CN117887963A - Method for microbial leaching of molybdenum ore - Google Patents
Method for microbial leaching of molybdenum ore Download PDFInfo
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- 238000002386 leaching Methods 0.000 title claims abstract description 149
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 title claims abstract description 117
- 229910052750 molybdenum Inorganic materials 0.000 title claims abstract description 85
- 239000011733 molybdenum Substances 0.000 title claims abstract description 85
- 238000000034 method Methods 0.000 title claims abstract description 50
- 230000000813 microbial effect Effects 0.000 title claims abstract description 11
- 241001467578 Microbacterium Species 0.000 claims abstract description 48
- 241000203815 Microbacterium testaceum Species 0.000 claims abstract description 46
- 230000008569 process Effects 0.000 claims abstract description 30
- 239000011449 brick Substances 0.000 claims abstract description 29
- 229910001385 heavy metal Inorganic materials 0.000 claims abstract description 12
- 239000000725 suspension Substances 0.000 claims description 17
- 230000001580 bacterial effect Effects 0.000 claims description 16
- 239000001963 growth medium Substances 0.000 claims description 15
- MYSWGUAQZAJSOK-UHFFFAOYSA-N ciprofloxacin Chemical compound C12=CC(N3CCNCC3)=C(F)C=C2C(=O)C(C(=O)O)=CN1C1CC1 MYSWGUAQZAJSOK-UHFFFAOYSA-N 0.000 claims description 13
- 239000011148 porous material Substances 0.000 claims description 12
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- 238000001764 infiltration Methods 0.000 claims description 5
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- 230000004913 activation Effects 0.000 claims description 4
- 239000002609 medium Substances 0.000 claims description 4
- 239000007788 liquid Substances 0.000 claims description 3
- 229910052770 Uranium Inorganic materials 0.000 claims description 2
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- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 abstract description 4
- 238000010276 construction Methods 0.000 abstract description 4
- 230000007547 defect Effects 0.000 abstract description 4
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- 229910052500 inorganic mineral Inorganic materials 0.000 description 16
- 239000011707 mineral Substances 0.000 description 16
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 9
- 238000005516 engineering process Methods 0.000 description 9
- 230000003647 oxidation Effects 0.000 description 9
- 238000007254 oxidation reaction Methods 0.000 description 9
- 239000000589 Siderophore Substances 0.000 description 8
- 241000193830 Bacillus <bacterium> Species 0.000 description 7
- 150000007524 organic acids Chemical class 0.000 description 7
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 6
- 238000004519 manufacturing process Methods 0.000 description 6
- 238000011161 development Methods 0.000 description 5
- 230000002378 acidificating effect Effects 0.000 description 4
- 230000003248 secreting effect Effects 0.000 description 4
- 239000002893 slag Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 241000605222 Acidithiobacillus ferrooxidans Species 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 230000006978 adaptation Effects 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- 238000004128 high performance liquid chromatography Methods 0.000 description 3
- 150000002500 ions Chemical class 0.000 description 3
- 230000007246 mechanism Effects 0.000 description 3
- 238000011084 recovery Methods 0.000 description 3
- PTISTKLWEJDJID-UHFFFAOYSA-N sulfanylidenemolybdenum Chemical compound [Mo]=S PTISTKLWEJDJID-UHFFFAOYSA-N 0.000 description 3
- 231100000331 toxic Toxicity 0.000 description 3
- 230000002588 toxic effect Effects 0.000 description 3
- 239000002699 waste material Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- BJEPYKJPYRNKOW-REOHCLBHSA-N (S)-malic acid Chemical compound OC(=O)[C@@H](O)CC(O)=O BJEPYKJPYRNKOW-REOHCLBHSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- 238000004833 X-ray photoelectron spectroscopy Methods 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- BJEPYKJPYRNKOW-UHFFFAOYSA-N alpha-hydroxysuccinic acid Natural products OC(=O)C(O)CC(O)=O BJEPYKJPYRNKOW-UHFFFAOYSA-N 0.000 description 2
- WUKWITHWXAAZEY-UHFFFAOYSA-L calcium difluoride Chemical compound [F-].[F-].[Ca+2] WUKWITHWXAAZEY-UHFFFAOYSA-L 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
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- 239000011737 fluorine Substances 0.000 description 2
- 229910052731 fluorine Inorganic materials 0.000 description 2
- -1 fluorine ions Chemical class 0.000 description 2
- 239000010436 fluorite Substances 0.000 description 2
- 238000000673 graphite furnace atomic absorption spectrometry Methods 0.000 description 2
