CN105136940A - Determining method for initial boiling point and final boiling point of coking-light benzene - Google Patents
Determining method for initial boiling point and final boiling point of coking-light benzene Download PDFInfo
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- CN105136940A CN105136940A CN201510670824.4A CN201510670824A CN105136940A CN 105136940 A CN105136940 A CN 105136940A CN 201510670824 A CN201510670824 A CN 201510670824A CN 105136940 A CN105136940 A CN 105136940A
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- boiling point
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Abstract
The invention discloses a determining method for an initial boiling point and a final boiling point of coking-light benzene. The determining method comprises the steps that a capillary tube gas chromatographic method is used for separating and determining a light benzene sample to be determined; the benzene pre-component content sum sigma pre-benzene is calculated; the p-xylene post-component content sum sigma post-p-xylene is calculated; initial boiling point data and final boiling point data are recorded through a light benzene sample distillation test; the initial boiling point data and the corresponding sigma pre-benzene are tabulated to obtain a first regression curve equation; the final boiling point data and the corresponding sigma post-p-xylene are tabulated to obtain a second regression curve equation; the initial boiling point and the final boiling point of the light benzene boiling range are calculated in the light benzene determination process by means of the gas chromatographic method on the basis of the first regression curve equation and the second regression curve equation. The method is high in accuracy, rapid and convenient to implement and free of pollution, and only needs 15 min; the working intensity of analysts can be relieved, the working environment can be improved, the working efficiency can be improved, and the body health of detection personnel is ensured.
Description
Technical field
The present invention relates to a kind of assay method of coking-light benzene boiling range, the assay method of especially a kind of coking-light benzene initial boiling point and the end point of distillation.
Background technology
Light benzene is the crude benzene vapor fractionation come by dephlegmator by two benzene towers, the detection Main Basis GB/T2282-2000 " mensuration of coker light oil series products boiling range " of current light benzene, this method advantage is that accuracy is higher, reproducible, but also there is complex operation, analysis time long (general more than 50 minutes), still-process is seriously polluted, artifical influence factor is many, and the hypertoxic benzene-like compounds grievous injury analyst produced in still-process is healthy.Because this analytical approach exists above-mentioned drawback, incompatible to the requirement of technical progress with modern enterprise, therefore innovate assay method, meet needs of production imperative.And vapor-phase chromatography has defined the trend of alternative manual method as the technological means that Analysis of Organic Substances is commonly used at many analysis fields, therefore innovating Gas Chromatographic Method mensuration light benzene boiling range has been advance the modern necessary means of analytical technology.
Summary of the invention
The technical problem to be solved in the present invention is to provide a kind of quick, pollution-free, light benzene initial boiling point of handling safety and the assay method of the end point of distillation.
For solving the problems of the technologies described above, the step of assay method of the present invention is: the assay method of a kind of coking-light benzene boiling range initial boiling point and the end point of distillation, and the step of this assay method is:
1) capillary gas chromatography is adopted to carry out separation determination to light benzene sample to be measured;
2) area percentage method is adopted to carry out accurate quantitative analysis to component each in light benzene sample;
3) calculating is summed up to chromatogram analysis data; First component concentration sum before calculating benzene, records this data Σ
before benzene, secondly component concentration sum after calculating P-xylene, records this data Σ
after P-xylene;
4) get above-mentioned light benzene sample to detect by the way of distillation, record initial boiling point data and end point of distillation data;
5) the light benzene sample of different initial boiling point and the end point of distillation is gathered, by step 1) ~ 4) test figure of each light benzene sample of method record;
6) by the initial boiling point data that obtain and corresponding Σ thereof
before benzenetabulation, then makes scatter diagram, for this scatter diagram makes Trendline; The first regression curve equation is obtained by this Trendline;
7) by the end point of distillation data that obtain and corresponding Σ thereof
after P-xylenetabulation, then makes scatter diagram, for this scatter diagram makes Trendline; The second regression curve equation is obtained by this Trendline;
8) utilize the first regression curve equation and the second regression curve equation, initial boiling point and the end point of distillation of light benzene can be calculated in the vapor-phase chromatography of light benzene.
