CN103146440A - Method for controlling emission of polycyclic aromatic hydrocarbons in coal-based gases - Google Patents
Method for controlling emission of polycyclic aromatic hydrocarbons in coal-based gases Download PDFInfo
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- CN103146440A CN103146440A CN2013100699577A CN201310069957A CN103146440A CN 103146440 A CN103146440 A CN 103146440A CN 2013100699577 A CN2013100699577 A CN 2013100699577A CN 201310069957 A CN201310069957 A CN 201310069957A CN 103146440 A CN103146440 A CN 103146440A
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Abstract
The invention discloses a method for controlling the emission of polycyclic aromatic hydrocarbons in coal-based gases, belongs to the technical field of air pollution control, and relates to a technical scheme of catalytically cracking sixteen polycyclic aromatic hydrocarbons such as benzopyrene which are contained in coal-based gases and strictly monitored to be emitted to the environment. The method is characterized in that a plurality of high-performance oxide catalysts are utilized to catalytically crack polycyclic aromatic hydrocarbons such as benzopyrene in the coal-based gases, so that the purpose of controlling polycyclic aromatic hydrocarbon emission is realized. By utilizing the method, the catalytic reaction temperature, catalyst granularity and catalyst usage are reasonably controlled, and the polycyclic aromatic hydrocarbons are effectively degraded. Moreover, the catalysts have the characteristics of high removal efficiency, low cost, no secondary pollution and the like.
Description
Technical field
The present invention is a kind of controls the method for polycyclic aromatic hydrocarbons discharging in coal-based gas, belongs to the air pollution control technique field, relate to in coal-based gas by 16 kinds of polycyclic aromatic hydrocarbonss of environment key monitoring the method by cracking with the technical scheme of its content reduction.
Background technology
Polycyclic aromatic hydrocarbon compounds (Polycyclic Aromatic Hydrocarbons PAHs) is the organic pollutant that a class extensively exists in surrounding medium, and they extensively exist in environment, and the mankind healthy had strong teratogenesis, carcinogenic nature.They can be attached to the particulate matter surface and are directly sucked by human body or affect HUMAN HEALTH by food chain.In the waste that the industry such as coke gas, low temperature pyrogenation coal gas, Coal Liquefaction, organic chemical industry, petroleum industry, steel-making ironmaking are discharged, considerable polycyclic aromatic hydrocarbons is arranged.Wherein in coking industry, due in production process in various degree exist the furnace binding tightness bad, the ground dedusting purification system is not very perfect, the discharging of the polycyclic aromatic hydrocarbonss such as benzopyrene is the most serious.Monitoring data shows, in the waste water that discharges in coke gas industry as the benzopyrene of polycyclic aromatic hydrocarbons contaminated index, content can up to 25.4 ~ 46ug/L, be much higher than the national standard of 0.03ug/L.According to World Health Organization's research report, in atmosphere, BaP content 2ng is carcinogenic limit content, and some coking zone benzopyrene content of China are higher than 60 to 100 times of ultimate values.There are data to show that one 600,000 tons coke-oven plants approximately discharge more than 30 kilogram of BaP every year, be about 2.75 hundred million tons according to China's coke year output in 2006, and according to relevant report per kilogram BaP to approximately 1,200,000 yuan of social indirect economic loss, the quantity discharged of being not difficult to find out the benzopyrene that derives from coking is not only to the serious harm environment but also national economy is caused damage.Therefore the quantity discharged of controlling the polycyclic aromatic hydrocarbonss such as benzopyrene in pyrolysis coal gas is significant.At present the improvement method of polycyclic aromatic hydrocarbons mainly contained biological restoration, UV photodissociation method, advanced oxidation processes, ultrasonic decomposition method and the catalytic cracking method etc.And biological restoration, UV photodissociation method, advanced oxidation processes, ultrasonic decomposition method all can not be controlled from root the discharging of polycyclic aromatic hydrocarbons.Therefore in industrial application, catalystic pyrolysis is the most effectively to administer method.
Summary of the invention
A kind of method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas of the present invention, purpose is as effectively controlling the problem of environmental pollution in China's gas industry, thereby provides a kind of efficient catalyzer to come the technical scheme of the benzopyrene polycyclic aromatic hydrocarbons that produces in cracking pyrolysis coal gas.