- 238000001095 inductively coupled plasma mass spectrometry Methods 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- 238000004895 liquid chromatography mass spectrometry Methods 0.000 description 2
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- 239000001630 malic acid Substances 0.000 description 2
- 235000011090 malic acid Nutrition 0.000 description 2
- 231100000783 metal toxicity Toxicity 0.000 description 2
- 238000004321 preservation Methods 0.000 description 2
- 229910052683 pyrite Inorganic materials 0.000 description 2
- 239000011028 pyrite Substances 0.000 description 2
- NIFIFKQPDTWWGU-UHFFFAOYSA-N pyrite Chemical compound [Fe+2].[S-][S-] NIFIFKQPDTWWGU-UHFFFAOYSA-N 0.000 description 2
- 230000027756 respiratory electron transport chain Effects 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 230000001954 sterilising effect Effects 0.000 description 2
- 238000004659 sterilization and disinfection Methods 0.000 description 2
- FEWJPZIEWOKRBE-JCYAYHJZSA-N Dextrotartaric acid Chemical compound OC(=O)[C@H](O)[C@@H](O)C(O)=O FEWJPZIEWOKRBE-JCYAYHJZSA-N 0.000 description 1
- VTLYFUHAOXGGBS-UHFFFAOYSA-N Fe3+ Chemical compound [Fe+3] VTLYFUHAOXGGBS-UHFFFAOYSA-N 0.000 description 1
- 241000589902 Leptospira Species 0.000 description 1
- 241000775208 Leptospirillum ferriphilum Species 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- FEWJPZIEWOKRBE-UHFFFAOYSA-N Tartaric acid Natural products [H+].[H+].[O-]C(=O)C(O)C(O)C([O-])=O FEWJPZIEWOKRBE-UHFFFAOYSA-N 0.000 description 1
- 241001052560 Thallis Species 0.000 description 1
- 229910001037 White iron Inorganic materials 0.000 description 1
- 241001148470 aerobic bacillus Species 0.000 description 1
- 238000013019 agitation Methods 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
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- 238000004458 analytical method Methods 0.000 description 1
- 230000001651 autotrophic effect Effects 0.000 description 1
- 229940041514 candida albicans extract Drugs 0.000 description 1
- 229910052951 chalcopyrite Inorganic materials 0.000 description 1
- DVRDHUBQLOKMHZ-UHFFFAOYSA-N chalcopyrite Chemical compound [S-2].[S-2].[Fe+2].[Cu+2] DVRDHUBQLOKMHZ-UHFFFAOYSA-N 0.000 description 1
- 150000001805 chlorine compounds Chemical class 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 239000010433 feldspar Substances 0.000 description 1
- 229940077441 fluorapatite Drugs 0.000 description 1
- 229910052587 fluorapatite Inorganic materials 0.000 description 1
- 229910001672 fluorine mineral Inorganic materials 0.000 description 1
- 229910052949 galena Inorganic materials 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 239000011019 hematite Substances 0.000 description 1
- 229910052595 hematite Inorganic materials 0.000 description 1
- 238000000589 high-performance liquid chromatography-mass spectrometry Methods 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- LIKBJVNGSGBSGK-UHFFFAOYSA-N iron(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Fe+3].[Fe+3] LIKBJVNGSGBSGK-UHFFFAOYSA-N 0.000 description 1
- XCAUINMIESBTBL-UHFFFAOYSA-N lead(ii) sulfide Chemical compound [Pb]=S XCAUINMIESBTBL-UHFFFAOYSA-N 0.000 description 1
- 238000001819 mass spectrum Methods 0.000 description 1
- 230000002503 metabolic effect Effects 0.000 description 1
- 230000004060 metabolic process Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000005272 metallurgy Methods 0.000 description 1
- 238000009629 microbiological culture Methods 0.000 description 1
- 238000005065 mining Methods 0.000 description 1
- 229910052961 molybdenite Inorganic materials 0.000 description 1
- CWQXQMHSOZUFJS-UHFFFAOYSA-N molybdenum disulfide Chemical compound S=[Mo]=S CWQXQMHSOZUFJS-UHFFFAOYSA-N 0.000 description 1
- KTEXACXVPZFITO-UHFFFAOYSA-N molybdenum uranium Chemical compound [Mo].[U] KTEXACXVPZFITO-UHFFFAOYSA-N 0.000 description 1
- 235000005985 organic acids Nutrition 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- VSIIXMUUUJUKCM-UHFFFAOYSA-D pentacalcium;fluoride;triphosphate Chemical compound [F-].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O VSIIXMUUUJUKCM-UHFFFAOYSA-D 0.000 description 1
- 230000001766 physiological effect Effects 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 238000004445 quantitative analysis Methods 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 230000001172 regenerating effect Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000028327 secretion Effects 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
- 241000894007 species Species 0.000 description 1
- 230000003068 static effect Effects 0.000 description 1
- WGPCGCOKHWGKJJ-UHFFFAOYSA-N sulfanylidenezinc Chemical compound [Zn]=S WGPCGCOKHWGKJJ-UHFFFAOYSA-N 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 230000004083 survival effect Effects 0.000 description 1
- 235000002906 tartaric acid Nutrition 0.000 description 1
- 239000011975 tartaric acid Substances 0.000 description 1
