CN106268258B - A method of absorbing liquid and mercury fume demercuration for mercury fume demercuration - Google Patents
A method of absorbing liquid and mercury fume demercuration for mercury fume demercuration Download PDFInfo
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- CN106268258B CN106268258B CN201610801749.5A CN201610801749A CN106268258B CN 106268258 B CN106268258 B CN 106268258B CN 201610801749 A CN201610801749 A CN 201610801749A CN 106268258 B CN106268258 B CN 106268258B
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- mercury
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/64—Heavy metals or compounds thereof, e.g. mercury
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/10—Oxidants
- B01D2251/108—Halogens or halogen compounds
Abstract
The invention discloses a kind of absorbing liquid for mercury fume demercuration and the methods of mercury fume demercuration, the absorbing liquid includes iodide ion, thiourea, two sulphur carbonamidines and odium stearate component, by mercury fume and the absorbing liquid haptoreaction, Elemental Mercury and oxidation state mercury in mercury fume enter in the absorbing liquid, efficient removal while Elemental Mercury and oxidation state mercury in mercury fume may be implemented, especially suitable for handling high mercury flue gas, to the removal efficiency of mercury 90% or more.
Description
Technical field
The present invention relates to a kind of absorbing liquid of mercury fume demercuration and its applications in mercury fume demercuration, more particularly to
A method of Elemental Mercury and mercury oxide being removed simultaneously for mercury fume based on absorbing liquid, particularly suitable for lead, zinc, copper, nickel
Equal heavy metals flue gas during smelting；Belong to pyrometallurgy fume treatment technical field.
Background technique
Since mercury has the characteristics that bioconcentration, global propagated, high toxicity make mercury pollution have become the whole world and get over
Come the environmental problem more paid close attention to.In 2013, more than 80 a countries including China signed the " Minamata about mercury in the whole world
Pact ", it is intended to reduce global mercury emissions.China is global mercury emissions big country, and considered critical mercury emissions are inevitable.Non-ferrous metal
Smelting industry is one of China main atmosphere mercury emissions source, newest " the lead-zinc smelting atmosphere that national environmental protection portion issues
Pollutant emission standard " in clear stipulaties mercury discharge be no more than 0.05mg/Nm3, this just proposes flue gas during smelting demercuration technology
Strict requirements.
Usually there are three types of forms for traditional mercury in flue gas: gaseous elemental mercury, gaseous state bivalent mercury and particle mercury.Usual particulate form
Mercury can remove in electrostatic precipitation or bag-type dust.Water-soluble gaseous state bivalent mercury is gone usually using wet scrubbing technology
It removes.Due to the insoluble of gaseous elemental mercury so that it is difficult to remove in existing flue gas purifying technique.The simple substance that do not can be removed
Mercury is largely evaporate into atmosphere, causes mercury pollution, therefore how to realize the removal constituent reduction mercury emissions of Elemental Mercury in flue gas
Critical issue.
Upper common special demercuration technology mainly includes calomel method, potassium iodide method etc. both at home and abroad, but these methods have demercuration
It is at high cost, the disadvantages of low concentration mercury fume can not be handled.Most of smelting enterprises, China are all de- without special flue gas at present
Mercury technique is all to utilize cooperation-removal during existing flue gas desulfurization and denitrification, not high to Elemental Mercury removal efficiency.This
Outside, that there are also mercury contents is high, fluctuation is big, SO for flue gas during smelting2The features such as content is high, these all cause prior art to be extremely difficult to mercury
Emission compliance.In order to reach mercury emissions standard, Chinese patent (CN 103111182A) proposes a kind of lime containing sodium hypochlorite
Solution oxide absorbs mercury, but is difficult to overcome high-content SO2Influence.Chinese patent (CN 103877844A) proposes one simultaneously
Kind of glyoxaline ion liquid and hydrogen peroxide mix novel mercury adsorption liquid, but the cost of ionic liquid valuableness greatly limit value
It is applied.Therefore developing a kind of cheap effective mercury in flue gas absorbing liquid that recycles becomes the task of top priority of flue gas demercuration.
