CN105771900A - Iron-loaded modified active carbon and preparation method thereof - Google Patents
Iron-loaded modified active carbon and preparation method thereof Download PDFInfo
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- CN105771900A CN105771900A CN201610309311.5A CN201610309311A CN105771900A CN 105771900 A CN105771900 A CN 105771900A CN 201610309311 A CN201610309311 A CN 201610309311A CN 105771900 A CN105771900 A CN 105771900A
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 59
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 24
- 229910052742 iron Inorganic materials 0.000 title claims abstract description 15
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- 229910052799 carbon Inorganic materials 0.000 title abstract 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 15
- 150000002505 iron Chemical class 0.000 claims abstract description 10
- 239000012153 distilled water Substances 0.000 claims abstract description 7
- 239000012670 alkaline solution Substances 0.000 claims abstract description 5
- 239000000203 mixture Substances 0.000 claims abstract description 5
- 238000007598 dipping method Methods 0.000 claims abstract 4
- 238000002156 mixing Methods 0.000 claims abstract 3
- 230000001105 regulatory effect Effects 0.000 claims abstract 3
- 239000000243 solution Substances 0.000 claims description 18
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 claims description 8
- -1 iron modified activated carbon Chemical class 0.000 claims description 7
- FBAFATDZDUQKNH-UHFFFAOYSA-M iron chloride Chemical group [Cl-].[Fe] FBAFATDZDUQKNH-UHFFFAOYSA-M 0.000 claims 2
- 229910000358 iron sulfate Inorganic materials 0.000 claims 2
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims 2
- 238000002604 ultrasonography Methods 0.000 claims 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 abstract description 20
- 229910052698 phosphorus Inorganic materials 0.000 abstract description 20
- 239000011574 phosphorus Substances 0.000 abstract description 20
- 244000144972 livestock Species 0.000 abstract description 6
- 238000000034 method Methods 0.000 abstract description 6
- 244000144977 poultry Species 0.000 abstract description 6
- 210000003608 fece Anatomy 0.000 abstract description 5
- 238000009395 breeding Methods 0.000 abstract description 4
- 230000001488 breeding effect Effects 0.000 abstract description 4
- 238000012986 modification Methods 0.000 abstract description 3
- 230000004048 modification Effects 0.000 abstract description 3
- 239000002699 waste material Substances 0.000 abstract description 3
- 239000002154 agricultural waste Substances 0.000 abstract description 2
- 230000007547 defect Effects 0.000 abstract 1
- 238000001035 drying Methods 0.000 abstract 1
- 238000001914 filtration Methods 0.000 abstract 1
- 238000002715 modification method Methods 0.000 abstract 1
- 239000000843 powder Substances 0.000 abstract 1
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 12
- 238000011161 development Methods 0.000 description 5
- 229910021578 Iron(III) chloride Inorganic materials 0.000 description 3
- APUPEJJSWDHEBO-UHFFFAOYSA-P ammonium molybdate Chemical compound [NH4+].[NH4+].[O-][Mo]([O-])(=O)=O APUPEJJSWDHEBO-UHFFFAOYSA-P 0.000 description 3
- 239000011609 ammonium molybdate Substances 0.000 description 3
- 229940010552 ammonium molybdate Drugs 0.000 description 3
- 235000018660 ammonium molybdate Nutrition 0.000 description 3
- 238000012851 eutrophication Methods 0.000 description 3
- 239000000706 filtrate Substances 0.000 description 3
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 description 3
- 238000002798 spectrophotometry method Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 238000007654 immersion Methods 0.000 description 2
- RUTXIHLAWFEWGM-UHFFFAOYSA-H iron(3+) sulfate Chemical compound [Fe+3].[Fe+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O RUTXIHLAWFEWGM-UHFFFAOYSA-H 0.000 description 2
- 229910000360 iron(III) sulfate Inorganic materials 0.000 description 2