- CXVCSRUYMINUSF-UHFFFAOYSA-N tetrathiomolybdate(2-) Chemical compound [S-][Mo]([S-])(=S)=S CXVCSRUYMINUSF-UHFFFAOYSA-N 0.000 description 1
- 238000000870 ultraviolet spectroscopy Methods 0.000 description 1
- 239000012138 yeast extract Substances 0.000 description 1
- 229910052984 zinc sulfide Inorganic materials 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B3/00—Extraction of metal compounds from ores or concentrates by wet processes
- C22B3/18—Extraction of metal compounds from ores or concentrates by wet processes with the aid of microorganisms or enzymes, e.g. bacteria or algae
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B34/00—Obtaining refractory metals
- C22B34/30—Obtaining chromium, molybdenum or tungsten
- C22B34/34—Obtaining molybdenum
-
- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
- Y02P10/20—Recycling
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- Biochemistry (AREA)
- Biotechnology (AREA)
- Microbiology (AREA)
- Environmental & Geological Engineering (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Geochemistry & Mineralogy (AREA)
- Geology (AREA)
- Manufacture And Refinement Of Metals (AREA)
Abstract
The invention discloses a method for microbial leaching of molybdenum ore. The most critical point of the invention is that by utilizing the excellent characteristics of the microbacterium brick red Microbacterium Testaceum XS-1 that has the toxicity of various heavy metals and excretes various metabolites with chelating ability, the invention can directly contact molybdenum ore, adsorb on the surface of the molybdenum ore and leach out molybdenum element with high efficiency, which is the only strain known at present to directly act on the molybdenum ore, but not through oxidizing sulfide/Fe 2+ Microorganisms that leach molybdenum indirectly. The flow leaching process can more effectively avoid the leaching inhibition effect caused by the accumulation of molybdenum elements in the leaching solution. Has the characteristics of high leaching efficiency, high degree, simple process, low equipment requirement, low construction and operation cost and the like, and can be leached within 15 days>90% of molybdenum element. Neutral condition leaching overcomes the defects of high acid leaching cost, heavy pollution emission, more impurities, HF biotoxicity and the like, and increases economic benefit and environmental protection benefit.
Description
Technical Field
The invention belongs to the technical field of biological leaching of molybdenum ores, and particularly relates to a biological leaching process of micro-bacilli on molybdenum ores.
Background
Molybdenum (Mo) is widely used as a strategic mineral resourceIs used for manufacturing high-temperature alloy, electronic devices and medical appliances. Molybdenum ore is widely distributed in China, and the main production areas comprise Hebei, inner Mongolia, fujian, chuanganan, qinling North uranium molybdenum ore-forming zone, xiangxi, hubei, henan, shanxi and other places [1] . Taking a certain molybdenum ore deposit in Hebei in China as an example, wherein the molybdenum ore types with economic exploitation value mainly comprise rubber sulfur molybdenum ore, molybdenite and blue molybdenum ore, and other metal minerals comprise rubber pyrite, a small amount of zinc blende, galena, chalcopyrite, white iron ore, hematite and the like; the nonmetallic minerals include quartz, feldspar, fluorite, hydromica, etc [2] . The molybdenum ore resources in China are rich, but part of the ore has lower grade and limited yield, and the increasingly growing production demands in China are difficult to meet. In order to improve the natural molybdenum resource productivity of China, the industrial upgrading and reconstruction of the current molybdenum ore beds, especially low-grade molybdenum-containing ores are urgent.
Currently, volcanic basin molybdenum ore is mainly mined by using a surface heap leaching (heap leaching) technology in China. Heap leaching technology is a method for leaching molybdenum element from raw ore or crushed ore transported to the surface by heap construction and leaching solution [3] . The leaching solution is typically a solution containing a strong acid, such as sulfuric acid. These leaching solutions enter the heap by osmosis and leaching, accelerating dissolution of the rock-making minerals, or forming soluble complexes with the molybdenum element in the ore, facilitating leaching of the molybdenum element. In the existing molybdenum deposit heap leaching practice process, the leaching rate of molybdenum element is low, the leaching period is long, and the grade of molybdenum remained in slag is high, so that the resource is greatly wasted; the demand for water resources is high, and the application of the water-saving agent in arid areas is limited; and more tailing slag is generated by heap leaching, which constitutes a potential threat to the environment.