A kind of method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas of the present invention, it is characterized in that a kind of utilization thermo-cracking instrument, gas-chromatography and mass spectrometric hyphenated technique, after 16 kinds of polycyclic aromatic hydrocarbonss of benzopyrene of being monitored by the environment emphasis in coal-based gas are introduced oxide catalyst and are carried out cracking its content is reduced in the exit, entering the GC-MS system detects online, effectively control the method for the quantity discharged of benzopyrene polycyclic aromatic hydrocarbons, its concrete technology step is:
I, raw coal sample preparation are collected
Coal sample is Pingshuo Coal, first coal sample is carried out fragmentation, grinding and screening before experiment, collects 100-120 purpose sample, sieve former coal sample for next step;
II, oxide catalyst sample preparation are collected
Oxide catalyst is magnesium oxide, calcium oxide or ferric oxide, and oxide compound is carried out fragmentation, grinding and screening, collects 60-160 purpose sample, sieve oxide catalyst for next step;
The pre-treatment of III, former coal sample
In the crystalline silica cracking tube of CDS cracking instrument special use, the quartz pushrod 3 of first packing into, then insert silica wool 2 and do support, the 1mg that then packs into processes the former coal sample 1 of collecting, silica wool 2 fixed samples of packing at last through I;
The pre-treatment of IV, oxide catalyst sample
In the crystalline silica cracking tube of CDS cracking instrument special use, the quartz pushrod 3 of first packing into, insert again silica wool 2 and do support, then pack successively 0.4-0.8mg into through II. process the different types of oxide compound sample 4 and the 1mg that collect and process the former coal sample 1 of collecting through I, and between separate with silica wool 2, the silica wool 2 of packing on coal sample top at last fixes sample;
V, the former coal sample of use thermo-cracking instrument pyrolysis
Pack into the cracking tube of former coal sample of III is put into the thermo-cracking instrument and carried out pyrolysis, and temperature rise rate is 10 ℃/ms, heats to 600-800 ℃, and the pyrolysis gas that produce this moment enters into GC-MS and automatically carries out on-line analysis;
Polycyclic aromatic hydrocarbons in the thermo-cracking instrument cracking pyrolysis gas of VI, use interpolation catalyzer
Cracking tube through the pretreated raw coal pyrolysis gas outlet of IV place's introducing catalyzer is carried out pyrolysis, temperature rise rate is 10 ℃/ms, heat to 600-800 ℃, consequent pyrolysis gas carries out on-line analysis automatically through entering into GC-MS after the effect of catalyzer;
VII, the benzopyrene polycyclic aromatic hydrocarbons that pyrolysis is produced carry out quantitative analysis
Benzopyrene polycyclic aromatic hydrocarbons after utilizing the external standard method benzopyrene polycyclic aromatic hydrocarbons that former pyrolysis of coal produces to V and VI process catalyst action on GC-MS carries out quantitative analysis, the PAHs amount and the raw coal pyrolysis product that draw former pyrolysis of coal generation are measured through the PAHs after catalyzer, and then calculate the transformation efficiency of polycyclic aromatic hydrocarbons according to this amount, its calculation formula is:
X=
。
A kind of above-mentioned method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas, it is characterized in that described magnesian working conditions is: temperature is 600 ℃, and particle diameter is 140 ~ 160 orders, and consumption is 0.6mg, its transformation efficiency to polycyclic aromatic hydrocarbons is 62.15%.
A kind of above-mentioned method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas, it is characterized in that the working conditions of described calcium oxide is: temperature is 700 ℃, and particle diameter is 60 ~ 80 orders, and consumption is 0.4mg, and its transformation efficiency to polycyclic aromatic hydrocarbons is 52.88%.
A kind of above-mentioned method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas, it is characterized in that the working conditions of described ferric oxide is: temperature is 600 ℃, and particle diameter is 60 ~ 80 orders, and consumption is 0.4mg, and its transformation efficiency to polycyclic aromatic hydrocarbons is 60.59%.
A kind of method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas of the present invention, compared with prior art, significantly advantage is:
(1) reasonably control the operational conditions such as temperature that catalyzer uses, granularity, quality, realize the catalytic pyrolysis of the polycyclic aromatic hydrocarbons such as benzopyrene, can effectively reduce its content in pyrolysis coal gas, have higher transformation efficiency.
(2) oxide catalyst that uses not only catalytic efficiency is higher, and cheap, in use operate and install simple, and non-secondary pollution.