Summary of the invention
In order to solve deficiency existing for traditional flue gas during smelting demercuration method, mesh of the invention is intended to provide one kind can be efficient
The absorbing liquid of Elemental Mercury and oxidation state mercury in mercury fume is removed simultaneously.
Another object of the present invention is to be to provide the method for being used for mercury fume demercuration based on the absorbing liquid, the party
Method efficiently can remove Elemental Mercury and oxidation state mercury in mercury fume simultaneously, and use scope is wide, low for equipment requirements, and subsequent place
Reason is simple, is widely applicable to various mercury fume washing, purifying treatment processes.
In order to achieve the above technical purposes, the present invention provides a kind of absorbing liquid for mercury fume demercuration, the absorptions
Liquid includes iodide ion (I-), thiourea, two sulphur carbonamidines and odium stearate component.
In technical solution of the present invention, absorb in formula of liquid thiourea mainly as mercury ligand, contained by sulphur
Urea functional group can efficiently be complexed with mercury, form stable mercury complex, can efficiently realize the removal of oxidation state mercury；Firmly
For resin acid sodium mainly as the surfactant of absorbing liquid, effect is to increase gas-liquid contact time in washing process, de- to improve
Mercury efficiency；For two sulphur carbonamidines mainly as the oxidant of gaseous elementary mercury, iodide ion promotes elemental mercury efficiency and oxidation rate,
Synergistic function is generated between the two, and the efficient oxidation of element mercury may be implemented.Meanwhile the presence of iodide ion can be with thiocarbamide
Class compound plays the role of cooperateing with ligand complex oxidizing elemental mercury, and element mercury in flue gas can be promoted fast and efficiently to be absorbed
Liquid absorbs.Specific reaction is as follows:
Hg2++4SC(NH2)2=Hg [SC (NH2)2]4 2+
Hg0+FDS+I-+2H+=Hg [SC (NH2)2]In 2-n(wherein two sulphur carbonamidines are referred to as FDS)
Present invention firstly provides the sides using iodide ion and thiourea collaboration complexing removal flue gas during smelting gaseous mercury
The efficient oxidation removing of mercury may be implemented in method under the conditions of existing for the two sulphur carbonamidine of oxidant.
Preferred scheme includes following components: iodide ion: 0.01~0.05mol in every liter of absorbing liquid；Thiourea chemical combination
Object: 0.1~0.6mol；Two sulphur carbonamidines: 0.005~0.015mol；Odium stearate: 0.001~0.003mol.This is preferably absorbed
Formula of liquid optimizes the proportion between each component, and elemental mercury may be implemented in the synergistic ability between strengthening ingredient
It is applied widely with the efficient removal of oxidation state mercury.
More preferably scheme, thiourea include at least one of thiocarbamide, bis-thiourea, thiosemicarbazides.
More preferably scheme, absorbing liquid are acid solution, and most preferred pH is 0.5~4.5.
The present invention also provides a kind of methods for being used for mercury fume demercuration based on the absorbing liquid, and this method is will to contain
Mercury flue gas and the absorbing liquid haptoreaction, Elemental Mercury and oxidation state mercury in mercury fume enter the absorbing liquid.
Preferred scheme, the temperature of absorbing liquid is within the scope of 15~75 DEG C.
Preferred scheme, the pH of absorbing liquid are 0.5~4.5.
The volume ratio of preferred scheme, absorbing liquid and mercury fume is 1:500~2000.The absorbability of absorbing liquid is strong,
Absorptive capacity is big, is adapted to the demercuration processing of different mercury content flue gases.
Preferred scheme, mercury content is 0.1~30mg/Nm in mercury fume3；Other predominant gas in the mercury fume
Volume percent content are as follows: O20.1%~15%；N240%~80%；SO20.01%~5%；CO20%~10%.