The microbial leaching technology mainly utilizes the metabolic activity of specific functional microbe and its secretion product to react with target component and dissolve it from solid matter. Compared with the traditional chemical leaching method, the microbial leaching technology has the advantages of high development efficiency, less investment, low acid consumption, little environmental hazard, simple process flow and the like, particularly has remarkable advantages in the field of low-grade mineral resource utilization, and has been applied to the development of copper, gold and other mineral resources in large scale at presentBy using [4] 。
Although microbial molybdenum leaching technology has great development potential, it is currently mainly limited to laboratory development stage, and there are many bottlenecks that limit its industrial application. At present, most biological mineral leaching researches are to utilize aerobic acidophilic autotrophic or facultative heterotrophic microorganisms with iron and sulfur oxidation performance such as acidophilic thiobacillus ferrooxidans (Acidithiobacillus ferrooxidans), leptospira ferrooxidans (Leptospirillum ferriphilum) and the like as mineral leaching flora of molybdenum ores under extremely low pH conditions [5-7] . The harsh acidic condition can leach out various impurity ions synchronously, so that the subsequent recovery of target molybdenum element is affected; forming a great amount of waste with toxic action and polluting the environment. Under the acidic leaching condition, fluorine ions are dissolved out from high-fluorine molybdenum ore containing minerals such as fluorite, fluorapatite and the like to form HF, and toxic action is caused on ore leaching microorganisms [5-7] . In addition, the aforementioned aerobic microorganisms tend to die in an anaerobic/anoxic environment in the lower part of the ore heap. The most important bottleneck of the current biological molybdenum leaching is that all the microorganisms in the leaching are not used for directly leaching molybdenum element, but are used for generating an oxidant Fe by (1) oxidizing sulfide pyrite in surrounding rock of the molybdenum ore 3+ (2) regenerating Fe in the leachate 3+ Thereby achieving the aim of indirectly accelerating the dissolution of molybdenum ore [5-7] . Thus, in the previously proposed bioleaching process of molybdenum ore, heap leaching and microbial oxidation regenerate Fe 3+ The biological contact oxidation tank is divided into two modules which are not synchronously carried out in different places [8] . The construction and operation costs are high, and the leaching efficiency of the molybdenum ore is limited. Therefore, it is important to develop a novel bioleaching process, particularly a technology for directly leaching molybdenum ore by utilizing microorganisms under neutral or near-neutral conditions.
[1] Meng Yanning, fan Honghai, chen Donghuan, et al, university of Donghua university of Hebei, U.S. Ming.460 mineral deposit, U.S. Ministry of uranium molybdenum mineralogy, nature science edition, 2015,38 (4): 335-343.
[2] Guo Hongjun and Ma Shenkun, analyzing the uranium-molybdenum ore control factor of Zhang Majing of Hebei province and the peripheral prospect of prospecting [ J ]. Geological investigation and research, 2009,32 (3): 210-215.
[3] Li Yingbing, ren Zhigang Mo Jun, et al, industrial process for oxygen pressure acid leaching of virgin uranium molybdenum ore [ J ]. China molybdenum industry, 2023,47 (05): 58.
[4] Li Anze, wang Hongjiang, wu Aixiang, et al, bioleaching state of the art hydrometallurgy 2014,33 (2): 82-85.
[5] Zheng Ying, fan Baotuan, liu Jian, et al bacterial leaching test study of uranium molybdenum intergrowth ore [ J ]. Hydrometallurgy, 2007,26 (2): 75-79.
[6] Li Xueli, niu Jianguo, song Jinru, etc. A uranium molybdenum ore microorganism leaching and uranium molybdenum enrichment separation method [ P ]. Jiangxi province: CN103866122B,2015-11-04.
[7] Upper officer, hao Yingxuan, zhang Zhanbo, experimental study on bioleaching of molybdenum, copper and iron in molybdenum tailings [ J ]. Mining and metallurgy engineering, 2019,39 (04): 119-122.
[8] Meng Yunsheng, fan Baotuan, liu Jian, et al. Biological contact oxidation tanks for heap leaching of uranium ore bacteria. Uranium mining metallurgy, 2004,23 (4): 182-186.
Disclosure of Invention
The invention aims to provide a biological leaching process of micro-bacillus to molybdenum ore. The key of the process is that a functional strain which can effectively leach molybdenum element in neutral or neutral environment, namely Microbacterium brick Microbacterium Testaceum XS-1, is used and is separated from a certain uranium-molybdenum-rare earth-containing polymetallic mine in China. The current strain is preserved in China general microbiological culture Collection center, address: beijing, chaoyang area, north Chenxi Lu No. 1, 3; the preservation number is CGMCC No. 28318, and the preservation date is 2023, 8 and 31; the classification is named: microbacterium rubrum Microbacterium Testaceum.
The invention screens out a strain of microbacterium Microbacterium Testaceum XS-1 with universal pH and temperature, is resistant to heavy metal toxicity, can secrete a plurality of metabolites with chelating ability, is efficiently attached to the surface of molybdenum ore, and can be used for efficiently leaching molybdenum element under neutral or near-neutral conditions.
A method for microbial mobile leaching of molybdenum ore, which utilizes microbacterium brick red Microbacterium Testaceum XS-1 to leach molybdenum-containing ore.
Further, the concentration of the thalli in the leaching systemDegree of 1×10 7 ～10 8 CFU/mL; the concentration range of the ore is 1-10g/L; the leaching temperature is 20-40 ℃.
Still further, the leaching system is configured by adopting a liquid oligotrophic OM culture medium, and the culture medium comprises the following components: 0.05-0.2g/L glucose, 0-0.02g/L NH 4 Cl, pH was adjusted to 5-8.
Further, the molybdenum-containing ore after the high-temperature sterilization is added into a leaching system for biological flow leaching. Adding crushed molybdenum-containing ore powder into the leaching system, and preferably crushing and grinding to 50-200 meshes.
Further, the microbacterium rubrum Microbacterium Testaceum XS-1 freeze-dried powder is activated before leaching.