- 235000015097 nutrients Nutrition 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000010561 standard procedure Methods 0.000 description 2
- 238000000967 suction filtration Methods 0.000 description 2
- 241000195493 Cryptophyta Species 0.000 description 1
- VTLYFUHAOXGGBS-UHFFFAOYSA-N Fe3+ Chemical compound [Fe+3] VTLYFUHAOXGGBS-UHFFFAOYSA-N 0.000 description 1
- 241000282414 Homo sapiens Species 0.000 description 1
- 238000009360 aquaculture Methods 0.000 description 1
- 244000144974 aquaculture Species 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 229910001447 ferric ion Inorganic materials 0.000 description 1
- 125000000524 functional group Chemical group 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- 229910017053 inorganic salt Inorganic materials 0.000 description 1
- 239000010871 livestock manure Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000005070 sampling Methods 0.000 description 1
- 238000003911 water pollution Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/0203—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising compounds of metals not provided for in B01J20/04
- B01J20/0225—Compounds of Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt
- B01J20/0229—Compounds of Fe
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/281—Treatment of water, waste water, or sewage by sorption using inorganic sorbents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/288—Treatment of water, waste water, or sewage by sorption using composite sorbents, e.g. coated, impregnated, multi-layered
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Hydrology & Water Resources (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Life Sciences & Earth Sciences (AREA)
- Analytical Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Carbon And Carbon Compounds (AREA)
- Water Treatment By Sorption (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
Description
技术领域 technical field
本发明属于活性炭的改性领域，尤其涉及一种负载铁改性活性炭及其制备方法。 The invention belongs to the field of modification of activated carbon, and in particular relates to an iron-loaded modified activated carbon and a preparation method thereof.
背景技术 Background technique
随着工业迅猛发展，人类在工农业发展及日常生活中，向水体中排放的污染物日益增多，加速了河流湖泊的富营养化进程。富营养化问题是当今世界面临的严峻水污染问题之一。水体富营养化主要是因为水体中含有的氮、磷等可供藻类利用的营养物质过多，其中磷是富营养化水体的限制因子，磷的去除对于营养化水体的修复具有重要意义。养殖业是我国农村发展的重要产业。近年来，随着规模化畜禽养殖业的发展，畜禽废弃物产量也随之不断增加。对畜禽粪便进行综合利用，使之无害化、资源化，才能有效解决其污染问题，从而实现畜禽养殖业的可持续发展。 With the rapid development of industry, human beings discharge more and more pollutants into water bodies in the development of industry and agriculture and daily life, which accelerates the eutrophication process of rivers and lakes. Eutrophication is one of the serious water pollution problems facing the world today. The eutrophication of the water body is mainly due to the fact that the water contains too many nutrients such as nitrogen and phosphorus that can be used by algae. Among them, phosphorus is the limiting factor of the eutrophic water body, and the removal of phosphorus is of great significance for the restoration of the nutrient water body. Aquaculture is an important industry for the development of rural areas in my country. In recent years, with the development of large-scale livestock and poultry breeding industry, the output of livestock and poultry waste has also been increasing. The comprehensive utilization of livestock and poultry manure to make it harmless and resourceful can effectively solve the pollution problem and achieve sustainable development of the livestock and poultry breeding industry.
发明内容 Contents of the invention
本发明的目的在于针对现有技术中存在的问题，提供一种负载铁改性活性炭的制备方法，采用畜禽养殖废弃物牛粪制备活性炭，实现农业废物的综合利用，并将其进一步用铁改性，提高其对污染物如磷的去除效率。 The purpose of the present invention is to solve the problems existing in the prior art, to provide a preparation method of iron-loaded modified activated carbon, using livestock and poultry breeding waste cow dung to prepare activated carbon, realizing the comprehensive utilization of agricultural waste, and further using iron Modification to improve its removal efficiency for pollutants such as phosphorus.