(3) this catalyzer is applicable to control the discharging of polycyclic aromatic hydrocarbons in different coal-based gas.
Description of drawings
Fig. 1. former pyrolysis of coal dress sample loading mode.
Fig. 2. the raw coal pyrolysis gas outlet fills sample loading mode after introducing catalyzer.
The former coal sample of code name title 1-in institute's diagram, 2-silica wool, 3-quartz pushrod, 4-oxide compound sample.
Embodiment
I, raw coal sample preparation are collected
First Pingshuo Coal is carried out fragmentation, grinding and screening before experiment, collects 100 purpose samples, sieve former coal sample for next step;
II, catalyst sample are processed and are collected
The MgO catalyzer is carried out fragmentation, grinding and screening, collects 140 purpose samples, sieve the MgO catalyzer for next step;
The pre-treatment of III, former coal sample
In the crystalline silica cracking tube of CDS cracking instrument special use, in the mode of Fig. 1, the quartz pushrod 3 of first packing into, then insert silica wool 2 and do support, the 1mg that then packs into processes the former coal sample 1 of collecting, silica wool 2 fixed samples of packing at last through I;
The pre-treatment of IV, catalyst sample
In the crystalline silica cracking tube of CDS cracking instrument special use, mode with Fig. 2, the quartz pushrod 3 of first packing into, insert again silica wool 2 and do support, then pack successively 0.4-0.8mg into through II. process the MgO sample and the 1mg that collect and process the former coal sample 1 of collecting through I, and between separate with silica wool 2, the silica wool 2 of packing on coal sample top at last fixes sample;
V, the former coal sample of use thermo-cracking instrument pyrolysis
Pack into the cracking tube of former coal sample of III is put into the thermo-cracking instrument and carried out pyrolysis, and temperature rise rate is 10 ℃/ms, heats to 600 ℃, and the pyrolysis gas that produce this moment enters into GC-MS and automatically carries out on-line analysis;
Polycyclic aromatic hydrocarbons in the thermo-cracking instrument cracking pyrolysis gas of VI, use interpolation catalyzer
Cracking tube through the pretreated raw coal pyrolysis gas outlet of IV place's introducing MgO is carried out pyrolysis, and temperature rise rate is 10 ℃/ms, heats to 600 ℃, and consequent pyrolysis gas carries out on-line analysis automatically through entering into GC-MS after the effect of catalyzer;
VII, the polycyclic aromatic hydrocarbonss such as benzopyrene that pyrolysis is produced carry out quantitative analysis
The polycyclic aromatic hydrocarbons such as the benzopyrene that former pyrolysis of coal is produced and former pyrolysis of coal utilize external standard method to carry out quantitative analysis through the polycyclic aromatic hydrocarbonss such as benzopyrene after catalyzer, and the transformation efficiency that calculates polycyclic aromatic hydrocarbons is 62.15%.Wherein the transformation efficiency of the polycyclic aromatic hydrocarbons of each number of rings sees the following form:
I, raw coal sample preparation are collected
First Pingshuo Coal is carried out fragmentation, grinding and screening before experiment, collects 120 purpose samples, sieve former coal sample for next step;
II, catalyst sample are processed and are collected
The CaO catalyzer is carried out fragmentation, grinding and screening, collects 80 purpose samples, sieve the CaO catalyzer for next step;
The pre-treatment of III, former coal sample
In the crystalline silica cracking tube of CDS cracking instrument special use, in the mode of Fig. 1, the quartz pushrod 3 of first packing into, then insert silica wool 2 and do support, the 1mg that then packs into processes the former coal sample 1 of collecting, silica wool 2 fixed samples of packing at last through I;
The pre-treatment of IV, catalyst sample
In the crystalline silica cracking tube of CDS cracking instrument special use, mode with Fig. 2, the quartz pushrod 3 of first packing into, insert again silica wool 2 and do support, then pack successively 0.4-0.8mg into through II. process the CaO sample and the 1mg that collect and process the former coal sample 1 of collecting through I, and between separate with silica wool 2, the silica wool 2 of packing on coal sample top at last fixes sample;
V, the former coal sample of use thermo-cracking instrument pyrolysis