The specific activation operation is as follows: the microbacterium brick red Microbacterium Testaceum XS-1 is revived in a GYM eutrophic culture medium (0.5-2 g/L glucose, 0.5-2g/L yeast extract, 2-5g/L malt extract) system, cultured to logarithmic phase, washed for at least 3 times by using a sterilized OM oligotrophic culture medium, and then added into a leaching system containing molybdenum ore.
The pH application range of the leaching system is 5-8; the tolerance temperature is 20-40 ℃; the classes of tolerant heavy metals include: cu, zn, U, th, mo.
Further, the invention adopts a flow leaching process, a leaching column is arranged from top to bottom according to the sequence of small Kong Lvwang, a sand infiltration layer, a nylon filter screen, a molybdenum ore layer, a nylon filter screen, a surrounding rock gravel layer and a small-hole filter screen, the leaching agent adopts microbacterium brick Microbacterium Testaceum XS-1 bacterial suspension dissolved in an OM oligotrophic culture medium, a constant-flow peristaltic pump is utilized to pump the bacterial suspension into the leaching column from bottom to top, and the flow rate of the bacterial suspension is controlled to carry out circulating leaching.
Further, a flow leaching process is adopted, a leaching column is arranged from top to bottom according to the sequence of a sand infiltration layer with the aperture of 100-500mm, the aperture of Kong Lvwang, the thickness of 5-20cm and the particle size of 0.5-4mm, a nylon filter screen with the aperture of 75-300 mu m, a molybdenum ore layer with the aperture of 2-30cm and the particle size of 50-200 meshes, a nylon filter screen with the aperture of 75-300 mu m, a surrounding rock gravel layer with the aperture of 5-20cm and the particle size of 0.5-2cm and a small pore filter screen with the aperture of 100-500mm, wherein a leaching agent is microbacterium brick red Microbacterium Testaceum XS-1 bacterial suspension dissolved in an OM oligonutrient medium, the flow rate of the bacterial suspension is controlled to be 0.01-50.00mL/min by a constant flow peristaltic pump, and the leaching time is 2-30 days.
In the leaching process, the method utilizes a high performance liquid chromatography-mass spectrometry HPLC-LC-MS combined method to determine the types of metabolites secreted by the microbacterium brick Microbacterium Testaceum XS-1 when the molybdenum ore is leached under the near neutral condition, such as organic acid, siderophores and the like. And separating different metabolites by utilizing High Performance Liquid Chromatography (HPLC), and then carrying out crushing analysis on molecules of different substances by combining liquid mass spectrum (LC-MS) to obtain a chemical structural formula and a three-dimensional space structure of a specific substance, and determining the composition information of the specific species. Quantitative analysis was performed using high performance liquid chromatography HPLC (organic acid) and an ultraviolet-visible spectrophotometer UV-vis (siderophore) for specific metabolite types.
The method monitors the concentration and valence state of molybdenum element in the leaching solution in real time. Measuring the total molybdenum concentration in the leaching solution by utilizing inductively coupled plasma mass spectrometry ICP-MS; the concentrations of Mo (V) and Mo (VI) in the leaching solution are respectively measured by a tartaric acid and phosphoric acid extraction method and a graphite furnace atomic absorption spectrometry GFAAS; and the relative content of Mo (IV)/Mo (V)/Mo (VI) in the leached residual solid is analyzed semi-quantitatively by X-ray photoelectron spectroscopy XPS. According to the change of Mo valence state, the oxidizing leaching capability of the bacillus strain on molybdenum element can be evaluated.
The microbacterium of the invention mainly reduces the pH of a leaching system by (1) secreting organic acid, and mainly comprises citric acid and malic acid with strong chelating ability; (2) A secretory siderophore including hydroxamate type siderophores; and (3) under neutral conditions, promote air oxidation of Mo (IV) minerals. As the bacillus strain is in direct contact with the molybdenum ore and is strongly adsorbed on the surface of the bacillus strain, various metabolites of the bacillus strain can directly act on the molybdenum ore, and the molybdenum element can be leached efficiently and rapidly. Direct contact on the physical level of the microbacterium-molybdenum ore can also induce physical weathering, namely the mechanical destruction of the molybdenum ore by the physiological activities of microorganisms, so as to further accelerate the leaching of molybdenum element.
Meanwhile, the bacillus strain can leach molybdenum element efficiently under neutral condition, so that the defects of a series of environmental pollution caused by acid leaching, influence of impurities on target Mo element recovery, toxicity of HF on microorganisms and the like are overcome, the requirement on leaching equipment is low, and the production and operation cost is reduced. As the microbacterium directly contacts with the molybdenum ore to leach the molybdenum element, an additional biological contact oxidation tank is not needed, and the production and maintenance cost is further reduced.