In step of the present invention (1), the condition determination of capillary gas chromatography is: high pure nitrogen is carrier gas, post flow is 1.5 ~ 2.5mL/min, before post, pressure is 0.06 ~ 0.09Mpa, hydrogen flowing quantity is 30 ~ 60mL/min, air mass flow is 300 ~ 400mL/min, make-up gas is 30 ~ 35mL/min, and split ratio is 30: 1 ~ 60: 1.
In step of the present invention (1), the condition determination of capillary gas chromatography is: chromatographic column is fused-silica capillary column, temperature programme: initial temperature 60 DEG C, keep 3min, with 10 DEG C/min ramp to 120 DEG C, keep 0min, continue with 40 DEG C/min ramp to 220 DEG C, keep 2.5min.
In step of the present invention (1), the condition determination of capillary gas chromatography is: gasification temperature is 250 DEG C, and detected temperatures is 250 DEG C.
In step of the present invention (1), the condition determination of capillary gas chromatography is: carrier gas is high pure nitrogen, post flow is 1.5mL/min, before post, pressure is 0.07Mpa, hydrogen flowing quantity is 30mL/min, air mass flow is 300mL/min, make-up gas flow is 30mL/min, split ratio 50: 1.
In step of the present invention (1), the detecting device of capillary gas chromatography is hydrogen flame detector.
In step of the present invention (6) and step (7), utilize Excel to tabulate and derive regression curve equation.
The coefficient R of the first regression curve equation in step of the present invention (6)
2be 0.95 ~ 1.
The coefficient R of the second regression curve equation in step of the present invention (7)
2be 0.95 ~ 1.
The light benzene sample way of distillation of the present invention detects presses GB/T2282-2000 " mensuration of coker light oil series products boiling range " detection.
Know-why of the present invention: the present invention utilizes capillary gas chromatography and light benzene initial boiling point-chromatogram relation curve, the end point of distillation-chromatogram relation curve to calculate light benzene initial boiling point and the end point of distillation, produces in order to instruct light benzene.The present invention is mainly relatively fixing according to light benzene component, and the chromatogram elution order of each component arranges from low to high by component boiling point, consistent with component elution order in light benzene distillation process, consistent by the principle of the different separation component of boiling point from rectification column.Before its benzene, component concentration and initial boiling point have good linear relationship, and after its P-xylene, component concentration and the end point of distillation have good linear relationship.The linear relationship equation that can derive by experiment calculates initial boiling point and the end point of distillation of light benzene, realizes new assay method and is connected with original assay method result is on all four.
The beneficial effect adopting technique scheme to produce is: first the present invention determines light benzene initial boiling point-chromatogram relation curve and the end point of distillation-chromatogram relation curve; Adopt capillary gas chromatography, utilize above-mentioned two curves, initial boiling point and the end point of distillation of light benzene can be detected fast.The inventive method accuracy is high, fast, convenient, pollution-free; Analyst's working strength can be alleviated, improve working environment, increase work efficiency, ensure that testing staff's is healthy; The whole analytic process of the present invention simultaneously only needs 15 minutes, is applicable to coal chemical enterprise fast pace, become more meticulous the requirement regulated, and is a kind of analytical approach being applicable to extensively promoting.
Accompanying drawing explanation
Fig. 1 is the gas chromatogram of light benzene in the present invention;
Fig. 2 is light benzene initial boiling point temperature of the present invention and chromatographic data graph of relation;
Fig. 3 is light benzene end point temperature of the present invention and chromatographic data graph of relation.
Embodiment
Below in conjunction with the drawings and specific embodiments, the present invention is further detailed explanation.