Pack into the cracking tube of former coal sample of III is put into the thermo-cracking instrument and carried out pyrolysis, and temperature rise rate is 10 ℃/ms, heats to 700 ℃, and the pyrolysis gas that produce this moment enters into GC-MS and automatically carries out on-line analysis;
Polycyclic aromatic hydrocarbons in the thermo-cracking instrument cracking pyrolysis gas of VI, use interpolation catalyzer
Cracking tube through the pretreated raw coal pyrolysis gas outlet of IV place's introducing CaO is carried out pyrolysis, and temperature rise rate is 10 ℃/ms, heats to 700 ℃, and consequent pyrolysis gas carries out on-line analysis automatically through entering into GC-MS after the effect of catalyzer;
VII, the polycyclic aromatic hydrocarbonss such as benzopyrene that pyrolysis is produced carry out quantitative analysis
The polycyclic aromatic hydrocarbons such as the benzopyrene that former pyrolysis of coal is produced and former pyrolysis of coal utilize external standard method to carry out quantitative analysis through the polycyclic aromatic hydrocarbonss such as benzopyrene after catalyzer, and the transformation efficiency that calculates polycyclic aromatic hydrocarbons is 52.88%.Wherein the transformation efficiency of the polycyclic aromatic hydrocarbons of each number of rings sees the following form:
I, raw coal sample preparation are collected
First Pingshuo Coal is carried out fragmentation, grinding and screening before experiment, collects 120 purpose samples, sieve former coal sample for next step;
II, catalyst sample are processed and are collected
To Fe
2O
3Catalyzer carries out fragmentation, grinding and screening, collects 70 purpose samples, sieve Fe
2O
3Catalyzer is for next step;
The pre-treatment of III, former coal sample
In the crystalline silica cracking tube of CDS cracking instrument special use, in the mode of Fig. 1, the quartz pushrod 3 of first packing into, then insert silica wool 2 and do support, the 1mg that then packs into processes the former coal sample 1 of collecting, silica wool 2 fixed samples of packing at last through I;
The pre-treatment of IV, catalyst sample
In the crystalline silica cracking tube of CDS cracking instrument special use, in the mode of Fig. 2, the quartz pushrod 3 of first packing into, then insert silica wool 2 and do support, then pack successively 0.4-0.8mg into through II. process the Fe that collects
2O
3The former coal sample 1 that sample and 1mg process to collect through I, and between separate with silica wool 2, the silica wool 2 of packing on coal sample top at last fixes sample;
V, the former coal sample of use thermo-cracking instrument pyrolysis
Pack into the cracking tube of former coal sample of III is put into the thermo-cracking instrument and carried out pyrolysis, and temperature rise rate is 10 ℃/ms, heats to 600 ℃, and the pyrolysis gas that produce this moment enters into GC-MS and automatically carries out on-line analysis;
VI, interpolation catalyzer thermo-cracking polycyclic aromatic hydrocarbons
To introduce Fe through the pretreated raw coal pyrolysis gas outlet of IV place
2O
3Cracking tube carry out pyrolysis, temperature rise rate is 10 ℃/ms, heats to 600 ℃, consequent pyrolysis gas carries out on-line analysis automatically through entering into GC-MS after the effect of catalyzer;
VII, the polycyclic aromatic hydrocarbonss such as benzopyrene that pyrolysis is produced carry out quantitative analysis
The polycyclic aromatic hydrocarbons such as the benzopyrene that former pyrolysis of coal is produced and former pyrolysis of coal utilize external standard method to carry out quantitative analysis through the polycyclic aromatic hydrocarbonss such as benzopyrene after catalyzer, and the transformation efficiency that calculates polycyclic aromatic hydrocarbons is 60.59%.Wherein the transformation efficiency of the polycyclic aromatic hydrocarbons of each number of rings sees the following form:
| The PAHs number of rings | Transformation efficiency (%) |
| 2 rings | 55.37 |
| 3 rings | 56.66 |
| 4 rings | 70.49 |
| 5 rings | 54.9 |
| 6 rings | 0 |
Claims (4)
1. control the method that in pyrolysis coal gas, polycyclic aromatic hydrocarbons discharges for one kind, it is characterized in that a kind of utilization thermo-cracking instrument, gas-chromatography and mass spectrometric hyphenated technique, after 16 kinds of polycyclic aromatic hydrocarbonss of benzopyrene of being monitored by the environment emphasis in coal-based gas are introduced oxide catalyst and are carried out cracking its content is reduced in the exit, entering the GC-MS system detects online, effectively control the method for the quantity discharged of benzopyrene polycyclic aromatic hydrocarbons, its concrete technology step is:
