CN109852803B - A kind of method for recovering valuable metals and iron in jarosite slag - Google Patents
A kind of method for recovering valuable metals and iron in jarosite slag Download PDFInfo
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- 239000002893 slag Substances 0.000 title claims abstract description 96
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 71
- 229910052742 iron Inorganic materials 0.000 title claims abstract description 35
- 238000000034 method Methods 0.000 title claims abstract description 35
- 229910052935 jarosite Inorganic materials 0.000 title claims abstract description 33
- 229910052751 metal Inorganic materials 0.000 title claims abstract description 32
- 239000002184 metal Substances 0.000 title claims abstract description 32
- 150000002739 metals Chemical class 0.000 title claims abstract description 23
- 238000006243 chemical reaction Methods 0.000 claims abstract description 54
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims abstract description 35
- 229910052725 zinc Inorganic materials 0.000 claims abstract description 35
- 239000011701 zinc Substances 0.000 claims abstract description 35
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims abstract description 34
- 229910052802 copper Inorganic materials 0.000 claims abstract description 34
- 239000010949 copper Substances 0.000 claims abstract description 34
- 229910052738 indium Inorganic materials 0.000 claims abstract description 34
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 claims abstract description 34
- 229910052732 germanium Inorganic materials 0.000 claims abstract description 33
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 claims abstract description 33
- 229910052595 hematite Inorganic materials 0.000 claims abstract description 28
- 239000011019 hematite Substances 0.000 claims abstract description 28
- LIKBJVNGSGBSGK-UHFFFAOYSA-N iron(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Fe+3].[Fe+3] LIKBJVNGSGBSGK-UHFFFAOYSA-N 0.000 claims abstract description 28
- 229910052709 silver Inorganic materials 0.000 claims abstract description 28
- 239000004332 silver Substances 0.000 claims abstract description 28
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims abstract description 24
- 238000000926 separation method Methods 0.000 claims abstract description 17
- 239000007787 solid Substances 0.000 claims abstract description 15
- 238000001556 precipitation Methods 0.000 claims abstract description 10
- 239000013078 crystal Substances 0.000 claims abstract description 7
- 238000005188 flotation Methods 0.000 claims abstract description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 6
- 239000007788 liquid Substances 0.000 claims description 14
- 238000005516 engineering process Methods 0.000 claims description 12
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims description 11
- 238000002156 mixing Methods 0.000 claims description 11
- 239000005083 Zinc sulfide Substances 0.000 claims description 6
- 229910052984 zinc sulfide Inorganic materials 0.000 claims description 6
- DRDVZXDWVBGGMH-UHFFFAOYSA-N zinc;sulfide Chemical compound [S-2].[Zn+2] DRDVZXDWVBGGMH-UHFFFAOYSA-N 0.000 claims description 6
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims 2
- 238000000746 purification Methods 0.000 claims 2
- 239000002002 slurry Substances 0.000 claims 2
- VDNSGQQAZRMTCI-UHFFFAOYSA-N sulfanylidenegermanium Chemical compound [Ge]=S VDNSGQQAZRMTCI-UHFFFAOYSA-N 0.000 claims 1
- 239000000243 solution Substances 0.000 abstract description 44
- 238000011084 recovery Methods 0.000 abstract description 6
- 239000007864 aqueous solution Substances 0.000 abstract description 3
- 230000009466 transformation Effects 0.000 abstract description 3
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 abstract description 2
- 239000011133 lead Substances 0.000 abstract 2
- 238000004140 cleaning Methods 0.000 abstract 1
- SURQXAFEQWPFPV-UHFFFAOYSA-L iron(2+) sulfate heptahydrate Chemical compound O.O.O.O.O.O.O.[Fe+2].[O-]S([O-])(=O)=O SURQXAFEQWPFPV-UHFFFAOYSA-L 0.000 description 21
- 229910000359 iron(II) sulfate Inorganic materials 0.000 description 21
- 238000002386 leaching Methods 0.000 description 13
- 239000002244 precipitate Substances 0.000 description 10
- 239000000126 substance Substances 0.000 description 7
- 238000000197 pyrolysis Methods 0.000 description 6
- 238000010438 heat treatment Methods 0.000 description 5
- 230000001376 precipitating effect Effects 0.000 description 5
- 238000004537 pulping Methods 0.000 description 5
- 238000004458 analytical method Methods 0.000 description 4