Preferred scheme, mercury fume demercuration are realized by spray absorber.
More preferably scheme, mercury fume are passed through in spray absorber from spray-absorption tower bottom, and from spray absorber
The absorbing liquid counter current contacting of top penetrating is reacted, and the Elemental Mercury and oxidation state mercury in mercury fume enter in absorbing liquid, and realization contains
Mercury flue gas demercuration.
Compared with the prior art, it is the advantages of technical solution of the present invention:
1, absorption formula of liquid through the invention can be realized simultaneously the efficient removal of Elemental Mercury and oxidation state mercury in flue gas.
2, by the complexing that cooperates with of iodide ion and thiourea, two sulphur carbonamidine Elemental Mercury of oxidant can be by two
The efficient oxidation of sulphur carbonamidine removes, and total demercuration efficiency is stablized 90% or more.
3, the present invention requires smoke components low, is suitable for the neck of the high mercury fume treatment of the metal smelts such as copper, lead, zinc
Domain is suitable for wet scrubbing purifying smoke process.
4, absorbing liquid of the invention saturation suction mercury quantity is big, and demercuration is at low cost, conducive to the subsequent processing of absorbing liquid.
5, absorbing liquid of the invention is lower to mercury in flue gas content requirement, has for higher and lower mercury content higher
Recovering effect, it is only necessary to it is easy to operate according to flue gas mercury content appropriate adjustment liquid absorption element.
Detailed description of the invention
[Fig. 1] is absorbing liquid under different thiocarbamide contents of the invention to the inhalation effects curve of oxidation state state mercury in flue gas
Figure.
[Fig. 2] is absorption of the absorbing liquid to elemental mercury in flue gas under different iodide ions of the invention and two sulphur carbonamidine contents
Influence curve figure.
[Fig. 3] is the inhalation effects curve graph of different absorbing liquid components of the invention to elemental mercury in flue gas.
[Fig. 4] is absorbing liquid application schematic diagram of the invention.
Specific embodiment
Following embodiment is intended to further illustrate the content of present invention, rather than limits the claims in the present invention protection scope.
Embodiment 1
The temperature for the flue gas that this implementation uses is 45 DEG C, the Contents of Main Components (volume) of flue gas: SO24%, O25%,
Hg2+1mg/Nm3, remaining is N2.Mercury adsorbent solution washes ingredient: the content of thiourea be respectively 0.1mol/L,
0.2mol/L, 0.3mol/L, iodide ion content 0.01mol/L, washing pH value of solution is 2.0, and two sulphur carbonamidine contents are
0.01mol/L, odium stearate 0.001mol/L.It is 500mL that the mercury fume that gas flow is 1L/min, which is passed through liquor capacity,
Washing solution simulated flue gas washing process, reaction time 60min.After washing, the removal effect of mercury in flue gas such as Fig. 1
It is shown.From figure 1 it appears that mercury adsorbent solution removes dimercurion in flue gas when thiocarbamide content is 0.1mol/L
Except efficiency is 97% or more, with the increase of thiocarbamide content, mercury removal efficiency increases, when thiocarbamide content increases to 0.3mol/L
When, oxidation state mercury removal efficiency is 99% or more.Result above it can be shown that novel mercury adsorbent solution in high-sulfur flue gas during smelting
Oxidation state mercury has good removal effect.