Existing H 2 SO 4 Heap leaching technology, leaching period is longer, mo grade remained in slag is still higher, and great waste of resources is caused; the water consumption is high, so that the application of the water-saving agent in arid areas is limited; and more tailing slag can be generated by heap leaching, which constitutes a potential threat to the environment; in contrast, the microbial technology has the advantages of high development efficiency, low investment, low acid consumption, little environmental hazard, simple process flow and the like, and particularly has remarkable advantages in the field of low-grade mineral resource utilization. Compared with the common microorganism acid leaching process, the invention has the following remarkable characteristics:
1. neutral leaching environment: the method overcomes the problem that (1) the leaching of a plurality of impurity ions possibly caused by the acidic leaching of microorganisms affects the recovery of the subsequent target Mo element; (2) dissolving the high-fluorine mineral to form HF poisoning microorganisms; (3) Acid waste disposal, which causes acid pollution to ecological systems such as surrounding soil, water body and the like; (4) Commonly used H 2 SO 4 As an acidic leaching agent, SO is brought about 4 2- Ion contamination.
2. Facultative anaerobic microbacterium: the microbacterium brick red Microbacterium Testaceum XS-1 used in the invention is facultative anaerobic microorganism, which can overcome the defect that aerobic bacteria die in anaerobic/anoxic environment at the lower part of the ore heap;
3. direct molybdenum leaching mechanism: the strain of microbacterium is no longer oxidized by sulfide or Fe as in the case of thiobacillus ferrooxidans Acidithiobacillus ferrooxidans 2+ Thereby indirectly leaching molybdenum element; but directly contacts molybdenum mineral, and directly leaches molybdenum element by secreting organic acid and siderophores and superposing an electron transfer mechanism.
4. Integrated molybdenum ore heap leaching: because the bacillus strain directly contacts molybdenum minerals to leach molybdenum elements, an additional biological contact oxidation tank is not needed, the equipment is simpler, the process is simpler, and the operation and maintenance cost can be greatly reduced.
5. High-efficiency leaching: because the strain of microorganism can be efficiently adsorbed on the surface of molybdenum ore, the metabolite can be efficiently acted on molybdenum ore, molybdenum element is preferentially leached, and the problems of low leaching efficiency, low leaching degree and the like commonly existing in the existing biological leaching technology are overcome.
6. Flow leaching: conventional static leaching or agitation leaching, the accumulation of Mo elements in the leachate can inhibit the microbial leaching action. And (3) carrying out mobile leaching, namely, using fresh microbacterium brick red Microbacterium Testaceum XS-1 bacterial suspension as a leaching agent to circularly leach ores, and promoting the efficient leaching of Mo element.
The microbacterium brick Microbacterium Testaceum XS-1 provided by the invention has the excellent characteristics of resisting various heavy metal toxicities and secreting various metabolites with chelating ability, can be directly contacted with molybdenum ore, is adsorbed on the surface of the molybdenum ore, and can be used for efficiently leaching molybdenum element, is a microorganism which is currently known to be only one strain to directly act on the molybdenum ore, and does not need to oxidize sulfide/Fe 2+ And indirectly leaching molybdenum element. Has the characteristics of high leaching efficiency, high degree, simple process, low equipment requirement, low construction and operation cost and the like, and can be leached within 15 days>90% of molybdenum element. Neutral condition leaching overcomes the defects of high acid leaching cost, heavy pollution emission, more impurities, HF biotoxicity and the like, and increases economic benefit and environmental protection benefit.
Drawings
Fig. 1: compared with a sterile control group, the microbacterium brick red Microbacterium Testaceum XS-1 provided by the invention has the advantages that the molybdenum element is subjected to standing leaching;
fig. 2: a field arrangement of a flow leaching device and a leaching column arrangement schematic diagram;
fig. 3: compared with a sterile control group, the microbacterium brick red Microbacterium Testaceum XS-1 provided by the invention has the advantages that the molybdenum element is leached in a flowing way;
fig. 4: the microbacterium brick red Microbacterium Testaceum XS-1 is strongly adhered to the surface of molybdenum ore in the mineral leaching process;
fig. 5: the microbacterium rubrum Microbacterium Testaceum XS-1 accelerates the oxidation process of molybdenum element in the mineral leaching process,
fig. 6: the microbacterium brick red Microbacterium Testaceum XS-1 of the invention has the result of high-efficiency leaching of molybdenum under the condition of universal and near neutral pH;
fig. 7: the microbacterium brick Microbacterium Testaceum XS-1 of the invention has the result of high-efficiency molybdenum leaching under the conditions of universal, medium and low temperature;
fig. 8: the microbacterium rubrum Microbacterium Testaceum XS-1 provided by the invention survives under various heavy metal stress conditions.
Detailed Description
The following examples are intended to further illustrate the invention, but not to limit it.
Example 1: the invention Microbacterium Testaceum XS-1 is characterized by leaching molybdenum element by standing
Experimental conditions: the molybdenum ore is extracted from Hebei source area of China, and the main molybdenum-containing ore is sulfur-molybdenum ore. Microbacterium rubrum Microbacterium Testaceum XS-1 (1×10) in logarithmic phase at room temperature and pH 7 7 CFU/mL) and 5g/L of high-temperature sterilized molybdenum ore powder (mainly thiomolybdate ore with particle size of 100 meshes) in an oligotrophic OM culture medium system (0.2 g/L glucose, 0.02g/L NH) 4 Cl) at room temperature for 30 days. Sterile control groups were established under equivalent conditions. The total molybdenum content of the raw rock is 340 mug/g; therefore, the total Mo content in the suspension experiment system is 1700ppb.
