CN1389564A - Thiobacillus thiooxidans and biological eliminating method of chromium in tanning sludge - Google Patents
Thiobacillus thiooxidans and biological eliminating method of chromium in tanning sludge Download PDFInfo
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- CN1389564A CN1389564A CN02137921A CN02137921A CN1389564A CN 1389564 A CN1389564 A CN 1389564A CN 02137921 A CN02137921 A CN 02137921A CN 02137921 A CN02137921 A CN 02137921A CN 1389564 A CN1389564 A CN 1389564A
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/20—Sludge processing
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Abstract
The invention relates to sulfur oxide sulfur bacilli and biological eliminating method of chromium in tanning mud. Bacterial strain is named as TS6, preserve mark is CGMCCNO.0759. The method of eliminate chromium in tanning mud by above mentioned sulfur oxide sulfur bacilli is adding 1-3 g/L sulfur into tanning mud in biology reactor, inocualting 10-15% (v/v, the same below) TS6 bacteria strain, stirring, ventilating and subsiding; that 10-20% of subsiding mud backflow to reactor; dehydrating suprplus subsiding mud; adding basic material into liquid part to turn Cr3+ into Cr(OH)3 and subside, sediment is dissolved by sulfuric acid, then there is the tannage stage; solid part is neutralized to agriculture. The elimianting rate of Cr in mud is 95%-100%, reserving rate of nutrient in mud is above 80%.
Description
One, technical field
The present invention relates to the biological eliminating method of chromium in thiobacillus thiooxidans and the leather-making mud, is a technology of utilizing the acidophilia thiobacillus to remove toxic heavy metal chromium in the leather-making mud, belongs to field of environment engineering technology.
Two, background technology
Leather-making mud (Tannery Sludge) is that tannery handles the throw out that produces in the waste water process, and it is the leather-making waste water that main technique is handled that the most of leather-making enterprises of China adopts chemical-biological method.According to China Association of Leather Industry's statistics, China's raw hide amount of finish in 1998 is about 100,000,000 marks to be opened, and the annual wastewater discharge of leather industry is 100,000,000 tons, produces 3,000,000 tons of leather-making muds (in solid content 10%).Leather-making mud contains abundant N (3~5%), P nutritive element and organic matters (about 60%) such as (0.5~1%), is good organic manure resource, and its fertilizer efficiency is equivalent to the fine chicken manure, is better than farm manures such as pig manure.Yet toxic metal Cr content (dry weight) exceeds 250~1000 times of soil background up to 10000~40000 mg/kg in the leather-making mud, but surpasses 10~40 times of the national mud agricultural standards (GB4284-84) that limits, and is a class Hazardous wastes.
At present, the main disposal options of China's leather-making mud is to stack nearby and simple landfill.This not only runs counter to waste and reclaims and the principle of utilizing again, and the chromium in the mud leach liquor can cause a significant threat soil and water surrounding and human and livestock health.Adopt micronucleus test monitoring leather-making mud leach liquor that the result of study of fish erythrocyte micronucleus mutagenesis is shown that the leather-making mud leach liquor has stronger mutagenesis and carcinogenesis.
High-load chromium is the limiting factor of the most critical of restriction leather-making mud resource utilization.Therefore remove that the content of chromium is to realize the leather-making mud resource utilization in the leather-making mud, make leather-making mud become " giving up " prerequisite into " treasured ".Macchi, G. etc. (1991) and Panswad, T. (1995) have proposed the scheme of chromium in the sulfuric acid extraction removal leather-making mud, and its principle is to utilize H
2SO
4Reduce pH with the Cr in dissolving and the lixiviate mud, though this method it can remove Cr at short notice significantly owing to there is acid consumption (about 1 ton of dense H greatly
2SO
4/ ton mud), shortcoming such as secondary pollutants such as processing costs height, severe operational environment, generation hydrogen sulfide and be difficult to be committed to engineering reality.
