CN105132691A - Method for refining metallic copper from used printed circuit board - Google Patents
Method for refining metallic copper from used printed circuit board Download PDFInfo
- Publication number
- CN105132691A CN105132691A CN201510610773.6A CN201510610773A CN105132691A CN 105132691 A CN105132691 A CN 105132691A CN 201510610773 A CN201510610773 A CN 201510610773A CN 105132691 A CN105132691 A CN 105132691A
- Authority
- CN
- China
- Prior art keywords
- copper
- circuit board
- printed circuit
- negative electrode
- bath
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 title claims abstract description 39
- 229910052802 copper Inorganic materials 0.000 title claims abstract description 38
- 239000010949 copper Substances 0.000 title claims abstract description 38
- 238000000034 method Methods 0.000 title claims abstract description 36
- 238000007670 refining Methods 0.000 title abstract 2
- 239000000758 substrate Substances 0.000 claims abstract description 15
- 238000005868 electrolysis reaction Methods 0.000 claims abstract description 12
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000010936 titanium Substances 0.000 claims abstract description 10
- 229910052719 titanium Inorganic materials 0.000 claims abstract description 10
- 239000002699 waste material Substances 0.000 claims description 29
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 10
- 239000008151 electrolyte solution Substances 0.000 claims description 8
- 238000006243 chemical reaction Methods 0.000 claims description 3
- 239000000284 extract Substances 0.000 claims description 3
- 239000007769 metal material Substances 0.000 abstract description 6
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 abstract description 5
- 239000003365 glass fiber Substances 0.000 abstract description 4
- 238000009776 industrial production Methods 0.000 abstract description 3
- 239000002344 surface layer Substances 0.000 abstract 3
- 239000003792 electrolyte Substances 0.000 abstract 2
- 238000005516 engineering process Methods 0.000 description 15
- 229910052751 metal Inorganic materials 0.000 description 8
- 239000002184 metal Substances 0.000 description 8
- 238000005336 cracking Methods 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- 238000013467 fragmentation Methods 0.000 description 4
- 238000006062 fragmentation reaction Methods 0.000 description 4
- 238000002386 leaching Methods 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- 229910021645 metal ion Inorganic materials 0.000 description 3
- 238000000197 pyrolysis Methods 0.000 description 3
- 238000004064 recycling Methods 0.000 description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 238000004587 chromatography analysis Methods 0.000 description 2
- 230000006378 damage Effects 0.000 description 2
- 238000001938 differential scanning calorimetry curve Methods 0.000 description 2
- 238000000605 extraction Methods 0.000 description 2
- 244000005700 microbiome Species 0.000 description 2
- 229910017604 nitric acid Inorganic materials 0.000 description 2
- 229910052755 nonmetal Inorganic materials 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 239000011347 resin Substances 0.000 description 2
- 229920005989 resin Polymers 0.000 description 2
- 238000002411 thermogravimetry Methods 0.000 description 2
- 238000001757 thermogravimetry curve Methods 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- HGUFODBRKLSHSI-UHFFFAOYSA-N 2,3,7,8-tetrachloro-dibenzo-p-dioxin Chemical compound O1C2=CC(Cl)=C(Cl)C=C2OC2=C1C=C(Cl)C(Cl)=C2 HGUFODBRKLSHSI-UHFFFAOYSA-N 0.000 description 1
- 238000003723 Smelting Methods 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000031018 biological processes and functions Effects 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 239000008139 complexing agent Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 229910000365 copper sulfate Inorganic materials 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000000113 differential scanning calorimetry Methods 0.000 description 1
- 238000006073 displacement reaction Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 150000002240 furans Chemical class 0.000 description 1
- 231100001261 hazardous Toxicity 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000007885 magnetic separation Methods 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 230000001473 noxious effect Effects 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000000053 physical method Methods 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 150000003071 polychlorinated biphenyls Chemical class 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 230000001698 pyrogenic effect Effects 0.000 description 1
- 238000012216 screening Methods 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 229920001187 thermosetting polymer Polymers 0.000 description 1
- -1 this Chemical compound 0.000 description 1
- 239000003440 toxic substance Substances 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
