation. Mix the solution with 10 ml of methanol/water
(4.4) Leave the column to remove the weaker impurities on the column. Followed by purging with nitrogen (4.12) and drying the column. And then 10 ml of a
Alcohol (4.3) The column was eluted at a flow rate of about 3 ml/min (about 1 drop/sec), and the eluate was received in the collection tube. The eluate was blown through nitrogen (4.12,
Pay attention to keep the liquid slightly fluctuate) to dry, dry with acetonitrile/water solution (4.5) to 1.0 ml, and finally add the internal standard liquid
5.0 μl (4.1.4), after mixing 0.22 μm filter (4.13), placed in the sample bottle, to be tested.
6.4 Preparation of blank sample
6.4.1 Lab blank
The samples were prepared in the same manner as in the water treatment (6.3.1) to prepare a blank sample with direct injection.
The solid phase extraction method was prepared according to the same procedure of water sample treatment (6.3.2) instead of the sample.
6.4.2 Full program blank
Before sampling, follow the sample collection (6.1) and sample preservation (6.2) method, with the experimental water preparation of the whole program blank sample, and with it
The sampling process is brought to the sampling site. The whole program blanks the sample with the actual sample and reaches the laboratory at the same time.
7 Analysis steps
7.1 Instrument reference conditions
7.1.1 Liquid Chromatographic Reference Conditions
Mobile phase. 0.002 mol/L ammonium acetate aqueous solution (A phase), acetonitrile (B phase), gradient elution program in Table 1.
Flow rate. 0.3 ml/min.
Column temperature. 40 ° C.
Injection volume. 10 μl.
Table 1 Liquid Chromatography Mobile Phase Gradient Elution Procedure
Time (min) A% B%
6.5 80 20
7.1.2 Mass Spectral Reference Conditions
Negative ion mode
Capillary voltage. 2.8 kV
Ion source temperature. 120 ° C
Atomization temperature. 350 ° C
Atomized gas flow rate. 800 L/h
Reverse blow flow rate. 10 L/h
Collision air flow rate. 0.10 ml/min
Multi-ion reaction monitoring mode (MRM), the specific conditions in Table 2.
Table 2 Monitoring conditions for the multi-ion reaction of the target compound
The compound parent ion (m/z)
Ion
(M/z)
Dwell time/s tap hole voltage/V collision voltage/V
199 * 141 20 15
2-methyl-4-chlorophenoxyacetic acid
0.02
219 * 161 16 12
2,4-dichlorophenoxyacetic acid
0.02
213 * 141 20 15 2- (2-methyl-4-chlorophenoxy
Yl) propionic acid 215 143
0.02
233 * 161 16 12 2- (2,4-dichlorophenoxy)
- propionic acid 235 163
0.02
253 * 195 16 12
2,4,5-trichlorophenoxyacetic acid
0.02
267 * 195 16 10 2- (2,4,5-trichlorophenoxy)
Yl) -propionic acid 269 197
0.02
247 * 161 10 10 4- (2,4-Dichlorophenoxy) -
Butyric acid 249 163
0.02
227 * 141 15 12 4- (2-methyl-4-chlorophenoxy
Yl) butyric acid 229 143
0.02
225 * 167 15 12 2,4-dichlorophenoxyacetic acid
-13C6 227 169
0.02
Note. with the * for the quantitative ion pair, for different mass spectrometry equipment, the parameters may be different, should be measured before the mass spectrometry parameters to optimize the best.
7.1.3 Instrument tuning
According to the instrument manual in the specified time and frequency of liquid chromatography/tandem mass spectrometer for the quality of the instrument and the sensitivity correction,
To ensure that the instrument is in the best test state.
In the course of the use of the instrument, if the instrument found that the quality of significant deviation or a significant decline in sensitivity, the instrument should be immediately re-
Perform quality and sensitivity correction.
7.2 Calibration
7.2.1 Drawing of calibration curves
(4.1.2) in a mixed solution of acetonitrile/water (4.5), at least 5 concentration points were prepared.
The standard concentrations of phenoxy carboxylic acids were 1.0 μg/L, 2.0 μg/L, 5.0 μg/L, 10.0 μg/L, 50.0 μg/L and 100 μg/L, respectively
(This is the reference concentration), in each standard solution of the standard solution by adding 5.0 μl standard internal standard liquid (4.1.4), so that the internal standard mass concentration
For 50.0 μg/L, stored in a brown sample vial, to be tested.