Application number is that the Chinese patent of 02112924.X has been introduced a method of utilizing thiobacillus ferrooxidant to remove heavy metal in the city sewage and sludge, adopt this method to remove heavy metal in the sewage sludge, Zn, the clearance of Cu reaches 95-100%, the clearance of Cr is more than 90%, yet because the content of Cr is lower in the city sewage and sludge, generally below 1000mg/kg (dry weight), and the composition of leather-making mud and city sewage and sludge have very big difference, the content of Cr is up to 10000~40000mg/kg in the leather-making mud, be 10~40 times of city sewage and sludge, simultaneously because some that also have other in the leather-making mud are unfavorable for that the thiobacillus ferrooxidant growth is stronger with the higher and sour resiliency of factor such as water soluble organic substance content of propagation.Therefore the biological removal that adopts this method to be used for leather-making mud Cr can not be obtained satisfied effect.Also be not specifically designed to microorganism strains and the method for removing chromium in the leather-making mud in the prior art.
Three, summary of the invention
1, goal of the invention: the biological eliminating method that the object of the present invention is to provide chromium in a kind of thiobacillus thiooxidans and the leather-making mud, overcome defectives such as expense height that chemical extraction method in the prior art exists, severe operational environment, generation secondary pollution, adopt biological method to remove toxic heavy metal Cr in the leather-making mud, make the clearance of Cr reach 95%-100%, plant nutrient N, P and organic retention rate are more than 80% in the mud.
2, technical scheme: thiobacillus thiooxidans bacterial strain provided by the invention, called after TS
6, classification number: Thiobacillus Thiobacillus thiooxidans, preserve at China Committee for Culture Collection of Microorganisms common micro-organisms center, and preservation date is on July 4th, 2002, and preservation registration number is CGMCC NO.0759; This characteristic of bacteria is: rod-short, and 0.5 * 1.0 μ m, Gram-negative bacteria, optimum temperuture is 28~35 ℃, appropriate pH 2~6 is aerobic, have a liking for acid, obligate chemoautotrophic bacteria, is characterized in tolerating the Cr of high density
3+And organism, at 1500~5000mg/L Cr
3+Under the condition that exists with 2000~5000mgC/L water soluble organic substance, its propagation generation time is 6.5~8.0 hours.
Thiobacillus ferrooxidant culture condition provided by the invention is:
1, substratum moiety (g/L)
(NH
4)
2SO
40.4; KH
2PO
43.0, CaCl
22H
2O 0.25, MgSO
47H
2O 0.5, FeSO
47H
2O 0.01,1 liter of distilled water.
2, transferring pH with dilute sulphuric acid is 3.0, places reciprocating type shaking table 180rpm shaking culture, and culture temperature is 30~35 ℃.
Utilize above-mentioned thiobacillus thiooxidans to remove the method for chromium in the leather-making mud, it is characterized in that:
1. in bio-reactor, add pending leather-making mud and 1~3g/L elementary sulfur, inoculation 10~20% (v/v) TS
6The thiobacillus thiooxidans bacterial strain is ventilated and stir process 3-6 days, pumps the mud of handling;
2. the mud of above-mentioned processing is through sedimentation, the sedimentation mud of 10-20% is back to replace TS in the bio-reactor
6Bacterial strain usefulness adds pending leather-making mud and 1~3g/L elementary sulfur, circular treatment;
3.80~90% residual settlement mud carries out processed, the liquid phase part that obtains removing the solid phase part of heavy metal and contain heavy metal;
4. the liquid phase part that contains heavy metal is by adding alkaline matter general Cr wherein
3+Become Cr (OH)
3Precipitation, precipitation enters the chrome tanner section behind sulfuric acid dissolution.Used alkaline matter refers to magnesium oxide, sodium bicarbonate, sodium hydroxide or unslaked lime, and wherein best is to use magnesium oxide.
5. remove behind the Cr the solid phase part through with in the alkaline matter and after directly agricultural, or be prepared into fertilizer.Used alkaline matter refers to lime or ammoniacal liquor, and wherein best is to use unslaked lime.