Embodiment 2
The temperature for the flue gas that this implementation uses is 35 DEG C, the Contents of Main Components (volume) of flue gas: SO24%, O25%,
Hg0 450μg/Nm3, CO23%, remaining is N2.Mercury adsorbent solution washes ingredient: the content of thiourea is 0.2mol/
L, iodide ion content are respectively 0.01mol/L, 0.02mol/L, 0.03mol/L, and washing pH value of solution is 1.5, two sulphur carbonamidine contents
It is divided into 0.01mol/L, odium stearate 0.002mol/L.The mercury fume that gas flow is 0.6L/min, which is passed through liquor capacity, is
The washing solution simulated flue gas washing process of 500mL, reaction time 60min.After washing, the removal effect of mercury in flue gas
As shown in Figure 2.From figure 2 it can be seen that mercury adsorbent solution has higher removal efficiency to elemental mercury, when iodide ion content is
0.03mol/L and two sulphur carbonamidine contents are 0.015mol/L, and the removal efficiency of Elemental Mercury is 90% or more at this time.Result above can
To show that novel mercury adsorbent solution also has preferable removal effect to elemental mercury in high-sulfur flue gas during smelting.Embodiment 3
The temperature for the flue gas that this implementation uses is 25 DEG C, the Contents of Main Components (volume) of flue gas: SO22%, O26%,
Hg0 450μg/Nm3, CO23%, remaining is N2.Mercury adsorbent solution washes ingredient: the content of thiourea is 0.2mol/
L, iodide ion content 0.01mol/L, washing pH value of solution be 1.5, two sulphur carbonamidine contents be respectively 0,0.005mol/L,
0.01mol/L, 0.015mol/L, odium stearate content are 0.002mol/L.The mercury fume for being 0.6L/min by gas flow
It is passed through the washing solution simulated flue gas washing process that liquor capacity is 500mL, reaction time 60min.As a result, it has been found that working as solution
In be free of two sulphur carbonamidines when, which is only 64.5% to the removal effect of Elemental Mercury, but 0.005mol/L is added in solution
After two sulphur carbonamidines, it is 85.8% that the removal efficiency of Elemental Mercury, which rises rapidly, and with the increase of two sulphur carbonamidine contents, Elemental Mercury is gone
Except rate is continuously increased, when two sulphur carbonamidine contents are to 0.015mol/L, the removal efficiency of Elemental Mercury is up to 90% or more.The above knot
Fruit shows that two sulphur carbonamidine of oxidant can greatly promote the removal efficiency of Elemental Mercury.
Embodiment 4
The temperature for the flue gas that this implementation uses is 35 DEG C, the Contents of Main Components (volume) of flue gas: SO22%, O26%,
Hg0 450μg/Nm3, CO23%, remaining is N2.Following three kinds of mercury adsorbent solutions are configured to wash: (1) thiourea complex cleaning solution,
I.e. content containing thiourea is respectively 0.1 5mol/L, and washing pH value of solution is 1.5, and two sulphur carbonamidine contents are divided into 0.01mol/
L, odium stearate 0.002mol/L, wherein being free of iodide ion；(2) iodide ion complex compound cleaning solution, i.e. iodide ion content are
0.01mol/L, is free of thiourea content, and other ingredients are identical as (1)；(3) thiocarbamide+iodide ion complex compound cleaning solution,
That is thiourea content
0.15mol/L, iodide ion content 0.01mol/L, other ingredients are identical with (1).It is 0.6L/ by gas flow
The mercury fume of min is passed through the washing solution simulated flue gas washing process that liquor capacity is 500mL, reaction time 60min.Through
After crossing washing, the removal effect of mercury in flue gas is as shown in Figure 3.Independent iodide ion or thiocarbamide effect complex ion realize element mercury
Oxidation removal effect is all bad, is only 23.8% and 52.8% to simple substance mercury removal efficiency；After the two is compound, complex ion it
Between generate synergistic effect, promote the removal of Elemental Mercury, removal efficiency can reach 90% or more.