The experimental results are shown in fig. 1: compared with a sterile control group, the microbacterium brick red Microbacterium Testaceum XS-1 can leach Mo element efficiently under a standing condition, and the leaching period is shorter. About 58% of Mo element can be leached in a period of 10 days; whereas at 20 days the Mo leaching rate had exceeded 63%.
Example 2: the invention Microbacterium Testaceum XS-1 mobile leached molybdenum element
Experimental conditions: microbacterium brick Microbacterium Testaceum XS-6-1 in logarithmic phase was dissolved in oligotrophic OM medium (0.2 g/L glucose,0.02g/L NH 4 cl) to form a bacterial suspension (1X 10) 7 CFU/mL) is used as a leaching agent, a constant-flow peristaltic pump is used for controlling the flow rate of bacterial suspension to be 2mL/min, and 5g/L of molybdenum ore powder (mainly rubber sulfur molybdenum ore) after high-temperature sterilization is subjected to flow leaching. Under the same condition, a sterile control group is established, namely, a sterile oligotrophic OM culture medium is used as a leaching agent. The total molybdenum content of the raw rock is 340 mug/g; therefore, the total Mo content in the suspension experiment system is 1700ppb.
The leaching agent is a brick red microbacterium Microbacterium Testaceum XS-1 bacterial suspension dissolved in OM oligotrophic culture medium, and a flow leaching process is adopted, wherein a leaching column is arranged from top to bottom according to the sequence of a sand infiltration layer with a pore diameter of 100mm and a diameter of Kong Lvwang, a nylon filter screen with a pore diameter of 2mm (thickness of 10 cm), a molybdenum ore layer with a pore diameter of 150 mu m (thickness of 20 cm), a nylon filter screen with a pore diameter of 150 mu m, a surrounding rock gravel layer with a particle diameter of 0.5cm (thickness of 10 cm) and a small pore filter screen with a pore diameter of 400 mm. The bacterial suspension is pumped into the leaching column from bottom to top and is circulated and reciprocated as shown in the structural schematic diagram of FIG. 2.
The experimental results are shown in fig. 3: compared with a sterile control group, the microbacterium brick red Microbacterium Testaceum XS-1 can leach Mo element efficiently under the condition of flow leaching. Compared with the standing leaching result of the example 1 (figure 1), the leaching efficiency and the leaching degree are greatly improved without a remarkable inhibition period (the leaching degree of Mo element is not obviously increased after the period of 5 days of the example 1) in a flowing leaching system. About 80% of Mo element can be leached in the flowing leaching system in 10 days; whereas the Mo leaching rate at 15 days has exceeded 90%.
Example 3: the flow leaching mechanism of the present invention Microbacterium Testaceum XS-1: production of organic acids and siderophores
Experimental conditions: same as in example 2
Experimental results: microbacterium brick Microbacterium Testaceum XS-1 secretes a large amount of organic acid, especially strong chelating citric acid and malic acid, to 2.81mM and 0.46mM respectively in the flowing leaching process; at the same time, a portion of siderophores was produced by metabolism, the total concentration reaching 67.44. Mu.M, see Table 1 below.
TABLE 1
Example 4: the microbacterium brick red Microbacterium Testaceum XS-1 of the invention is strongly adsorbed in the molybdenum ore Dan Biaomian in the flowing leaching process
Experimental conditions: same as in example 2
The experimental results are shown in fig. 4: the microbacterium brick Microbacterium Testaceum XS-1 can be strongly adhered to the surface of molybdenum ore in the process of mobile leaching, so as to strengthen the interaction process of microorganism metabolites (such as organic acid and siderophore) and the molybdenum ore.
Example 5: the microbacterium rubrum Microbacterium Testaceum XS-1 accelerates the oxidation of molybdenum Mo element in the flowing leaching process
Experimental conditions: same as in example 2
The experimental results are shown in fig. 5: the microbacterium brick Microbacterium Testaceum XS-1 can accelerate the oxidation process of molybdenum element in the flowing leaching process, directly oxidize Mo element or catalyze the electron transfer process between air and Fe (III) -containing minerals, and accelerate the leaching of molybdenum element. The entire ore leaching system is gradually oxidized along with the extension of the flow leaching action time.
Example 6: PH adaptation range determination of flow leached molybdenum of microbacterium brick red Microbacterium Testaceum XS-1 of the invention
Experimental conditions: microbacterium rubrum Microbacterium Testaceum XS-1 (1×10) in logarithmic phase after activation at pH 5-8 7 CFU/mL) and 5g/L of sterilized molybdenum ore powder in an oligotrophic OM culture medium system (0.2 g/L glucose, 0.02g/L NH) 4 Cl) was co-cultured at room temperature for 7 days. Sterile control groups of corresponding pH were established with HCl and NaOH.
The experimental results are shown in fig. 6: compared with a sterile control, the microbacterium brick Microbacterium Testaceum XS-1 can leach molybdenum element with high efficiency, and has no obvious change in the pH range of 5-8, which indicates that the microbacterium can leach molybdenum element with high efficiency in a neutral environment.
