CN105879840A - Organic-inorganic compound and application thereof in water treatment - Google Patents
Organic-inorganic compound and application thereof in water treatment Download PDFInfo
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- CN105879840A CN105879840A CN201610249628.4A CN201610249628A CN105879840A CN 105879840 A CN105879840 A CN 105879840A CN 201610249628 A CN201610249628 A CN 201610249628A CN 105879840 A CN105879840 A CN 105879840A
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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
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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
- B01J20/04—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising compounds of alkali metals, alkaline earth metals or magnesium
- B01J20/048—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising compounds of alkali metals, alkaline earth metals or magnesium containing phosphorus, e.g. phosphates, apatites, hydroxyapatites
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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
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
- B01J20/103—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate comprising silica
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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
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
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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
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
- B01J20/223—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material containing metals, e.g. organo-metallic compounds, coordination complexes
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- 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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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
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- Chemical Kinetics & Catalysis (AREA)
- Inorganic Chemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
The invention discloses an organic-inorganic compound and application thereof in water treatment. A preparation method of the organic-inorganic compound includes: adding a disodium hydrogen phosphate compound, silica sol and hexadecyltrimethylammonium chloride into water, and reacting for 3 h while back-flowing; adding inorganic ammonium salt, and continuing reaction for 1 h to obtain mixed liquid; adjusting temperature of the mixed liquid to 60 DEG C; filtering the mixed liquid, and drying a filter cake at 105 DEG C to obtain a solid material; dispersing the solid material in alcohol, adding a sodium acrylate water solution, and stirring for 20 min; adding acrylic acid and 2-acrylamido-2-methylpropanesulfonic acid, and stirring for 25 min; adding tetramethylorthosilicate and ammonium persulfate, and reaction at 80 DEG C for 4 h; drying reaction liquid to obtain the organic-inorganic compound. By using the organic-inorganic compound, wastewater can be effectively treated into water meeting emission standards.
Description
Technical field
The present invention relates to a kind of useless material for water treatment, be specifically related to a kind of organic-inorganic composite body removing metal in waste water and application thereof, belong to field of Environment Protection.
Background technology
Contaminated wastewater is one of environmentally hazardous major way.The plating that accounting is bigger the most in the industry, in the saline solution containing pre-plating, with plated parent metal as negative electrode, pass through electrolysis, make the cation of pre-plating in plating solution be deposited in base metal surface, form a kind of method of surface finish of coating.Electroplate the difference according to plating, the electroplating technology groove arranged also is not quite similar, but before general plated item completes the next electroplating technology groove of electroplating process entrance of an electroplating technology groove, will wash at rinsing bowl, the effect of rinsing bowl is the residual electroplate liquid wash clean above workpiece, under the influence of not, one technique is carried out, and does not pollute electroplate liquid in lower one electroplating bath, thus ensures the quality of plating.In electroplating processes process, according to the production of plating, need in the titanium basket of electroplating device, constantly add metal and in groove, add liquid medicine, through liquid medicine electrolytic metal to decomposite metal ion, be attached on plated item.The metal added such as copper ball also can produce when decompositing copper ion copper ashes,
The impurity such as copper wire, these metal impurities all can be discharged in water body, causes various problem.The waste water of electroplating facility discharge and waste liquid, such as plating piece washings, useless tank liquor, component cooling water and the flushing surface water etc., its water quality is different because of production technology, often oil-containing many kinds of metal ions, in general, often contains Cr6+、Cd2+、Ni2+、Cu2+、Zn2+、Fe2+Etc. heavy metal；Electroplating wastewater is poisonous, and harm is big.As cyanogen can cause people and animals' acute poisoning, lethal, low concentration long term also can cause chronic poisoning.Cadmium can make kidney generation pathological changes, and can cause itai-itai.Cr VI can cause pulmonary carcinoma, intestines and stomach disease and anemia, and can be in bone, the dirty interior accumulation of spleen and liver.Therefore, electroplating wastewater must strictly control, and deals carefully with.
Additionally or the industry such as intermetallic composite coating, framework welding, also it is the major source producing metallic wastewater.Prior art is mainly by adsorption treatment metal, but has little effect；The most necessary research and development are a kind of can effectively remove the material of metal in waste water.
Summary of the invention
It is an object of the invention to provide a kind of organic-inorganic composite body, it can effectively absorb the heavy metal in waste water, can be used for the efficient process of heavy metal-containing waste water.