- 238000003466 welding Methods 0.000 description 1
Classifications
-
- 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
Landscapes
- Processing Of Solid Wastes (AREA)
- Manufacture And Refinement Of Metals (AREA)
- Electrolytic Production Of Metals (AREA)
Abstract
The invention relates to a method for refining metallic copper from a used printed circuit board. The method comprises the steps as follows: (a), a surface layer of the used printed circuit board is separated from a substrate of the used printed circuit board; (b), the surface layer serves as an anode, a titanium plate serves as a cathode, a copper sulphate solution serves as an electrolyte, and a disconnected electrolytic tank is formed after a direct-current supply is connected; and (c), the space between the anode and the cathode is adjusted to be in a range of 2-12 cm, the voltage of the direct-current supply is 1-5 V, the temperature of the copper sulphate solution is in a range of 25-50 DEG C, the circuit is switched on, and electrolysis is carried out for 0.5-5 h, so that copper obtained from the cathode is collected. The surface layer serves as the anode, the titanium plate serves as the cathode, the copper sulphate solution serves as the electrolyte, so that the electrolytic tank is formed; electrolytic parameters are controlled precisely, high-purity copper can be obtained from the cathode, and the copper can be directly used for industrial production; and besides, the used copper sulphate solution can be reused, secondary pollution cannot be caused to the environment, and the used printed circuit board is not required to be broken up, so that not only the electrolysis process is simplified, but also the property of non-metallic materials such as glass fibers is avoided from being damaged.
Description
Technical field
The invention belongs to salvage material field, relate to a kind of method extracting metallic copper, be specifically related to a kind of method extracting metallic copper from waste printed circuit board.
Background technology
Printed-wiring board (PWB) (PrintedcircuitBonds, PCBs) is that substrate, copper rivet on substrate and Copper Foil and the electronic devices and components etc. prepared by resin and glass fiber material are formed.Printed-wiring board (PWB) is widely used in the fields such as information, communication, electronics, military affairs, space flight.Along with the development of science and technology and the continuous expansion of every field demand printed-wiring board (PWB), the quantity also sharp increase of the waste printed circuit board produced.Multiple hazardous and noxious substances on the one hand in waste printed circuit board has to pass through recycling; Heavy metal element on the other hand in waste printed circuit board substrate has again high resource recycling and is worth, and is a kind of potential secondary resource.Therefore, rationally the effective waste printed circuit board that reclaims all has great significance to economy and environmental protection.
At present, the technology extracting metal both at home and abroad from old circuit board is mainly four kinds, i.e. mechanical treatment technology, heat treatment technics, hydrometallurgical technology and biotechnology.
What mechanical treatment technology mainly adopted is physical method, first realizes waste printed circuit board metal by fragmentation and nonmetallicly to dissociate, different then according to institute's containing metal and nonmetal character, utilizes different sorting ways to be separated by these materials.The mechanical treatment technology of discarded circuit board has: disassemble, fragmentation, pneumatic separating, magnetic separation, screening, eddy current sorting, electric separation etc.This method can be separated with nonmetal realization preferably to metal, and its flow process is simple, and to environment without destruction, but will pulverize waste printed circuit board substrate during sorting, after sorting, the purity of each component of gained is not high, can not directly be recycled by industry.
Hydrometallurgical technology processes waste and old circuit board with the acid of strong oxidizing property, the metal ion then in purification leach liquor, adopts displacement or electrolysis treatment technique Footwall drift.The shortcoming of the method is that the strong oxidizers such as the nitric acid used can discharge NO in treating processes
x, contaminate environment, and create a large amount of waste liquid, easily cause secondary pollution.In addition, when leaching the metal in substrate with the strong acid such as nitric acid, sulfuric acid, can there is oxidation and be destroyed in substrate non-metallic material on the one hand; The metal ion dissolved on the other hand also can destroy the molecular structure of non-metallic material on substrate makes non-metallic material performance reduce.