Example 7: temperature adaptation range determination of flow leached molybdenum of microbacterium brick red Microbacterium Testaceum XS-1 of the invention
Experimental conditions: microbacterium rubrum Microbacterium Testaceum XS-1 (1×10) in logarithmic phase after activation at pH 7 at different temperatures 7 CFU/mL) and 5g/L of molybdenum ore powder sterilized at high temperature are mixed in an oligotrophic culture medium system (0.2 g/L glucose, 0.02g/L NH) 4 Cl) for 7 days. A sterile control group of corresponding temperature was established.
The experimental results are shown in fig. 7: compared with a sterile control, the microbacterium rubrum Microbacterium Testaceum XS-1 can leach molybdenum element with high efficiency, and has no obvious change in the range of 20-40 ℃. Namely, the bacillus strain can leach molybdenum element with high efficiency in a wider temperature range.
Example 8: heavy metal species tolerance adaptation range determination of flow leaching molybdenum of microbacterium brick red Microbacterium Testaceum XS-1
Experimental conditions: the initial concentration was 3.6X10 at room temperature pH 4.5 8 CFU/mL Microbacterium rubrum Microbacterium Testaceum XS-1 was mixed with different heavy metal chlorides (1 mM) and incubated for 24h, and the survival status was determined by plating. The pH is set at 4.5 because of heavy metal ions such as Cu 2+ 、UO 2 2+ At pH value>Precipitation occurs at 5.
The experimental results are shown in fig. 8: compared with the initial bacterial load and the blank control group without heavy metal, the heavy metal addition does not cause obvious toxic action on the microbacterium rubrum Microbacterium Testaceum XS-1, namely the microbacterium strain has stronger heavy metal tolerance.
Claims (10)
1. A method for microbial leaching of molybdenum ore, which is characterized in that the molybdenum-containing ore is leached by using Microbacterium rubrum Microbacterium Testaceum XS-1.
2. The method according to claim 1, wherein the concentration of the cells in the leaching system is 1X 10 7 ～10 8 CFU/mL; the concentration range of the ore is 1-10g/L; the leaching temperature is 20-40 ℃.
3. The method of claim 1, wherein the leaching system is configured with a liquid oligotrophic OM culture medium, the culture medium composition comprising: 0.05-0.2g/L glucose, 0-0.02g/L NH 4 Cl, pH was adjusted to 5-8.
4. A method according to any one of claims 1-3, characterized in that the molybdenum-bearing ore after autoclaving is added to a leaching system for leaching.
5. A method according to any one of claims 1-3, characterized in that crushed molybdenum-containing ore powder is added to the leaching system, preferably crushed to 50-200 mesh.
6. The method of claim 1, wherein the microbacterium rubrum Microbacterium Testaceum XS-1 lyophilized powder is activated prior to leaching.
7. The method according to claim 6, characterized in that the specific activation operation is as follows: reviving Microbacterium brick Microbacterium Testaceum XS-1 in GYM eutrophic culture medium system, culturing to logarithmic phase, washing with sterilized OM oligotrophic culture medium for at least 3 times, and adding leaching system containing molybdenum ore.
8. The method according to any one of claims 1 to 7, wherein the leaching system has a pH application range of 5 to 8; the tolerance temperature is 20-40 ℃; the classes of tolerant heavy metals include: cu, zn, U, th, mo.
9. The method of claim 1, wherein a flow leaching process is adopted, a leaching column is arranged from top to bottom according to the sequence of small Kong Lvwang, a sand infiltration layer, a nylon filter screen, a molybdenum ore layer, a nylon filter screen, a surrounding rock gravel layer and a small-hole filter screen, the leaching agent is microbacterium brick Microbacterium Testaceum XS-1 bacterial suspension dissolved in the OM oligotrophic culture medium, a constant-flow peristaltic pump is used for pumping the bacterial suspension into the leaching column from bottom to top, and the flow rate of the bacterial suspension is controlled for circular leaching.
10. The method according to claim 9, wherein a flow leaching process is adopted, a leaching column is arranged from top to bottom according to the sequence of a sand infiltration layer with a pore diameter of 100-500mm, a thickness of 5-20cm and a particle diameter of 0.5-4mm, a nylon filter screen with a pore diameter of 75-300 μm, a molybdenum ore layer with a thickness of 2-30cm and a particle diameter of 50-200 meshes, a nylon filter screen with a pore diameter of 75-300 μm, a surrounding rock gravel layer with a thickness of 5-20cm and a particle diameter of 0.5-2cm, and a pore filter screen with a pore diameter of 100-500mm, wherein a leaching agent is selected from a microbacterium brick-Microbacterium Testaceum XS-1 bacterial suspension dissolved in an OM oligotrophic medium, a constant flow peristaltic pump is used for controlling the bacterial suspension flow rate to be 0.01-50.00mL/min, and the leaching time is 2-30 days.
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| CN114437998A (en) * | 2022-04-08 | 2022-05-06 | 中国农业科学院生物技术研究所 | Microbacterium rubrum for promoting growth of rice and improving cold resistance of seedlings and application thereof |
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