To achieve the above object of the invention, the technical solution used in the present invention is: a kind of organic-inorganic composite body, following steps prepare: disodium hydrogen phosphate compound, Ludox, hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding inorganic ammonium salt, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then solid material is scattered in ethanol, adds aqueous sodium acrylate solution, stir 20 minutes；It is subsequently adding acrylic acid and 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding methyl silicate and Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
In the present invention, described disodium hydrogen phosphate compound is disodium hydrogen phosphate, ten water disodium hydrogen phosphates or six water disodium hydrogen phosphates；Described inorganic ammonium salt is ammonium sulfate, ammonium chloride or ammonium phosphate.Complex can be formed with silicon dioxide, increase the activity of silicon dioxide.
In the present invention, the mass concentration of described Ludox is 25%.The silicon dioxide gel of low concentration, can increase the dispersibility of inorganic matter, it is to avoid reunite.
In the present invention, described disodium hydrogen phosphate compound, Ludox, hexadecyltrimethylammonium chloride, the mass ratio of inorganic ammonium salt are (0.15～0.20): 1: (0.05～0.06): (0.15～0.18)；Described solid material, ethanol, sodium acrylate, acrylic acid, 2-acrylamide-2-methylpro panesulfonic acid, methyl silicate, the mass ratio of Ammonium persulfate. are (0.18～0.20): (0.5～0.6): (0.4～0.5): 1: (0.25～0.27): (0.15～0.17): (0.005～0.006).
The organic-inorganic composite body stable in properties of the present invention, has stronger adsorptivity to the heavy metal in waste water；Therefore the invention also discloses the application in water processes of the above-mentioned organic-inorganic composite body.
Present invention thing based on Ludox first, through series modified, cover organic polymer layers, thus obtains the metal-adsorbing material of stable performance on its surface；When the waste water containing metal processes, there is advantage efficient, segregative.
Detailed description of the invention
Embodiment one
A kind of organic-inorganic composite body, is prepared by following steps: 15g disodium hydrogen phosphate, 100g Ludox (25wt%), 5g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 15g ammonium sulfate, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 18g solid material is scattered in 50g ethanol, adds 400g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 25g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 15g methyl silicate and 0.5g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment two
A kind of organic-inorganic composite body, is prepared by following steps: 15g ten water disodium hydrogen phosphate, 100g Ludox (25wt%), 5g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 15g ammonium chloride, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 18g solid material is scattered in 50g ethanol, adds 400g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 25g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 15g methyl silicate and 0.5g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment three
A kind of organic-inorganic composite body, is prepared by following steps: 15g six water disodium hydrogen phosphate, 100g Ludox (25wt%), 5g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 15g ammonium phosphate, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 18g solid material is scattered in 50g ethanol, adds 400g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 25g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 15g methyl silicate and 0.5g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment four
A kind of organic-inorganic composite body, is prepared by following steps: 20g ten water disodium hydrogen phosphate, 100g Ludox (25wt%), 6g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 18g ammonium sulfate, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 18g solid material is scattered in 50g ethanol, adds 400g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 25g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 15g methyl silicate and 0.5g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment five
A kind of organic-inorganic composite body, is prepared by following steps: 15g ten water disodium hydrogen phosphate, 100g Ludox (25wt%), 5g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 15g ammonium sulfate, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 20g solid material is scattered in 60g ethanol, adds 500g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 27g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 17g methyl silicate and 0.6g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment six
A kind of organic-inorganic composite body, is prepared by following steps: 20g six water disodium hydrogen phosphate, 100g Ludox (25wt%), 6g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 18g ammonium phosphate, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 18g solid material is scattered in 50g ethanol, adds 400g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 25g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 15g methyl silicate and 0.5g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment seven
A kind of organic-inorganic composite body, is prepared by following steps: 20g disodium hydrogen phosphate, 100g Ludox (25wt%), 6g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 18g ammonium chloride, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 18g solid material is scattered in 50g ethanol, adds 400g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 25g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 15g methyl silicate and 0.5g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment eight
A kind of organic-inorganic composite body, is prepared by following steps: 15g disodium hydrogen phosphate, 100g Ludox (25wt%), 5g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 15g ammonium chloride, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 20g solid material is scattered in 60g ethanol, adds 500g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 27g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 17g methyl silicate and 0.6g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment nine
A kind of organic-inorganic composite body, is prepared by following steps: 15g six water disodium hydrogen phosphate, 100g Ludox (25wt%), 5g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 15g ammonium phosphate, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 20g solid material is scattered in 60g ethanol, adds 500g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 27g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 17g methyl silicate and 0.6g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Embodiment ten
A kind of organic-inorganic composite body, is prepared by following steps: 18g disodium hydrogen phosphate, 100g Ludox (25wt%), 6g hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding 15g ammonium sulfate, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then 19g solid material is scattered in 50g ethanol, adds 400g aqueous sodium acrylate solution (10wt%), stir 20 minutes；It is subsequently adding 100g acrylic acid and 26g 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding 15g methyl silicate and 0.5g Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Utilize above-mentioned water treatment agent to carry out waste water process, the results are shown in Table 1, it can be seen that waste water effectively is processed as meeting the water body of discharge standard by the water treatment agent of the present invention.