Heat treatment technics old circuit board is placed in high-temperature smelting pot burn, and removes the inorganic components such as resin, recycles the precious metal in pyrogenic process and electrolytic process recovery lime-ash afterwards.The shortcoming of present method is: can produce a large amount of smog also having the toxic substances such as dioxin, furans and polychlorobiphenyl in burning process, there is secondary pollution and personnel safety hidden danger.
Biotechnology a kind ofly utilizes microorganism to carry out the technology of specific absorption or cooperation to special metal ion.This method technique is simple, running cost is low, easy and simple to handle, but the cultivation fee of microorganism is comparatively large and treatment cycle is longer.At present, the correlative study of biological process is still in laboratory stage.
Hydrometallurgical technology and heat treatment technics grow up on the basis that metalliferous mineral is smelted, and technology is comparatively ripe, and cost is lower, and Footwall drift purity is higher.Relative to heat treatment technics, hydrometallurgical technology needs to consume the leaching that a large amount of chemical reagent carries out metal, but technique is simply ripe, and do not produce a large amount of toxic and harmful, energy consumption is less, and proper handling can greatly reduce the pollution to environment.For hydrometallurgical technology, the key problem in technology extracting copper is the purity problem etc. of the leaching aspect of copper and the copper of extraction.At present, the technology of conventional wet underwater welding copper is relatively loaded down with trivial details, not only relate to the configuration of complicated leaching copper system solution, as complexing agent, strong oxidizer, extraction agent, the choosing and consumption of strippant, also can produce a large amount of toxic and harmful contaminate environment in the process extracting copper.
Summary of the invention
The present invention seeks to provide a kind of method extracting metallic copper from waste printed circuit board to overcome the deficiencies in the prior art.
For achieving the above object, the technical solution used in the present invention is: a kind of method extracting metallic copper from waste printed circuit board, and it comprises the following steps:
A the upper layer of waste printed circuit board is separated from its substrate by ();
(b) with described upper layer be anode, titanium plate is negative electrode, copper-bath for electrolytic solution, form the electrolyzer of open circuit after connecting direct supply;
C the spacing of () adjustment anode and negative electrode is 2 ~ 12cm, direct current power source voltage is 1 ~ 5V, the temperature of copper-bath is 25 ~ 50 DEG C, connects circuit electrolysis 0.5 ~ 5h, collects the copper that negative electrode obtains.
Optimally, the concentration of described copper-bath is 0.1 ~ 1mol/L.
Optimally, described copper-bath is obtained by the copper that negative electrode obtains and sulfuric acid reaction.
Because technique scheme is used, the present invention compared with prior art has following advantages: the present invention extracts the method for metallic copper from waste printed circuit board, take upper layer as anode, titanium plate is negative electrode, copper-bath forms electrolyzer for electrolytic solution, and accurately control electrolytic parameter, high purity volume copper can be obtained on negative electrode, can industrial production be directly used in; And the copper-bath used can recycle, secondary pollution can not being caused to environment, because waste and old circuit board is without the need to carrying out fragmentation, not only simplify electrolysis process, also make the character of non-metallic material as glass fibre do not damaged, greatly expand its second stage employ scope.
Embodiment
The present invention extracts the method for metallic copper from waste printed circuit board, and it comprises the following steps: the upper layer of waste printed circuit board is separated from its substrate by (a); (b) with described upper layer be anode, titanium plate is negative electrode, copper-bath for electrolytic solution, form the electrolyzer of open circuit after connecting direct supply; C the spacing of () adjustment anode and negative electrode is 2 ~ 12cm, direct current power source voltage is 1 ~ 5V, the temperature of copper-bath is 25 ~ 50 DEG C, connects circuit electrolysis 0.5 ~ 5h, collects the copper that negative electrode obtains.Take upper layer as anode, titanium plate is negative electrode, copper-bath forms electrolyzer for electrolytic solution, and accurately control electrolytic parameter, high purity volume copper can be obtained on negative electrode, can industrial production be directly used in; And the copper-bath used can recycle, secondary pollution can not being caused to environment, because waste and old circuit board is without the need to carrying out fragmentation, not only simplify electrolysis process, also make the character of non-metallic material as glass fibre do not damaged, greatly expand its second stage employ scope.The concentration of copper-bath is preferred 0.1 ~ 1mol/L, and copper-bath is obtained by the copper that negative electrode obtains and sulfuric acid reaction, can save the consumption of copper sulfate like this, cost-saving, reduces the destruction to environment.