- 238000009854 hydrometallurgy Methods 0.000 description 4
- 238000002441 X-ray diffraction Methods 0.000 description 3
- 230000007547 defect Effects 0.000 description 3
- 239000002699 waste material Substances 0.000 description 3
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 2
- KFZAUHNPPZCSCR-UHFFFAOYSA-N iron zinc Chemical compound [Fe].[Zn] KFZAUHNPPZCSCR-UHFFFAOYSA-N 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- 238000003723 Smelting Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- SZVJSHCCFOBDDC-UHFFFAOYSA-N ferrosoferric oxide Chemical compound O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 description 1
- 239000003546 flue gas Substances 0.000 description 1
- 231100001261 hazardous Toxicity 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
- 239000002910 solid waste Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
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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
- 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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- Manufacture And Refinement Of Metals (AREA)
Abstract
本发明涉及一种回收铁矾渣中有价金属及铁的方法，属于湿法冶金清洁综合回收技术领域。将铁矾渣采用水或稀硫酸溶液按照液固比为2~10:1L/kg混合调浆得到矿浆，稀硫酸溶液浓度为0.1~10g/L；将得到的矿浆，加入浓度为0~60g/L的赤铁矿晶种，升温至温度为160~250℃，分解和转化反应60~300min，然后液固分离后得到转化液和转化渣，转化液中回收锌、铜、铟、锗有价金属，转化渣中浮选铅、银后得到赤铁矿渣。本发明在高温水溶液中铁矾渣发生分解与转化，锌、铜、铟、锗等有价金属溶解进入转化液，伴生铁转化为赤铁矿渣，铅、银以硫酸盐沉淀形式富集于赤铁矿铁渣，经分离和富集铅、银等有价成分后，赤铁矿渣可作为二次资源实现其资源化利用。
The invention relates to a method for recovering valuable metals and iron in jarosite slag, and belongs to the technical field of hydrometallurgical cleaning and comprehensive recovery. The jarosite slag is mixed with water or dilute sulfuric acid solution according to the liquid-solid ratio of 2~10:1L/kg to obtain ore pulp, and the concentration of the dilute sulfuric acid solution is 0.1~10g/L; the obtained ore pulp is added with a concentration of 0~60g /L of hematite seed crystals, heated to a temperature of 160~250℃, decomposed and converted for 60~300min, and then liquid-solid separation was performed to obtain a conversion solution and a conversion slag. The zinc, copper, indium, and germanium recovered from the conversion solution were Hematite slag is obtained after flotation of lead and silver in the conversion slag. In the present invention, the jarosite slag is decomposed and transformed in the high-temperature aqueous solution, and valuable metals such as zinc, copper, indium, germanium and the like are dissolved into the transformation solution, the associated iron is transformed into hematite slag, and lead and silver are enriched in the hematite slag in the form of sulfate precipitation. Iron ore slag, after separation and enrichment of valuable components such as lead and silver, hematite slag can be used as a secondary resource to realize its resource utilization.
Description
Technical Field
The invention relates to a method for recovering valuable metals and iron in jarosite slag, and belongs to the technical field of clean and comprehensive recovery of hydrometallurgy.
Background
The metal zinc and the products thereof are important strategic resources, the zinc yield in 2017 China accounts for more than 50% of the global yield, 85% of zinc is produced by adopting a zinc hydrometallurgy process, and the zinc-iron separation is one of the most critical processes of zinc hydrometallurgy. The jarosite method is a zinc-iron separation process which occupies a leading position in modern zinc hydrometallurgy, but because the jarosite slag contains 20-30% of iron, and is also rich in valuable metals such as zinc, copper, indium, germanium and the like, and a large amount of harmful elements such as heavy metals such as lead, cadmium and the like, the jarosite slag can continuously dissolve out to pollute underground water and soil under the condition of natural stockpiling, and the environmental pollution is serious. Therefore, from 1/8 of 2008, jarosite slag produced by the jarosite process has been listed in the national hazardous solid waste array (waste codes 331-005-48). At present, the amount of iron vitriol slag stockpiled in China exceeds 3500 million tons, the iron vitriol slag is increased at a speed of 100 million tons every year, huge potential pollution is caused to the environment, and associated iron resources and valuable metal resources such as zinc, copper, indium, germanium and the like are seriously wasted. Therefore, the clean and high-efficiency treatment of the jarosite slag becomes a great environmental protection problem in the domestic metallurgical industry.