Embodiment 1
The accuracy testing of the assay method of light benzene initial boiling point and the end point of distillation in tar:
(1) under selected experiment condition, taken amount gets the light benzene sample of 2mL in 12mL sample bottle, get 0.2 μ L Sample Injection after shaking up and (before note sample, suck a certain amount of air in gas chromatograph, the volatilization of noting benzene in sample process is avoided to bring error), can obtain corresponding chromatogram, its chromatogram is shown in Fig. 1.Its selected experiment condition is: detecting device is hydrogen flame detector, chromatographic column is HP-5MS fused-silica capillary column (30m × 0.25mm × 0.25 μm), temperature programme: initial temperature 60 DEG C, keep 3min, with 10 DEG C/min ramp to 120 DEG C, keep 0min, continue with 40 DEG C/min ramp to 220 DEG C, keep 2.5min, amount to 14min.Vaporizer is 250 DEG C, and detecting device is 250 DEG C, split ratio 50: 1, and carrier gas is high pure nitrogen, and post flow is 1.5mL/min, and before post, pressure is 0.07Mpa, and hydrogen flowing quantity is 30mL/min, and air mass flow is 300mL/min, and make-up gas flow is 30mL/min.
(2) adopt area percentage method to carry out accurate quantitative analysis to each component in Fig. 1 light benzene, it the results are shown in Table 1.
Each measured portions result (area percentage method) in table 1 light benzene
(3) before utilizing the benzene in Excel his-and-hers watches 1, component concentration (not comprising benzene) sums up calculating, is designated as Σ
before benzene=0.96, after P-xylene, component concentration sum (not comprising P-xylene) sums up calculating, is designated as Σ
after P-xylene=2.89.
(4) do distillation test by the way of distillation simultaneously.Get in the above-mentioned light benzene sample of 100mL and cucurbit and do distillation test, record initial boiling point and the end point of distillation on request.And carry out temperature correction on request, after correction, initial boiling point is: 78.8 DEG C, and the end point of distillation is: 145.4 DEG C.
(5) strive for the light benzene sample (being no less than 100) gathering different initial boiling point and the end point of distillation, initial boiling point scope contains some data inside and outside production control claimed range, and end point of distillation scope contains some data inside and outside production control claimed range.All samples is pressed (1) ~ (4) methods experiment and records Σ
before benzene, initial boiling point, Σ
right after dimethylbenzeneand the end point of distillation.
(6) by representative initial boiling point data and corresponding Σ thereof
before benzenetabulate in Excel, as table 2:
Table 2
| Initial boiling point DEG C | 77.6 | 78.2 | 78.8 | 79.2 | 80.0 |
| Σ Before benzene％ | 1.09 | 1.02 | 0.96 | 0.91 | 0.80 |
(7) utilize drafting instrument to make scatter diagram (Fig. 2), simultaneously for this scatter diagram makes Trendline, utilize Excel to be that this Trendline calculates and adds the first regression curve equation.First regression curve equation and the linear relationship between light benzene initial boiling point and chromatographic data.
First regression curve equation is y=-8.343x+86.736, and slope is-8.343, coefficient R
2be 0.9956, coefficient R is 0.9978, and coefficient R, more close to 1, represents that the reliability of this equation is better, proves initial boiling point and Σ
before benzenebetween there is good linear relationship, can Σ be used
before benzenedata derivation light benzene initial boiling point.
(8) by representative end point of distillation data and corresponding Σ thereof
after P-xylenetabulate in Excel, as table 3:
Table 3
| The end point of distillation DEG C | 132.0 | 136.6 | 141.3 | 145.4 | 148.6 | 150.0 | 154.0 | 157.0 | 172.0 |
| Σ After P-xylene | 1.52 | 1.82 | 2.54 | 2.89 | 3.03 | 3.22 | 3.44 | 3.7 | 5.11 |
(9) utilize drafting instrument to make scatter diagram (Fig. 3), simultaneously for this scatter diagram makes Trendline, utilize Excel to be that this Trendline calculates and adds the second regression curve equation.Second regression curve equation and the linear relationship between the light benzene end point of distillation and chromatographic data.
Second regression curve equation is y=11.175x+114.68, and slope is 11.175, R
2be 0.9908, R be 0.9954, prove the end point of distillation and Σ
after P-xylenebetween there is good linear relationship, can Σ be used
after P-xylenethe data derivation light benzene end point of distillation.
(10) according to the linear equation that step (7), (9) are derived, determine to replace the way of distillation by vapor-phase chromatography.