一种负载铁改性活性炭，通过以下步骤制备得到： A kind of loaded iron modified activated carbon is prepared through the following steps:
(1)称取质量比为1:1～1:10的粉末活性炭和铁盐混合，溶于常温下的蒸馏水中； (1) Take powdered activated carbon and iron salt with a mass ratio of 1:1 to 1:10 and mix them, and dissolve them in distilled water at normal temperature;
(2)将所述步骤(1)中的混合物在超声波下浸渍15～45min，浸渍温度为25～55℃； (2) impregnating the mixture in the step (1) under ultrasonic waves for 15 to 45 minutes, and the immersion temperature is 25 to 55° C.;
(3)用碱性溶液调节溶液pH为7～8，静置24h后，过滤并烘干。 (3) Adjust the pH of the solution to 7-8 with an alkaline solution, and after standing for 24 hours, filter and dry.
所述粉末活性炭，采用牛粪为原料，通过现有制备方法制备得到。 The powdered activated carbon is prepared by using cow dung as a raw material through an existing preparation method.
进一步地，所述铁盐为含三价铁离子的无机盐，包括氯化铁、硫酸铁、硝酸铁。 Further, the iron salt is an inorganic salt containing ferric ions, including ferric chloride, ferric sulfate, and ferric nitrate.
优选地，所述粉末活性炭与铁盐的质量比为1:2。 Preferably, the mass ratio of the powdered activated carbon to the iron salt is 1:2.
优选地，所述浸渍温度为30℃。 Preferably, the immersion temperature is 30°C.
进一步地，所述碱性溶液为氢氧化钠溶液。 Further, the alkaline solution is sodium hydroxide solution.
本发明的制备方法，摒弃传统的直接浸渍法耗时长的缺点，利用超声波，使活性炭对氯化铁的负载效率达到99.6％，几乎完全负载，并且耗时时间短。改性后的活性炭对含磷溶液去除率最高达96％。 The preparation method of the present invention abandons the time-consuming shortcoming of the traditional direct impregnation method, and uses ultrasonic waves to make the loading efficiency of activated carbon on ferric chloride reach 99.6%, which is almost completely loaded, and takes a short time. The modified activated carbon can remove up to 96% of phosphorus-containing solution.
附图说明 Description of drawings
图1为本发明实施例1改性活性炭的SEM图； Fig. 1 is the SEM figure of the embodiment of the present invention 1 modified activated carbon;
图2为本发明实施例1改性活性炭的红外光谱图； Fig. 2 is the infrared spectrogram of the embodiment of the present invention 1 modified activated carbon;
图3为本发明实施例1改性活性炭的XRD图。 Fig. 3 is the XRD figure of the modified activated carbon of Example 1 of the present invention.
具体实施方式 detailed description
实施例1 Example 1
称取1g粉末活性炭和2g氯化铁混合，溶于100ml蒸馏水中；然后置于超声波仪中，在30℃下浸渍40min后拿出；用氢氧化钠溶液调节pH为7～8，静置24h后，用真空抽滤机过滤溶液，再将所剩活性炭用马弗炉110℃烘干。 Weigh 1g of powdered activated carbon and 2g of ferric chloride, dissolve in 100ml of distilled water; then place it in an ultrasonic instrument, soak it at 30°C for 40min and take it out; adjust the pH to 7-8 with sodium hydroxide solution, and let it stand for 24h Finally, filter the solution with a vacuum filter, and then dry the remaining activated carbon with a muffle furnace at 110°C.
如图所示，负载Fe3+后活性炭的表面结构发生了明显的改变，含铁化合物均匀的填充了活性炭的孔隙，大部分为团聚的颗粒，使得活性炭表面更加的粗糙，无序。负载的铁与牛粪基活性炭中的含氧官能团进行了结合，促进了与磷系物的吸附结合，从而达到去除水质中磷的效果。 As shown in the figure, the surface structure of activated carbon changed significantly after loading Fe 3+ , and the iron-containing compounds uniformly filled the pores of activated carbon, most of which were agglomerated particles, making the surface of activated carbon rougher and disordered. The loaded iron is combined with the oxygen-containing functional groups in the cow dung-based activated carbon, which promotes the adsorption and combination with phosphorus, so as to achieve the effect of removing phosphorus in water quality.