At present, the treatment of the iron vitriol slag mainly adopts a combined process of a fire method, a wet method and a fire method and a wet method to realize the recovery of iron and valuable metals, and the methods have respective advantages and disadvantages. Patents with patent application numbers 201610068022.0, 201611063342.3 and 201710091764 respectively disclose a method for preparing micaceous iron oxide and ferroferric oxide by converting iron vitriol slag, and iron elements in the iron vitriol slag are converted into iron chemical products, so that recycling of iron resources is realized. However, the methods have the defects that valuable metals such as zinc, copper, indium, germanium and the like in the jarosite slag cannot be recycled, intermediate conversion solution cannot be properly treated, and secondary pollution is easily caused.
The main method for recovering valuable metals in jarosite slag at present comprises roasting-water leaching or solvent leaching, the method can realize the recovery of various valuable metals, but has the defects that the reaction is required to be carried out at the high temperature of 400 plus-1000 ℃, the flue gas which produces a large amount of sulfur dioxide with low concentration is easy to cause low-altitude pollution, the obtained leached slag needs to be further properly treated, the resource utilization of associated iron resources in the jarosite slag is not realized, and the process flow is complex.
Disclosure of Invention
In order to solve the problems and the defects of the prior art, the invention provides a method for recovering valuable metals and iron in jarosite slag. In a high-temperature aqueous solution, iron vitriol slag is decomposed and converted at high temperature, valuable metals such as zinc, copper, indium, germanium and the like are dissolved and enter a conversion solution, associated iron is converted into hematite slag at high temperature, lead and silver are enriched in the hematite iron slag in a sulfate precipitation mode, and the hematite slag can be used as a secondary resource to realize resource utilization after valuable components such as lead, silver and the like are separated and enriched. The invention is realized by the following technical scheme.
A method for recovering valuable metals and iron in jarosite slag comprises the following steps:
step 1, mixing and pulping jarosite slag by adopting water or a dilute sulfuric acid solution according to a liquid-solid ratio of 2-10: 1L/kg to obtain ore pulp, wherein the concentration of the dilute sulfuric acid solution is 0.1-10 g/L;
and 2, adding hematite seed crystals with the concentration of 0-60 g/L into the ore pulp obtained in the step 1, heating to 160-250 ℃, carrying out pyrolysis and conversion reaction for 60-300 min, then carrying out liquid-solid separation to obtain conversion liquid and conversion slag, recovering valuable metals such as zinc, copper, indium and germanium from the conversion liquid, and carrying out floatation separation on lead and silver in the conversion slag to obtain hematite slag.
The jarosite slag comprises the following components in percentage by mass: 20-30% of iron, 2-8% of zinc, 0.05-0.4% of copper, 0.01-0.08% of indium, 0.007-0.07% of germanium, 1-15% of lead and 0.007-0.06% of silver.
And (3) precipitating the conversion solution in the step (2) step by adopting a known sulfide precipitation technology and recovering zinc, copper, indium and germanium in the conversion solution to obtain sulfide precipitates of copper, indium and germanium, zinc sulfide precipitates and a purifying solution respectively, and returning the purifying solution to the step (1) to be used as a size mixing solution.
And (3) separating and recovering lead and silver from the transformation slag in the step (2) by adopting a known flotation separation technology to obtain hematite slag.
The invention has the beneficial effects that:
(1) the invention overcomes the limitation that the existing treatment process of the iron vitriol slag can only recover iron or valuable metals, and simultaneously realizes the high-efficiency recovery of the valuable metals such as zinc, copper, indium, germanium, lead, silver and the like in the iron vitriol slag and the resource utilization of the associated iron.
(2) In a high-temperature aqueous solution, the high-efficiency leaching of valuable metals and the conversion of iron are combined to be completed in one step, the conversion liquid is returned to the process for use, the hematite conversion slag is recycled, no waste liquid or waste solid is generated in the process, and the method has the advantages of high metal recovery rate, simple process flow, environment friendliness and the like.