In step (a), by the concrete grammar that the upper layer of waste printed circuit board is separated from its substrate be: (S1) gets discarded circuit board and carry out differential scanning calorimetry (DSC) respectively and thermogravimetric analysis (TGA) test obtains corresponding analytic curve, determines cracking temperature region; It should be noted that cracking temperature region needs comprehensively to analyze according to DSC curve and TGA curve, first the temperature range of component or material fast degradation in TGA curve determination discarded circuit board is utilized, subsequently according to the main peak of first on DSC curve and second main peak determination cracking temperature region (cracking temperature region is that first main peak peak value place to the second main peak starts temperature range corresponding to forming position, is preferably 300 ~ 450 DEG C); (S2) tube furnace is warming up to the arbitrary temperature in described cracking temperature region, (inert gas flow can adjust according to actual process to pass into rare gas element continuously, as long as guarantee that discarded circuit board is not oxidized), subsequently sample is pushed away boat feeding effective heating warm area and carry out insulation 10 ~ 60 minutes, until metal level generation warpage; (S3) collection container is connected in described tube furnace exit, the gas discharged in heat-obtaining solution preocess carries out gas chromatographic analysis, according to gas chromatographic analysis result determination recovery scheme, carry out recycling that (pyrolysis gas produced in pyrolytic process and pyrolysis oil can be reclaimed, to make the energy or starting material carry out secondary use, to reach the maximum utilizationization of resource); (S4) by after the discarded circuit board cooling after pyrolysis, glasscloth and metal level is peeled off; The upper layer obtained like this has higher quality, is conducive to the productive rate improving metallic copper.
Below in conjunction with embodiment, the present invention is further described.
Embodiment 1
The present embodiment provides a kind of method extracting metallic copper from waste printed circuit board, and it comprises the following steps:
A the upper layer of waste printed circuit board is separated from its substrate by ();
(b) with described upper layer be anode, titanium plate is negative electrode, 0.1mol/L copper-bath for electrolytic solution, form the electrolyzer of open circuit after connecting direct supply;
C the spacing of () adjustment anode and negative electrode is 12cm, direct current power source voltage is 1V, the temperature of copper-bath is 50 DEG C, connects circuit electrolysis 5h, collects the copper that negative electrode obtains; Because electrolysis time is longer, after copper-bath concentration is thinning, the copper that power taking solution obtains adds in sulfuric acid, adds thermosetting copper-bath, adds in thinning previous solu, makes its concentration keep being about 0.1mol/L.
Embodiment 2
The present embodiment provides a kind of method extracting metallic copper from waste printed circuit board, and it comprises the following steps:
A the upper layer of waste printed circuit board is separated from its substrate by ();
(b) with described upper layer be anode, titanium plate is negative electrode, 1mol/L copper-bath for electrolytic solution, form the electrolyzer of open circuit after connecting direct supply;
C the spacing of () adjustment anode and negative electrode is 2cm, direct current power source voltage is 5V, the temperature of copper-bath is 25 DEG C, connects circuit electrolysis 0.5h, collects the copper that negative electrode obtains.
Embodiment 3
The present embodiment provides a kind of method extracting metallic copper from waste printed circuit board, and it comprises the following steps:
A the upper layer of waste printed circuit board is separated from its substrate by ();
(b) with described upper layer be anode, titanium plate is negative electrode, 0.5mol/L copper-bath for electrolytic solution, form the electrolyzer of open circuit after connecting direct supply;
C the spacing of () adjustment anode and negative electrode is 5cm, direct current power source voltage is 3V, the temperature of copper-bath is 30 DEG C, connects circuit electrolysis 2h, collects the copper that negative electrode obtains.
Above-described embodiment is only for illustrating technical conceive of the present invention and feature; its object is to person skilled in the art can be understood content of the present invention and implement according to this; can not limit the scope of the invention with this; all equivalences done according to spirit of the present invention change or modify, and all should be encompassed within protection scope of the present invention.