Each content of material (mg/L) before and after the process of table 1 water
| Ni2+ | Fe2+/3+ | Cr6+ | COD | Ag2+ | |
| Before process | 32.1 | 25.3 | 22.5 | 166.5 | 15.4 |
| Embodiment one | 0.01 | 0.01 | 0.01 | 11 | 0.01 |
| Embodiment two | 0.01 | 0.01 | 0.01 | 12 | 0.01 |
| Embodiment three | 0.01 | 0.01 | 0.01 | 10 | 0.01 |
| Embodiment four | 0.01 | 0.01 | 0.01 | 12 | 0.01 |
| Embodiment five | 0.01 | 0.01 | 0.01 | 10 | 0.01 |
| Embodiment six | 0.01 | 0.01 | 0.01 | 11 | 0.01 |
| Embodiment seven | 0.01 | 0.01 | 0.01 | 12 | 0.01 |
| Embodiment eight | 0.01 | 0.01 | 0.01 | 11 | 0.01 |
| Embodiment nine | 0.01 | 0.01 | 0.01 | 12 | 0.01 |
| Embodiment ten | 0.01 | 0.01 | 0.01 | 11 | 0.01 |
Claims (7)
1. an organic-inorganic composite body, it is characterised in that described organic-inorganic composite body is prepared by following steps: disodium hydrogen phosphate compound, Ludox, hexadecyltrimethylammonium chloride are added to the water, the lower reaction of backflow 3 hours；It is subsequently adding inorganic ammonium salt, continues reaction and obtain mixed liquor in 1 hour；Then regulation mixeding liquid temperature is 60 DEG C；Then filter mixed liquor, by filter cake in 105 DEG C of drying, obtains solid material；Then solid material is scattered in ethanol, adds aqueous sodium acrylate solution, stir 20 minutes；It is subsequently adding acrylic acid and 2-acrylamide-2-methylpro panesulfonic acid, stirs 25 minutes；Being subsequently adding methyl silicate and Ammonium persulfate., 80 DEG C are reacted 4 hours；Then dry reaction liquid i.e. obtains organic-inorganic composite body.
Organic-inorganic composite body the most according to claim 1, it is characterised in that: described disodium hydrogen phosphate compound is disodium hydrogen phosphate, ten water disodium hydrogen phosphates or six water disodium hydrogen phosphates.
Organic-inorganic composite body the most according to claim 1, it is characterised in that: described inorganic ammonium salt is ammonium sulfate, ammonium chloride or ammonium phosphate.
Organic-inorganic composite body the most according to claim 1, it is characterised in that: the mass concentration of described Ludox is 25%.
Organic-inorganic composite body the most according to claim 1, it is characterised in that: described disodium hydrogen phosphate compound, Ludox, hexadecyltrimethylammonium chloride, the mass ratio of inorganic ammonium salt are (0.15～0.20): 1: (0.05～0.06): (0.15～0.18).
Organic-inorganic composite body the most according to claim 1, it is characterised in that: described solid material, ethanol, sodium acrylate, acrylic acid, 2-acrylamide-2-methylpro panesulfonic acid, methyl silicate, the mass ratio of Ammonium persulfate. are (0.18～0.20): (0.5～0.6): (0.4～0.5): 1: (0.25～0.27): (0.15～0.17): (0.005～0.006).
7. the application in water processes of the organic-inorganic composite body described in claim 1.
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| CN111285504A (en) * | 2020-03-27 | 2020-06-16 | 无锡清诺环境工程有限公司 | Nickel-containing wastewater recycling treatment process and treatment system thereof |
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Application publication date: 20160824 |