Embodiment 5
The temperature for the flue gas that this implementation uses is 35 DEG C, the Contents of Main Components (volume) of flue gas: SO24%, O25%,
Hg0 450μg/Nm3, Hg2+1mg/Nm3,CO23%, remaining is N2.Mercury adsorbent solution washes ingredient: thiourea contains
Amount is respectively 0.1mol/L, and iodide ion content is divided into 0.01mol/L, and washing pH value of solution is 1.5, and two sulphur carbonamidine contents are divided into
0.01mol/L, odium stearate 0.002mol/L.The mercury fume that gas flow is 1.5L/min, which is passed through liquor capacity, is
The washing solution simulated flue gas washing process of 500mL, reaction time 60min.After mercury adsorbent solution, oxidation state in flue gas
Mercury and elemental mercury have all obtained effective removal, and wherein oxidation state mercury removal efficiency 98% or more, imitate by the removal of elemental mercury
Rate is 89% or more, and comprehensive flue gas total mercury removal efficiency is 95% or more.
Claims (9)
1. a kind of absorbing liquid for mercury fume demercuration, it is characterised in that: include following components in every liter of absorbing liquid:
Iodide ion: 0.01~0.05mol；
Thiourea: 0.1~0.6mol；
Two sulphur carbonamidines: 0.005~0.015mol；
Odium stearate: 0.001~0.003mol.
2. the absorbing liquid according to claim 1 for mercury fume demercuration, it is characterised in that: the Thiourea chemical combination
Object includes at least one of thiocarbamide, bis-thiourea, thiosemicarbazides.
3. the method for being used for mercury fume demercuration based on absorbing liquid of any of claims 1 or 2, it is characterised in that:
By mercury fume and the absorbing liquid haptoreaction, Elemental Mercury and oxidation state mercury in mercury fume enter the absorbing liquid
In.
4. the method according to claim 3 for being used for mercury fume demercuration based on absorbing liquid, it is characterised in that:
The temperature of the absorbing liquid is within the scope of 15~75 DEG C.
5. the method according to claim 3 for being used for mercury fume demercuration based on absorbing liquid, it is characterised in that:
The pH of the absorbing liquid is 0.5~4.5.
6. the method according to claim 3 for being used for mercury fume demercuration based on absorbing liquid, it is characterised in that:
The volume ratio of the absorbing liquid and mercury fume is 1:500~2000.
7. the method according to claim 6 for being used for mercury fume demercuration based on absorbing liquid, it is characterised in that:
Mercury content is 0.1~30mg/Nm in the mercury fume3；
Other predominant gas volume percent contents in the mercury fume are as follows:
8. the method according to claim 3 for being used for mercury fume demercuration based on absorbing liquid, it is characterised in that:
Mercury fume demercuration is realized by spray absorber.
9. the method according to claim 8 for being used for mercury fume demercuration based on absorbing liquid, it is characterised in that:
Mercury fume is passed through in spray absorber from spray-absorption tower bottom, inverse with the absorbing liquid that sprays into from spray-absorption top of tower
Stream contact is reacted, and the Elemental Mercury and oxidation state mercury in mercury fume enter in absorbing liquid, realizes mercury fume demercuration.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN103097495A (en) * | 2010-09-16 | 2013-05-08 | 雪佛龙美国公司 | Process, method, and system for removing heavy metals from fluids |
| CN105073643A (en) * | 2013-03-14 | 2015-11-18 | 雪佛龙美国公司 | Process, method, and system for removing heavy metals from fluids |
| CN105289261A (en) * | 2015-11-20 | 2016-02-03 | 中南大学 | Washing liquid for eluting mercury in mercury-containing flue gas and method for recovering mercury form mercury-containing flue gas |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103097495A (en) * | 2010-09-16 | 2013-05-08 | 雪佛龙美国公司 | Process, method, and system for removing heavy metals from fluids |
| CN105073643A (en) * | 2013-03-14 | 2015-11-18 | 雪佛龙美国公司 | Process, method, and system for removing heavy metals from fluids |
| CN105289261A (en) * | 2015-11-20 | 2016-02-03 | 中南大学 | Washing liquid for eluting mercury in mercury-containing flue gas and method for recovering mercury form mercury-containing flue gas |
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