称量0.1g实施例1所述成品于100ml带塞锥形瓶中，加入100ml20mg/L含磷溶液，在30℃下，放置于恒温振荡器中，24h后取出抽滤，用水质总磷的测定国标法(GB-1189389)钼酸铵分光光度法测量滤液的含磷溶液浓度0.698mg/L，故本试样对含磷溶液的去除率为(20-0.698)/20＝96.51％。 Weigh 0.1g of the finished product described in Example 1 into a 100ml Erlenmeyer flask with a stopper, add 100ml of 20mg/L phosphorus-containing solution, place it in a constant temperature oscillator at 30°C, take it out after 24h for suction filtration, and use water quality total phosphorus Determining national standard method (GB-1189389) ammonium molybdate spectrophotometry measures the phosphorus-containing solution concentration 0.698mg/L of filtrate, so this sample is to the removal rate of phosphorus-containing solution (20-0.698)/20=96.51%.
称量0.1g实施例1所述成品于100ml带塞锥形瓶中，加入100ml20mg/L含磷溶液，在25℃下，放置于恒温振荡器中，分别在2、5、10、20、30、40、60、80、120、240min取样，抽滤，用水质总磷的测定国标法(GB-1189389)钼酸铵分光光度法测量滤液的含磷溶液浓度采用准二级动力学方程进行拟合：v0＝k2qe 2。得到R2＝0.9996的方程，根据方程系数得吸附平衡浓度达15.02mg/g。 Weigh 0.1g of the finished product described in Example 1 into a 100ml Erlenmeyer flask with a stopper, add 100ml of 20mg/L phosphorus-containing solution, place it in a constant temperature oscillator at 25°C, and set it at 2, 5, 10, 20, 30 , 40, 60, 80, 120, 240min sampling, suction filtration, water quality total phosphorus determination national standard method (GB-1189389) ammonium molybdate spectrophotometric method to measure the concentration of phosphorus-containing solution in the filtrate using pseudo-second-order kinetic equation to simulate combine: v 0 =k 2 q e 2 . The equation of R 2 =0.9996 is obtained, and the adsorption equilibrium concentration reaches 15.02mg/g according to the coefficient of the equation.
对比例1 Comparative example 1
称量0.1g非改性活性炭于100ml带塞锥形瓶中，加入100ml20mg/L含磷溶液，在30℃下，放置于恒温振荡器中，24h后取出抽滤，用水质总磷的测定国标法(GB-1189389)钼酸铵分光光度法测量滤液的含磷溶液浓度，相比原始含磷浓度不降反升，去除率为负。 Weigh 0.1g of non-modified activated carbon into a 100ml conical flask with stopper, add 100ml of 20mg/L phosphorus-containing solution, place it in a constant temperature oscillator at 30°C, take it out and filter it after 24 hours, and use it to determine the national standard for total phosphorus Method (GB-1189389) ammonium molybdate spectrophotometric method to measure the phosphorus-containing solution concentration of the filtrate, compared with the original phosphorus-containing concentration does not fall but rises, and the removal rate is negative.
研究所得，非本发明方法改性制得的活性炭对磷的最优去除率仅40％-50％。 According to research results, the optimal removal rate of phosphorus by activated carbon not modified by the method of the present invention is only 40%-50%.
实施例2 Example 2
称取1g粉末活性炭和5g硫酸铁混合，溶于100ml蒸馏水中；然后置于超声波仪中，在25℃下浸渍15min后拿出；用氢氧化钠溶液调节pH为7～8，静置24h后，用真空抽滤机过滤溶液，再将所剩活性炭用马弗炉110℃烘干。 Weigh 1g of powdered activated carbon and 5g of ferric sulfate, dissolve them in 100ml of distilled water; then place them in an ultrasonic instrument, soak them at 25°C for 15 minutes and take them out; adjust the pH to 7-8 with sodium hydroxide solution, and let them stand for 24 hours , filter the solution with a vacuum filter, and then dry the remaining activated carbon with a muffle furnace at 110°C.