From the low concentration to the high concentration, the standard series solution was sequentially injected with the concentration of the target component in the standard series solution as the abscissa
The calibration curve is established by plotting the ratio of the peak area (or peak height) to the peak area of the internal standard (or peak height) and the product of the internal standard concentration.
The calibration curve has a correlation coefficient ≥0.995, otherwise the calibration curve is redrawn.
Y = ax b (1)
Where. x - target component concentration, μg/L
Y - the product of the peak area (or peak height) ratio of the target component and the internal standard substance and the concentration of the internal standard substance
A - calibration curve slope
B - calibration curve intercept
7.2.2 Liquid Chromatography/Mass Spectrometry
Fig.1 Total ion chromatogram (concentration. 50 μg/L) of liquid chromatography/mass spectrometry of 8 phenoxy carboxylic acid herbicides and internal standard
Note. 1. 2-Methyl-4-chlorophenoxyacetic acid; 2,3. 2,4-dichlorophenoxyacetic acid, 2,4-dichlorophenoxyacetic acid-13C6; 4. 2- (2- 4-chlorophenoxy) propionic acid;
5. 2- (2,4-dichlorophenoxy) -propionic acid; 6. 2,4,5-trichlorophenoxyacetic acid; 7. 2- (2,4,5-trichlorophenoxy) - propionic acid; 8. 4- (2,4-dichlorophenoxy) -but
Acid; 9. 4- (2-methyl-4-chlorophenoxy) butyric acid
7.3 Determination
7.3.1 Specimen determination
The same instrumental analysis conditions were used to determine the calibration curve.
7.3.2 Blank test
The measurement of the blank sample (6.4) was carried out according to the same instrument analysis condition (7.1) as the test sample.
Calculation and representation of results
8.1 Qualitative analysis of the target compound
Each of the tested components was selected for 1 parent ion and 2 daughter ions for monitoring. Under the same experimental conditions, the components of the sample to be tested
The absolute value of the relative standard deviation should be less than 2.5% compared to the retention time of the target component in the standard sample; and the sample spectrum
In the figure, the relative abundance (Ksam) of the qualitative ions of each component is the relative relative abundance of the qualitative ions in the standard solution spectrum close to the concentration
(Kstd), the deviation does not exceed the range specified in Table 3, and it can be determined that there is a corresponding analyte in the sample.
(2)
Where. Ksam - the relative abundance of qualitative ions in a sample in a sample,%
A2 - the peak area (or peak height) of the qualitative ion pair of a group in the sample
A1 - the peak area (or peak height) of the quantitative ion pair of a component in the sample
(3)
Where. Kstd - the relative abundance of qualitative ions in a standard sample,%
Astd2 - the peak area (or peak height) of the qualitative ion pair of a group in the standard sample
Astd1 - the peak area (or peak height) of the quantitative ion pair of a component in the standard sample
Table 3 Qualitative confirmation of the maximum allowable deviation of the relative abundance of ions
unit.%
A qualitative ion of a component in a standard sample
Relative ion abundance (Kstd)
Kstd> 50 20 < Kstd ≤ 50 10 < Kstd ≤ 20 Kstd ≤ 10
The relative ionization of a component in a sample
The maximum allowable deviation of ion abundance (Ksam)
± 20 ± 25 ± 30 ± 50
8.2 Quantitative analysis of the target compound
The target compound is qualitatively identified and quantified by the standard curve method or the average response factor method according to the peak area of the quantitative ion.
8.3 Calculation of results
8.3.1 Standard curve method
According to the peak area of phenoxy carboxylic acid herbicides in the sample, the corresponding peak area of internal standard and the concentration of internal standard were calculated according to formula (4)
The concentration of phenoxy carboxylic acid herbicides in the sample.
(4)
Where. ρi - mass concentration of target component i in the sample, μg/L;
Ai - the peak area (or peak height) of the target component i in the sample;
Ais - the peak area (or peak height) of the internal standard in the sample;
Ρis - the concentration of the internal standard in the sample, μg/L;
A - the slope of the standard curve;
B - the intercept of the standard curve;
V1 - volume after volume, ml;
V - water sample volume, ml.
8.3.2 Average Response Factor Method
Using the average response factor method, according to the formula (5) ~ (7) calculation.
(5)
(6)
(7)
Where. ρi - mass concentration of target component i in the sample, μg/L;
Ai - the peak area (or peak height) of the target component i in the sample;
Ais - the peak area (or peak height) of the internal standard in the sample;
Ρis - the concentration of the internal standard in the sample, μg/L;
V1 - volume after volume, mL;
V - water sample volume, mL;
RRF - the relative response of the target in the standard series, dimensionless;
RRF - the average response factor of the target, dimensionless;
N - standard series points.