Claims (3)
1. from waste printed circuit board, extract a method for metallic copper, it is characterized in that, it comprises the following steps:
A the upper layer of waste printed circuit board is separated from its substrate by ();
(b) with described upper layer be anode, titanium plate is negative electrode, copper-bath for electrolytic solution, form the electrolyzer of open circuit after connecting direct supply;
C the spacing of () adjustment anode and negative electrode is 2 ~ 12cm, direct current power source voltage is 1 ~ 5V, the temperature of copper-bath is 25 ~ 50 DEG C, connects circuit electrolysis 0.5 ~ 5h, collects the copper that negative electrode obtains.
2. the method extracting metallic copper from waste printed circuit board according to claim 1, is characterized in that: the concentration of described copper-bath is 0.1 ~ 1mol/L.
3. the method extracting metallic copper from waste printed circuit board according to claim 1, is characterized in that: described copper-bath is obtained by the copper that negative electrode obtains and sulfuric acid reaction.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510610773.6A CN105132691B (en) | 2015-09-23 | 2015-09-23 | A kind of method that metallic copper is extracted from waste printed circuit board |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510610773.6A CN105132691B (en) | 2015-09-23 | 2015-09-23 | A kind of method that metallic copper is extracted from waste printed circuit board |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN105132691A true CN105132691A (en) | 2015-12-09 |
| CN105132691B CN105132691B (en) | 2018-02-13 |
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201510610773.6A Active CN105132691B (en) | 2015-09-23 | 2015-09-23 | A kind of method that metallic copper is extracted from waste printed circuit board |
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| Country | Link |
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| CN (1) | CN105132691B (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106676577A (en) * | 2017-02-06 | 2017-05-17 | 中国科学院过程工程研究所 | Method for recovering copper from used circuit board |
| CN112439521A (en) * | 2020-11-02 | 2021-03-05 | 安徽瀚中菲欧新材料有限公司 | Copper recovery device of waste circuit board |
Citations (1)
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| CN103388160A (en) * | 2013-07-19 | 2013-11-13 | 北京科技大学 | Method for preparation of ultrafine copper powder by waste circuit board copper dissolution-electrodeposition combined method |
-
2015
- 2015-09-23 CN CN201510610773.6A patent/CN105132691B/en active Active
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103388160A (en) * | 2013-07-19 | 2013-11-13 | 北京科技大学 | Method for preparation of ultrafine copper powder by waste circuit board copper dissolution-electrodeposition combined method |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106676577A (en) * | 2017-02-06 | 2017-05-17 | 中国科学院过程工程研究所 | Method for recovering copper from used circuit board |
| CN106676577B (en) * | 2017-02-06 | 2019-03-22 | 中国科学院过程工程研究所 | A method of recycling copper from waste and old circuit board |
| CN112439521A (en) * | 2020-11-02 | 2021-03-05 | 安徽瀚中菲欧新材料有限公司 | Copper recovery device of waste circuit board |
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| CN105132691B (en) | 2018-02-13 |
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Effective date of registration: 20231128 Address after: Building 8, No. 1 and No. 2, No. 999 Haifeng North Road, Cidong Binhai District, Longshan Town, Cixi City, Ningbo City, Zhejiang Province, 315100 Patentee after: NINGBO HENGCHUANG ENVIRONMENTAL PROTECTION TECHNOLOGY Co.,Ltd. Patentee after: NINGBO TONGDAO HENGXIN ENVIRONMENTAL PROTECTION TECHNOLOGY Co.,Ltd. Patentee after: INSTITUTE OF CHEMISTRY, CHINESE ACADEMY OF SCIENCES Address before: 315311, No.1 and No.2, Building 8, No. 999 Haifeng North Road, Cidong Binhai District, Longshan Town, Cixi City, Ningbo City, Zhejiang Province Patentee before: NINGBO HENGCHUANG ENVIRONMENTAL PROTECTION TECHNOLOGY Co.,Ltd. Patentee before: NINGBO TONGDAO HENGXIN ENVIRONMENTAL PROTECTION TECHNOLOGY Co.,Ltd. |
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