Drawings
FIG. 1 is a pyrolysis flow diagram of the present invention;
FIG. 2 is an XRD pattern of jarosite slag 1 in example 1 of the present invention;
FIG. 3 is an XRD of the slag obtained in example 1 of the present invention.
Detailed Description
The invention is further described with reference to the following drawings and detailed description.
The iron vitriol slag in the embodiment of the invention is respectively taken from two domestic wet zinc smelting enterprises which adopt iron vitriol method to remove iron, the iron vitriol slag is dried and finely ground until the grain diameter is less than 0.074 mm accounts for more than 90 percent, and the main components of the raw material iron vitriol slag are analyzed by chemical components as shown in Table 1.
TABLE 1 main chemical composition of iron vitriol slag
Example 1
As shown in FIG. 1, the method for recovering valuable metals and iron from jarosite slag comprises the following steps:
step 1, mixing and pulping 0.15kg of iron vitriol slag (iron vitriol slag 1) by using a dilute sulfuric acid solution according to a liquid-solid ratio of 10:1L/kg to obtain ore pulp, wherein the concentration of the dilute sulfuric acid solution is 0.1 g/L;
and 2, adding hematite seed crystals with the concentration of 20g/L into the ore pulp obtained in the step 1, heating to 180 ℃, carrying out pyrolysis and conversion reaction for 180min, and then carrying out liquid-solid separation to obtain 1.35L of valuable metal conversion liquid rich in zinc, copper, indium, germanium and the like and 0.103kg of conversion slag.
Precipitating the conversion solution in the step 2 step by adopting a known sulfide precipitation technology and recovering zinc, copper, indium and germanium in the conversion solution to respectively obtain sulfide precipitates of copper, indium and germanium, zinc sulfide precipitates and a purifying solution, and returning the purifying solution to the step 1 to be used as a size mixing solution; and (3) separating and recovering lead and silver by using a known flotation separation technology in the transformed slag in the step (2) to obtain hematite slag.
The XRD pattern of the jarosite slag 1 is shown in figure 2, and the XRD pattern of the transformation slag is shown in figure 3; FIG. 2 shows jarosite (KFe) in the jarosite slag 13(SO4)2(OH)6) And ammonioiarosite (NH)4Fe3(SO4)2(OH)6) The phase-average high-temperature decomposition is converted into hematite conversion slag, and the lead and silver in the hematite conversion slag can be separated and enriched to realize resource utilization.
Respectively taking the conversion solution and the hematite conversion slag enriched with lead and silver for chemical component analysis, wherein the conversion solution contains zinc of 7.44g/L, copper of 316mg/L, indium of 13.32mg/L and germanium of 6.4mg/L, and the conversion slag contains iron of 58.9wt%, lead of 1.7 wt% and silver of 0.013 wt%; the leaching rate of zinc, copper, indium and germanium in this example was 98.5%, 98.2%, 85.6% and 82.3%, respectively, and the enrichment ratio of lead and silver in the slag was 99.8% and 99.6%, respectively.
Example 2
As shown in FIG. 1, the method for recovering valuable metals and iron from jarosite slag comprises the following steps:
step 1, mixing and pulping 0.5kg of iron vitriol slag (iron vitriol slag 1) by using a dilute sulfuric acid solution according to a liquid-solid ratio of 6:1L/kg to obtain ore pulp, wherein the concentration of the dilute sulfuric acid solution is 5 g/L;
and 2, adding 60g/L hematite seed crystal into the ore pulp obtained in the step 1, heating to 160 ℃, carrying out pyrolysis and conversion reaction for 300min, and then carrying out liquid-solid separation to obtain 2.7L valuable metal conversion liquid rich in zinc, copper, indium, germanium and the like and 0.43 kg conversion slag.
Precipitating the conversion solution in the step 2 step by adopting a known sulfide precipitation technology and recovering zinc, copper, indium and germanium in the conversion solution to respectively obtain sulfide precipitates of copper, indium and germanium, zinc sulfide precipitates and a purifying solution, and returning the purifying solution to the step 1 to be used as a size mixing solution; and (3) separating and recovering lead and silver by using a known flotation separation technology in the transformed slag in the step (2) to obtain hematite slag.