(11) choose 20 samples representing different initial boiling point and the end point of distillation and carry out distillation test and chromatography test respectively, analysis result is added up, in table 4
Table 4 distillation test and chromatography test contrast
As can be seen from Table 4, the initial boiling point that this assay method utilizes chromatogram analog computation to go out, the end point of distillation are substantially identical with the initial boiling point that the way of distillation obtains, the end point of distillation, maximum error is no more than 2 DEG C, regulation precision≤2.0 DEG C in GB/T2282-2000 " mensuration of coker light oil series products boiling range ", visible instrument analytical method meets the precision that former method requires to reach, and can replace the way of distillation completely.
Embodiment 2
Get 2mL light benzene sample in 12mL sample bottle, 0.2 μ L Sample Injection is got in chromatograph after shaking up, obtain corresponding chromatogram, utilize the first regression curve equation y=-8.343x+86.736 in embodiment 1 and the second regression curve equation y=11.175x+114.68 result of calculation; Calculate Σ
before benzene=0.98, corresponding initial boiling point is 78.6 DEG C; Calculate Σ
after P-xylene=2.86, the end point of distillation is 146.6 DEG C.
In sum, this assay method key is to have found the good linear corresponding relation between chromatographic data and distillation data; But linear formula is not fixing, because various places operating personnel there are differences and the difference in geographic position, the temperature of same sample initial boiling point and the end point of distillation also can produce fine difference; This assay method provides a kind of like this operation thinking finding linear relationship, those of ordinary skill in the art can modify to technical scheme of the present invention or equivalent replacement, and not departing from the spirit and scope of technical solution of the present invention, it all should be encompassed in the middle of right of the present invention.
Claims (9)
1. an assay method for coking-light benzene boiling range initial boiling point and the end point of distillation, is characterized in that, the step of this assay method is:
1) capillary gas chromatography is adopted to carry out separation determination to light benzene sample to be measured;
2) area percentage method is adopted to carry out accurate quantitative analysis to component each in light benzene sample;
3) calculating is summed up to chromatogram analysis data; First component concentration sum before calculating benzene, records this data Σ
before benzene, secondly component concentration sum after calculating P-xylene, records this data Σ
after P-xylene;
4) get above-mentioned light benzene sample to detect by the way of distillation, record initial boiling point data and end point of distillation data;
5) the light benzene sample of different initial boiling point and the end point of distillation is gathered, by step 1) ~ 4) test figure of each light benzene sample of method record;
6) by the initial boiling point data that obtain and corresponding Σ thereof
before benzenetabulation, then makes scatter diagram, for this scatter diagram makes Trendline; The first regression curve equation is obtained by this Trendline;
7) by the end point of distillation data that obtain and corresponding Σ thereof
after P-xylenetabulation, then makes scatter diagram, for this scatter diagram makes Trendline; The second regression curve equation is obtained by this Trendline;
8) utilize the first regression curve equation and the second regression curve equation, initial boiling point and the end point of distillation of light benzene can be calculated in the vapor-phase chromatography of light benzene.
2. the assay method of coking-light benzene initial boiling point according to claim 1 and the end point of distillation, it is characterized in that, in described step (1), the condition determination of capillary gas chromatography is: high pure nitrogen is carrier gas, post flow is 1.5 ~ 2.5mL/min, before post, pressure is 0.06 ~ 0.09Mpa, and hydrogen flowing quantity is 30 ~ 60mL/min, and air mass flow is 300 ~ 400mL/min, make-up gas is 30 ~ 35mL/min, and split ratio is 30: 1 ~ 60: 1.
3. the assay method of coking-light benzene initial boiling point according to claim 1 and the end point of distillation, it is characterized in that, in described step (1), the condition determination of capillary gas chromatography is: chromatographic column is fused-silica capillary column, temperature programme: initial temperature 60 DEG C, keep 3min, with 10 DEG C/min ramp to 120 DEG C, keep 0min, continue with 40 DEG C/min ramp to 220 DEG C, keep 2.5min.
4. the assay method of coking-light benzene initial boiling point according to claim 1 and the end point of distillation, is characterized in that, in described step (1), the condition determination of capillary gas chromatography is: gasification temperature is 250 DEG C, and detected temperatures is 250 DEG C.