Know-why of the present invention is, with the nutritive substance of the contained inorganic salt of leather-making mud itself as the acidophilia thiobacillus, add the sulphur powder simultaneously as its energy substance, thiobacillus thiooxidans breeds in a large number, the element S of sulfide in the leather-making mud and external source interpolation is oxidized to sulfuric acid, mud medium pH is reduced to below 3.0, and redox potential is increased to 700mV, thereby makes the insoluble Cr (OH) in the mud
3Become the Cr of solubility
3+, remove chromium in the mud by solid-liquid separation then.
3, beneficial effect: the biological eliminating of chromium in the leather-making mud provided by the invention has the following advantages and positively effect:
(1) TS
6Bacterial strain is directly to be separated to from leather-making mud, can tolerate the heavy metal Cr and the organism of high density.Experiment showed, that this bacterial strain can be at 1500~5000mg/L Cr
3+Under the condition that exists with 2000~5000mgC/L water soluble organic substance, utilize the sulphur powder to breed rapidly for energy substance, its propagation generation time is 6.5~8.0 hours.In addition, thiobacillus thiooxidans has begun to be widely used in industrial circles such as hydrometallurgy in the sixties in last century, and is acknowledged as non-pathogenic bacteria, and is harmless to human body and animal;
(2) utilize the biological eliminating method of chromium in the leather-making mud provided by the invention, the clearance of the Cr in the leather-making mud meets pollutent control criterion (GB4284-84) in the agricultural mud fully 95%~100%; After the present invention handled, plant nutrient N, P in the leather-making mud and organic retention rate were more than 80%, and wherein the retention rate of N, P is 80~85%, and organic matter is 85~90%, and the manurial value loss of leather-making mud is less;
(4) after the present invention handles, the small amount of sulfur powder of the sulfide of unborn high density and interpolation is converted into vitriol with 100% in the leather-making mud, therefore no longer exist " back acidifying " effect (to refer to exist in the detoxification mud not elementary sulfur or other reduced sulfur of complete oxidation after the soil utilization of detoxification mud, after this mud is manured into soil, owing to sulfur oxidizing bacterium causes the rapid acidifying phenomenon of soil to the continuation oxidation of reduced sulfur).
(5) invention obtains the Cr in the chromate waste water
3+Generate Cr (OH) through adding alkaline matter
3Post precipitation enters the chrome tanner section again as chrome tanning agent behind sulfuric acid dissolution, thereby realizes the recycle of leather-making enterprises chromium;
(6) with prior art---the sulfuric acid extraction is compared, and the present invention adopts production by biological acid, its reaction temperature and, operating environment close friend does not produce secondary pollution, running cost is cheap.The sulfuric acid extraction is removed in the operating process of chromium in the leather-making mud, and (general add-on is about 1 ton of dense H owing to need add a large amount of mineral acids
2SO
4/ ton mud), the sulfuric acid leather-making mud reaction abundant with containing organic and sulfide produces a large amount of hydrogen sulfide foams and stink, makes severe operational environment.And the present invention utilizes microorganism self metabolism to produce acidifying and oxygenizement, reaction temperature and, no bubble and stink generation;
Four, description of drawings
Accompanying drawing is the schema that thiobacillus thiooxidans is used for the biological eliminating method of leather-making mud chromium.
Embodiment 1:
(1) sampling
Get the concentration basin mud of Haining leather-making waste water treatment plant, this leather-making mud essential property sees Table 1.Table 1 is for the essential property of trial-production leather mud
(2) TS
6Separation of bacterium and enlarged culturing:
Organic the mg/kg------------%------------of pH Cr solid content N P |
??8.05????15900????11.84????3.03?????0.51???54.6 |
Thiobacillus thiooxidans bacterial strain provided by the invention is named as TS
6Classification number: thiobacillus Thiobacillusthiooxidans, in specified depositary institution of Patent Office of the People's Republic of China---preserve at China Committee for Culture Collection of Microorganisms common micro-organisms center, and preservation date is on July 4th, 2002, and preservation registration number is CGMCC NO.0759.This bacterium is characterized as: rod-short, Gram-negative bacteria, single utmost point flagellum, optimum temperuture is 28~35 ℃, appropriate pH 2~6, for aerobic, have a liking for acid, the inorganic chemoautotrophic bacteria of obligate.