Respectively taking the conversion solution and the hematite conversion slag enriched with lead and silver for chemical component analysis, wherein the conversion solution contains 12.1g/L of zinc, 0.53g/L of copper, 22.5mg/L of indium and 10.77mg/L of germanium, and the conversion slag contains 62.2wt% of iron、1.36 wt% of lead and 0.01 wt% of silver; the leaching rate of zinc, the leaching rate of copper, the leaching rate of indium, and the leaching rate of germanium in this example were 97.8%, 98.5%, 86.8%, and 83.1%, respectively, and the enrichment ratios of lead and silver in the slag were 99.6% and 99.2%, respectively.
Example 3
As shown in FIG. 1, the method for recovering valuable metals and iron from jarosite slag comprises the following steps:
step 1, mixing and pulping 0.5kg of iron vitriol slag (iron vitriol slag 2) by using a dilute sulfuric acid solution according to a liquid-solid ratio of 2:1L/kg to obtain ore pulp, wherein the concentration of the dilute sulfuric acid solution is 10 g/L;
and 2, heating the ore pulp obtained in the step 1 to 250 ℃ without adding hematite seed crystals, carrying out pyrolysis and conversion reaction for 60min, and then carrying out liquid-solid separation to obtain 0.9L of valuable metal conversion liquid rich in zinc, copper, indium, germanium and the like and 0.25kg of conversion slag.
Precipitating the conversion solution in the step 2 step by adopting a known sulfide precipitation technology and recovering zinc, copper, indium and germanium in the conversion solution to respectively obtain sulfide precipitates of copper, indium and germanium, zinc sulfide precipitates and a purifying solution, and returning the purifying solution to the step 1 to be used as a size mixing solution; and (3) separating and recovering lead and silver by using a known flotation separation technology in the transformed slag in the step (2) to obtain hematite slag.
Respectively carrying out chemical component analysis on the conversion liquid in the step (2) and the hematite conversion slag enriched with lead and silver, wherein the conversion liquid contains 12.24g/L of zinc, 1.58g/L of copper, 146.5mg/L of indium and 35.78mg/L of germanium, and the conversion slag contains 56.8wt% of iron, 3.49 wt% of lead and 0.018 wt% of silver; the leaching rate of zinc, the leaching rate of copper, the leaching rate of indium, the leaching rate of germanium and the concentration ratio of lead and silver in the slag are respectively 99.2% and 99.6% in the example, which are calculated to be 97.5%, 98.1%, 82.4% and 80.5%.
Example 4
As shown in FIG. 1, the method for recovering valuable metals and iron from jarosite slag comprises the following steps:
step 1, mixing and pulping 0.5kg of iron vitriol slag (iron vitriol slag 2) and water according to a liquid-solid ratio of 8:1L/kg to obtain ore pulp;
and 2, adding hematite seed crystals with the concentration of 40g/L into the ore pulp obtained in the step 1, heating to the temperature of 220 ℃, carrying out pyrolysis and conversion reaction for 210min, and then carrying out liquid-solid separation to obtain 3.6L of valuable metal conversion liquid rich in zinc, copper, indium, germanium and the like and 0.4kg of conversion slag.
Precipitating the conversion solution in the step 2 step by adopting a known sulfide precipitation technology and recovering zinc, copper, indium and germanium in the conversion solution to respectively obtain sulfide precipitates of copper, indium and germanium, zinc sulfide precipitates and a purifying solution, and returning the purifying solution to the step 1 to be used as a size mixing solution; and (3) separating and recovering lead and silver by using a known flotation separation technology in the transformed slag in the step (2) to obtain hematite slag.
Respectively taking the conversion liquid in the step (2) and the hematite conversion slag enriched with lead and silver for chemical component analysis, wherein the conversion liquid contains 3.08g/L of zinc, 0.4g/L of copper, 37.6mg/L of indium and 9.17mg/L of germanium, and the conversion slag contains 58.2wt% of iron, 2.29wt% of lead and 0.011 wt% of silver; the leaching rate of zinc, copper, indium and germanium in this example was 98.1%, 98.9%, 84.6% and 82.5%, respectively, and the enrichment ratios of lead and silver in the slag were 99.5% and 99.7%, respectively.
While the present invention has been described in detail with reference to the embodiments shown in the drawings, the present invention is not limited to the embodiments, and various changes can be made without departing from the spirit and scope of the present invention.
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