I, raw coal sample preparation are collected
Coal sample is Pingshuo Coal, first coal sample is carried out fragmentation, grinding and screening before experiment, collects 100-120 purpose sample, sieve former coal sample for next step;
II, oxide catalyst sample preparation are collected
Oxide catalyst is magnesium oxide, calcium oxide or ferric oxide, and oxide compound is carried out fragmentation, grinding and screening, collects 60-160 purpose sample, sieve oxide catalyst for next step;
The pre-treatment of III, former coal sample
In the crystalline silica cracking tube of CDS cracking instrument special use, the quartz pushrod (3) of first packing into, then insert silica wool (2) and do support, the 1mg that then packs into processes the former coal sample (1) of collecting, silica wool (2) fixed sample of packing at last through I;
The pre-treatment of IV, oxide catalyst sample
In the crystalline silica cracking tube of CDS cracking instrument special use, the quartz pushrod (3) of first packing into, insert again silica wool (2) and do support, then pack successively 0.4-0.8mg into through II. process the different types of oxide compound sample (4) and the 1mg that collect and process the former coal sample (1) of collecting through I, and between separate with silica wool (2), the silica wool (2) of packing on coal sample top at last fixes sample;
V, the former coal sample of use thermo-cracking instrument pyrolysis
Pack into the cracking tube of former coal sample of III is put into the thermo-cracking instrument and carried out pyrolysis, and temperature rise rate is 10 ℃/ms, heats to 600-800 ℃, and the pyrolysis gas that produce this moment enters into GC-MS and automatically carries out on-line analysis;
Polycyclic aromatic hydrocarbons in the thermo-cracking instrument cracking pyrolysis gas of VI, use interpolation catalyzer
Cracking tube through the pretreated raw coal pyrolysis gas outlet of IV place's introducing catalyzer is carried out pyrolysis, temperature rise rate is 10 ℃/ms, heat to 600-800 ℃, consequent pyrolysis gas carries out on-line analysis automatically through entering into GC-MS after the effect of catalyzer;
VII, the benzopyrene polycyclic aromatic hydrocarbons that pyrolysis is produced carry out quantitative analysis
Benzopyrene polycyclic aromatic hydrocarbons after utilizing the external standard method benzopyrene polycyclic aromatic hydrocarbons that former pyrolysis of coal produces to V and VI process catalyst action on GC-MS carries out quantitative analysis, the PAHs amount and the raw coal pyrolysis product that draw former pyrolysis of coal generation are measured through the PAHs after catalyzer, and then calculate the transformation efficiency of polycyclic aromatic hydrocarbons according to this amount, its calculation formula is:
X=
。
2. according to a kind of described method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas of claim 1, it is characterized in that described magnesian working conditions is: temperature is 600 ℃, particle diameter is 140 ~ 160 orders, and consumption is 0.6mg, and its transformation efficiency to polycyclic aromatic hydrocarbons is 62.15%.
3. according to a kind of described method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas of claim 1, the working conditions that it is characterized in that described calcium oxide is: temperature is 700 ℃, particle diameter is 60 ~ 80 orders, and consumption is 0.4mg, and its transformation efficiency to polycyclic aromatic hydrocarbons is 52.88%.
4. according to a kind of described method of controlling polycyclic aromatic hydrocarbons discharging in pyrolysis coal gas of claim 1, the working conditions that it is characterized in that described ferric oxide is: temperature is 600 ℃, particle diameter is 60 ~ 80 orders, and consumption is 0.4mg, and its transformation efficiency to polycyclic aromatic hydrocarbons is 60.59%.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104130799A (en) * | 2014-08-04 | 2014-11-05 | 太原理工大学 | Coal tar catalytic upgrading method |
-
2013
- 2013-03-06 CN CN2013100699577A patent/CN103146440A/en active Pending
Non-Patent Citations (1)
| Title |
|---|
| 张京: "金属氧化物对煤热解过程中多环芳烃排放的影响", 《硕士学位论文》 * |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104130799A (en) * | 2014-08-04 | 2014-11-05 | 太原理工大学 | Coal tar catalytic upgrading method |
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Application publication date: 20130612 |