This TS
6Bacterium separates from leather-making mud and obtains.Substratum moiety (g/L) is: (NH
4)
2SO
40.4; KH
2PO
43.0, CaCl
22H
2O 0.25, MgSO
47H
2O 0.5, FeSO
47H
2O 0.01,1 liter of distilled water, pH3.0.Its separation method is: draw 20ml mud in the sterilized above-mentioned substratum of 200ml, the 180rpm shaking culture drops to 2.0 to pH in 28 ℃ of reciprocating type shaking tables.Get the above-mentioned culture of 1ml subsequently and carry out doubling dilution to 10
-9, get 10
-4-10
-9Dilution diluent is coated on the flat board, cultivates the faint yellow bacterium colony that occurred the 1-3mm size in 15-20 days on the rear plate.The faint yellow bacterium colony of picking is made bacteria suspension and is done dilution by last method and separate, so repeats after 2 times, and gram stain microscopy, observing size is 0.5 * 1.0 μ m, the rod-short bacterium of form unanimity is the thiobacillus thiooxidans of purifying.Adopt same liquid nutrient medium to carry out the enlarged culturing of this bacterium.Thiobacillus thiooxidans has begun to be widely used in industrial circles such as hydrometallurgy in the sixties in last century, and is acknowledged as non-pathogenic bacteria, and is harmless to human body and animal.
(3) Cr biological eliminating reaction in the leather-making mud
Add the 2.0g/L elementary sulfur, inoculation TS
610% (v/v), the 180rpm shaking culture was handled 4 days in shaking table;
(4) handle the solid-liquid separation of back mud and the recycling of chrome waste liquid
Above-mentioned processing mud obtains chrome waste liquid and takes off the chromium sludge filter cake after centrifugal.Take off the chromium sludge filter cake and meet pollutent control criterion (GB4284-84) in the agricultural mud fully, in unslaked lime and after can as fertilizer sources use.It is 7-8 that chrome waste liquid adds MgO adjusting pH, makes Cr in the chrome waste liquid
3+Become Cr (OH)
3The precipitation, again with behind the sulfuric acid dissolution as chrome tanning agent.
(5) interpretation of result:
(wherein full N adopts semimicro Kelvin nitriding (K for EDWARDS Pirani 501, USA) dry filter cake, and mensuration full N, full P, organic matter and total Cr wherein to adopt the vacuum freezing and drying lyophilization
2SO
4-CuSO
4-Se distillation method); Full P adopts HNO
3-HClO
4Disappear and boil, molybdenum blue colorimetric method is surveyed phosphorus; The outer heating method of potassium bichromate is measured organic; Total Cr adopts three acid (HCl-HNO
3-HClO
4) digestion, the diphenylcarbazide method is measured.According to the difference of Cr and plant nutrient content in the sample before and after the test, the rate of loss of Cr clearance and plant nutrient in the calculating mud.As calculated, the clearance of Cr is 97% in the leather-making mud, and the full N of plant nutrient, full P and organic rate of loss are respectively 16%, 18% and 10%.Table 2 is handled the variation of front and back heavy metal and plant nutrient content for sewage sludge.
Leather-making mud Cr and plant nutrient content before and after table 2 is handled
Before the processing | After the processing |
Organic the mg/kg------------%------------15,900 3.03 0.51 54.6 of the full P of the full N of Cr | Organic mg/kg-------%------477 2.55 0.42 49.1 of the full P of the full N of Cr |
Embodiment 2:
(1) sampling:
Get the concentration basin leather-making mud of Haining leather-making waste water treatment plant, this mud is identical with mud sample among the embodiment 1.
(2) TS
6Separation of bacterium and enlarged culturing:
With embodiment 1.