实施例3 Example 3
称取1g粉末活性炭和10g硝酸铁混合，溶于100ml蒸馏水中；然后置于超声波仪中，在55℃下浸渍45min后拿出；用氢氧化钠溶液调节pH为7～8，静置24h后，用真空抽滤机过滤溶液，再将所剩活性炭用马弗炉110℃烘干。 Weigh 1g of powdered activated carbon and 10g of ferric nitrate, dissolve in 100ml of distilled water; then place it in an ultrasonic instrument, soak it at 55°C for 45min and take it out; adjust the pH to 7-8 with sodium hydroxide solution, and let it stand for 24h , filter the solution with a vacuum filter, and then dry the remaining activated carbon with a muffle furnace at 110°C.
Claims (6)
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Cited By (6)
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| CN106902733A (en) * | 2017-02-15 | 2017-06-30 | 上海理工大学 | A kind of preparation method of cotton leftover bits and pieces base load iron absorbent charcoal material |
| CN107970890A (en) * | 2017-11-30 | 2018-05-01 | 华南理工大学 | A kind of hydroxyl iron-loaded modified activated carbon composite material and preparation method thereof |
| CN110684539A (en) * | 2019-10-24 | 2020-01-14 | 河南城建学院 | Conditioner for heavy metal polluted soil and preparation method thereof |
| CN111644153A (en) * | 2019-07-26 | 2020-09-11 | 中山大学 | Supported activated carbon and preparation method and device thereof |
| CN111729646A (en) * | 2020-06-15 | 2020-10-02 | 安徽农业大学 | A kind of EGCG-iron particulate green material for removing phosphorus in water and its preparation method and application |
| WO2021256946A1 (en) * | 2020-06-17 | 2021-12-23 | Qatar Foundation For Education, Science And Community Development | Activated carbon-composite materials, filters, and preparation methods thereof |
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| CN106902733A (en) * | 2017-02-15 | 2017-06-30 | 上海理工大学 | A kind of preparation method of cotton leftover bits and pieces base load iron absorbent charcoal material |
| CN107970890A (en) * | 2017-11-30 | 2018-05-01 | 华南理工大学 | A kind of hydroxyl iron-loaded modified activated carbon composite material and preparation method thereof |
| CN111644153A (en) * | 2019-07-26 | 2020-09-11 | 中山大学 | Supported activated carbon and preparation method and device thereof |
| CN110684539A (en) * | 2019-10-24 | 2020-01-14 | 河南城建学院 | Conditioner for heavy metal polluted soil and preparation method thereof |
| CN110684539B (en) * | 2019-10-24 | 2022-04-19 | 河南城建学院 | Conditioner for heavy metal polluted soil and preparation method thereof |
| CN111729646A (en) * | 2020-06-15 | 2020-10-02 | 安徽农业大学 | A kind of EGCG-iron particulate green material for removing phosphorus in water and its preparation method and application |
| WO2021256946A1 (en) * | 2020-06-17 | 2021-12-23 | Qatar Foundation For Education, Science And Community Development | Activated carbon-composite materials, filters, and preparation methods thereof |
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Inventor after: Liu Tingfeng Inventor after: Hu Zhixin Inventor after: Lu Weiwei Inventor after: Wang Er Inventor after: Qin Ling Inventor after: Tao Bingchi Inventor after: Chen Fei Inventor before: Lu Weiwei Inventor before: Liu Tingfeng Inventor before: Wang Er Inventor before: Qin Ling Inventor before: Tao Bingchi Inventor before: Chen Fei |
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Application publication date: 20160720 |