5. the coking-light benzene initial boiling point according to claim 1-4 any one and the assay method of the end point of distillation, it is characterized in that, in described step (1), the condition determination of capillary gas chromatography is: carrier gas is high pure nitrogen, post flow is 1.5mL/min, before post, pressure is 0.07Mpa, and hydrogen flowing quantity is 30mL/min, and air mass flow is 300mL/min, make-up gas flow is 30mL/min, split ratio 50: 1.
6. the coking-light benzene initial boiling point according to claim 1-4 any one and the assay method of the end point of distillation, is characterized in that, in described step (1), the detecting device of capillary gas chromatography is hydrogen flame detector.
7. the coking-light benzene initial boiling point according to claim 1-4 any one and the assay method of the end point of distillation, is characterized in that: in described step (6) and step (7), utilize Excel to tabulate and derive regression curve equation.
8. the coking-light benzene initial boiling point according to claim 1-4 any one and the assay method of the end point of distillation, is characterized in that: the coefficient R of the first regression curve equation in described step (6)
2be 0.95 ~ 1.
9. the coking-light benzene initial boiling point according to claim 1-4 any one and the assay method of the end point of distillation, is characterized in that: the coefficient R of the second regression curve equation in described step (7)
2be 0.95 ~ 1.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109839495A (en) * | 2019-03-22 | 2019-06-04 | 杭州辛孚能源科技有限公司 | A method of light petroleum fraction boiling range is calculated according to molecular composition |
| CN112630335A (en) * | 2020-12-16 | 2021-04-09 | 马钢奥瑟亚化工有限公司 | Method for determining contents of benzene, toluene and xylene in coal tar light oil fraction |
| CN113671062A (en) * | 2021-07-12 | 2021-11-19 | 包头钢铁（集团）有限责任公司 | Method for improving detection accuracy of light benzene final distillation point by distillation method |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101587100A (en) * | 2008-11-20 | 2009-11-25 | 武汉钢铁(集团)公司 | Method for determining benzene compounds in coked lean and fat oil by capillary gas chromatography |
| CN102331469A (en) * | 2011-08-09 | 2012-01-25 | 宣化钢铁集团有限责任公司 | Method for determining initial boiling point and final boiling point of three-oil mixture in tar |
| CN103149287A (en) * | 2013-02-04 | 2013-06-12 | 吉林建龙钢铁有限责任公司 | Crude benzene detection method |
-
2015
- 2015-10-15 CN CN201510670824.4A patent/CN105136940A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101587100A (en) * | 2008-11-20 | 2009-11-25 | 武汉钢铁(集团)公司 | Method for determining benzene compounds in coked lean and fat oil by capillary gas chromatography |
| CN102331469A (en) * | 2011-08-09 | 2012-01-25 | 宣化钢铁集团有限责任公司 | Method for determining initial boiling point and final boiling point of three-oil mixture in tar |
| CN103149287A (en) * | 2013-02-04 | 2013-06-12 | 吉林建龙钢铁有限责任公司 | Crude benzene detection method |
Non-Patent Citations (3)
| Title |
|---|
| 徐春梅等: "轻苯初馏点及终点的气相色谱分析", 《昆钢科技》 * |
| 薛笑莉等: "用气相色谱法测定轻苯干点", 《化学分析计量》 * |
| 陈德东等: "轻苯终馏点的色谱分析", 《河北冶金》 * |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109839495A (en) * | 2019-03-22 | 2019-06-04 | 杭州辛孚能源科技有限公司 | A method of light petroleum fraction boiling range is calculated according to molecular composition |
| CN109839495B (en) * | 2019-03-22 | 2021-07-23 | 广东辛孚科技有限公司 | Method for calculating distillation range of light petroleum fraction according to molecular composition |
| CN112630335A (en) * | 2020-12-16 | 2021-04-09 | 马钢奥瑟亚化工有限公司 | Method for determining contents of benzene, toluene and xylene in coal tar light oil fraction |
| CN113671062A (en) * | 2021-07-12 | 2021-11-19 | 包头钢铁（集团）有限责任公司 | Method for improving detection accuracy of light benzene final distillation point by distillation method |
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