(3) startup of bio-reactor and operation
In bio-reactor, add the above-mentioned not leather-making mud of dehydration, add the 1g/L elementary sulfur, add above-mentioned TS simultaneously
610% (v/v) stir and aerated culture to start the reaction that microorganism removes Cr, the pH that treats leather-making mud in the biological reactor reduces to (needing 3-5 days) at 2.0 o'clock by 8.05, extract the mud in the bio-reactor out, enter settling bowl and carry out gravity settling, the sedimentation mud of 15% (v/v) is back to bio-reactor again, remaining 85% solid-liquid separation;
(4) recycling of solid-liquid separation and chrome waste liquid
Above-mentioned residual settlement mud obtains chrome waste liquid and takes off the chromium sludge filter cake after centrifugal.Take off the chromium sludge filter cake and meet pollutent control criterion (GB4284-84) in the agricultural mud fully, in unslaked lime and after can as fertilizer sources use.Chrome waste liquid adds NaHCO
3Adjusting pH is 7-8, makes Cr in the chrome waste liquid
3+Become Cr (OH)
3The precipitation, again with behind the sulfuric acid dissolution as chrome tanning agent.
(5) interpretation of result:
(wherein full N adopts semimicro Kelvin nitriding (K for EDWARDS Pirani 501, USA) dry filter cake, and mensuration full N, full P, organic matter and total Cr wherein to adopt the vacuum freezing and drying lyophilization
2SO
4-CuSO
4-Se distillation method); Full P adopts HNO
3-HClO
4Disappear and boil, molybdenum blue colorimetric method is surveyed phosphorus; The outer heating method of potassium bichromate is measured organic; Total Cr adopts three acid (HCl-HNO
3-HClO
4) digestion, the diphenylcarbazide method is measured.According to the difference of Cr and plant nutrient content in the sample before and after the test, the rate of loss of Cr clearance and plant nutrient in the calculating mud.As calculated, the clearance of Cr is 98% in the leather-making mud, and the full N of plant nutrient, full P and organic rate of loss are respectively 19%, 20% and 12%.Table 3 is the variation of sludge treatment front and back heavy metal and plant nutrient content.
Leather-making mud Cr and plant nutrient content before and after table 3 is handled
Embodiment 3:(1) sampling: get the not dewatered sludge of Nanjing tannery, this mud fundamental characteristics sees Table 4.
Before the processing | After the processing |
The organic mg/kg----------%----------15,900 3.03 0.51 54.6 of the full P of the full N of Cr | Organic mg/kg-------%-------318 2.45 0.41 48.1 of the full P of the full N of Cr |
Table 4 is for the fundamental characteristics of trial-production leather mud
PH Cr contains solid N P probability matter mg/kg----------%------------ |
??7.55??19000??9.60??3.48??1.05????60.2 |
(2) TS
6Separation of bacterium and enlarged culturing:
With embodiment 1.
(3) startup of bio-reactor and operation
In bio-reactor, add the above-mentioned not mud of dehydration, add the 3g/L elementary sulfur, add above-mentioned TS
6(10%, v/v) stir and aerated culture to start the reaction of removal of microorganisms heavy metal, the pH that treats sewage sludge in the biological reactor reduces to (needing 3-6 days) at 2.0 o'clock by 7.55, just can extract mud in the bio-reactor out by peristaltic pump, the mud of 20% (v/v) is back to bio-reactor again, and remaining 80% carries out solid-liquid separation through solid-liquid separator;
(4) recycling of solid-liquid separation and chrome waste liquid
Above-mentioned residual settlement mud obtains chrome waste liquid and takes off the chromium sludge filter cake after centrifugal.Take off the chromium sludge filter cake and meet pollutent control criterion (GB4284-84) in the agricultural mud fully, in unslaked lime and after can as fertilizer sources use.It is 7-8 that chrome waste liquid adds MgO adjusting pH, makes Cr in the chrome waste liquid
3+Become Cr (OH)
3The precipitation, again with behind the sulfuric acid dissolution as chrome tanning agent.