8.3 results show
Direct injection method. When the determination is greater than or equal to 10.0μg/L, the data retained three significant digits; when the result is less than 10.0μg/L,
To one after the decimal point;
Solid phase extraction method. When the determination is greater than or equal to 1μg/L, the retention of three significant figures. When the determination result is less than 1 μg/L, the number
It is reserved for three after the decimal point.
9 precision and accuracy
9.1 precision
9.1.1 Direct injection method
Six labs were used for the concentration of phenoxy carboxylic acid herbicides at concentrations of 1.0 μg/L, 10.0 μg/L and 50.0 μg/L, respectively.
6 repeated measurements.
The relative standard deviations in the laboratory were 2.4% ~ 13.9%, 1.1% ~ 7.3%, 2.0% ~ 6.6% respectively.
The relative standard deviations were 1.5% ~ 6.8%, 0.6% ~ 4.8%, 0.7 ~ 4.2%, respectively.
The reproducibility limits were. 0.2μg/L ~ 0.3μg/L, 0.9μg/L ~ 1.4μg/L, 5.1μg/L ~ 6.3μg/L.
The reproducibility limits were. 0.2μg/L ~ 0.3μg/L, 1.1μg/L ~ 1.5μg/L, 5.3μg/L ~ 7.4μg/L.
9.1.2 Solid phase extraction
6 laboratories with a concentration of 0.050μg/L of phenoxy carboxylic acid herbicides, 0.500μg/L and 1.00μg/L of the uniform blank sample
Line six times to repeat the determination.
The relative standard deviations in the laboratory were 1.4% ~ 8.9%, 0.6% ~ 3.3% and 0.4% ~ 1.8% respectively.
The relative standard deviations were 1.2% ~ 2.1%, 0.2% ~ 0.8%, 0.2% ~ 0.6%, respectively.
The limit of reproducibility was 0.005μg/L ~ 0.007μg/L, 0.018μg/L ~ 0.031μg/L, 0.019μg/L ~ 0.032μg/L.
The reproducibility limits were. 0.005μg/L ~ 0.007μg/L, 0.019μg/L ~ 0.033μg/L, 0.02μg/L ~ 0.033μg/L.
9.2 Accuracy
9.2.1 Direct injection method
Six laboratories were tested for surface water and waste water, and the spiked concentrations were 10.0 μg/L and 50.0 μg/L, respectively. Spiked recovery rate
The results were. 88.0% ~ 102%, 87.5% ~ 102%, the final recoveries were 90.8% ± 5.2% ~ 99.8% ± 3.6%
93.3% ± 4.2% ~ 97.5% ± 8.0%.
9.2.2 Solid phase extraction
Six laboratories carried out spike recovery experiments on surface water. The spiked concentrations were 0.100 μg/L and 1.00 μg/L, respectively.
The results showed that the titer was 2.00μg/L and 20.0μg/L, respectively. The recoveries of spiked were 74.2%
89.2%, 75.2% ~ 89.9%, and the final recoveries were 75.9% ± 1.4% ~ 87.5% ± 3.0% and 76.4 ± 1.4% ~ 89.3% ± 1.0%.
The accuracy and accuracy of the results are given in Appendix B.
10 quality assurance and quality control
10.1 blank analysis
Each analysis is done at least one lab blank and full program blank. To check for possible interference.
The concentration of each target compound in the laboratory blank and the program blank should not exceed the detection limit of the method, otherwise it should be resampled.
10.2 Determination of parallel samples
A parallel sample is to be analyzed for every 20 samples or for each batch (less than 20 samples/batch). The relative standard deviation of the parallel samples should be controlled
20% or less.
10.3 matrix spikes
Approximately 20 samples or per batch (less than 20 samples/batch) need to be a matrix plus standard sample. The range of recoveries should be determined by direct injection
Between 85% and 110%, the recoveries of the solid phase extraction were between 70% and 120%.
10.4 Calibration
10.4.1 Initial calibration
The initial calibration is required for the initial use of the instrument, or when the instrument is repaired, the column is replaced, or the continuous calibration is not acceptable. That is to establish the standard
Quasi-curve.
10.4.2 Continuous calibration
Continuous calibration was performed using the intermediate concentration point of the analytical calibration curve, 1 for every 20 samples or per batch (less tha...
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