(5) interpretation of result:
(wherein full N adopts semimicro Kelvin nitriding (K for EDWARDS Pirani 501, USA) dry filter cake, and mensuration full N, full P, organic matter and total Cr wherein to adopt the vacuum freezing and drying lyophilization
2SO
4-CuSO
4-Se distillation method); Full P adopts HNO
3-HClO
4Disappear and boil, molybdenum blue colorimetric method is surveyed phosphorus; The outer heating method of potassium bichromate is measured organic; Total Cr adopts three acid (HCl-HNO
3-HClO
4) digestion, the diphenylcarbazide method is measured.According to the difference of Cr and plant nutrient content in the sample before and after the test, the rate of loss of Cr clearance and plant nutrient in the calculating mud.As calculated, the clearance of Cr is 98% in the leather-making mud, and the full N of plant nutrient, full P and organic rate of loss are respectively 15%, 16% and 9%.Table 5 is the variation of sludge treatment front and back heavy metal and plant nutrient content.
Leather-making mud Cr and plant nutrient content before and after table 5 is handled
Before the processing | After the processing |
The organic mg/kg----------%-----------19,000 3.48 1.05 60.2 of the full P of the full N of Cr | The organic mg/kg---------%---------380 2.93 0.88 54.8 of the full P of the full N of Cr |
Claims (4)
1, a kind of thiobacillus thiooxidans bacterial strain, called after TS
6, classification number: Thiobacillus Thiobacillusthiooxidans, preserve at China Committee for Culture Collection of Microorganisms common micro-organisms center, and preservation registration number is CGMCC NO.0759; This characteristic of bacteria is: rod-short, and 0.5 * 1.0 μ m, Gram-negative bacteria, optimum temperuture is 28~35 ℃, appropriate pH 2~6 is aerobic, have a liking for acid, obligate chemoautotrophic bacteria, is characterized in tolerating the Cr of high density
3+And organism, at 1500~5000mg/L Cr
3+Under the condition that exists with 2000~5000mgC/L water soluble organic substance, its propagation generation time is 6.5~8.0 hours.
2, utilize the described thiobacillus thiooxidans of claim 1 to remove the method for chromium in the leather-making mud, it is characterized in that:
1) in bio-reactor, adds pending leather-making mud and 1~3g/L elementary sulfur, inoculation 10~20% (v/v) TS
6The thiobacillus thiooxidans bacterial strain is ventilated and stir process 3-6 days, pumps the mud of handling;
2) mud of above-mentioned processing is through sedimentation, the sedimentation mud of 10-20% is back to replace TS in the bio-reactor
6Bacterial strain usefulness adds pending leather-making mud and 1~3g/L elementary sulfur, circular treatment;
3) 80~90% residual settlement mud carries out processed, the liquid phase part that obtains removing the solid phase part of heavy metal and contain heavy metal;
4) contain the liquid phase part of heavy metal by adding alkaline matter general Cr wherein
3+Become Cr (OH)
3Precipitation, precipitation enters the chrome tanner section behind sulfuric acid dissolution;
5) remove behind the Cr the solid phase part through with in the alkaline matter and after directly agricultural, or be prepared into fertilizer.
3, the method for utilizing thiobacillus thiooxidans to remove chromium in the leather-making mud according to claim 2 is characterized in that the alkaline matter that adds refers to magnesium oxide, sodium bicarbonate, sodium hydroxide or unslaked lime in the 4th step, wherein best is to use magnesium oxide;
4, the method for utilizing thiobacillus thiooxidans to remove chromium in the leather-making mud according to claim 2 is characterized in that used alkaline matter is lime or ammoniacal liquor in the 5th step, and wherein best is to use unslaked lime;
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CN107716519A (en) * | 2017-11-07 | 2018-02-23 | 河南科技大学 | A kind of incineration of refuse flyash is innoxious and heavy metal resources method |
CN108529722A (en) * | 2018-04-09 | 2018-09-14 | 中南大学 | A kind of method of biological oxidation, ferromagnetism absorption combined removal cyanide |
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