CN103861542A - Reaction device for preparing hydrogen through solar photocatalysis - Google Patents
Reaction device for preparing hydrogen through solar photocatalysis Download PDFInfo
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- CN103861542A CN103861542A CN201210556202.5A CN201210556202A CN103861542A CN 103861542 A CN103861542 A CN 103861542A CN 201210556202 A CN201210556202 A CN 201210556202A CN 103861542 A CN103861542 A CN 103861542A
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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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
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Abstract
The invention discloses a novel reaction device for preparing hydrogen through solar photocatalysis. A light source adopts sunshine gathered by a shaft type sun focuser; the shaft type sun focuser mainly comprises a linear paraboloid condenser and an automatic sun tracking system or only consists of a linear paraboloid condenser; a snake-shaped coil pipe type reactor is arranged at a center light spot of the linear paraboloid condenser; a circulating water cooling device is additionally arranged around the snake-shaped coil pipe type reactor. Under the action of the condensed sunshine, reaction liquid fully mixed with a catalyst is subjected to photocatalysis reaction in the snake-shaped coil pipe type reactor; generated hydrogen is finally subjected to detection and collection after being subjected to gas-liquid separation and being purified by a filter. The reaction system realizes full mixing of the catalyst and the reaction liquid on the premise of utilizing sunshine to the greatest extent and has the advantages of reasonable manufacturing cost, high reaction rate, convenience in operation and stable running.
Description
Technical field
The invention belongs to regenerative resource scale preparation field, relate to photochemical catalyzing under a kind of direct solar illuminating with pollutant and reforming biomass hydrogen preparation, hydrogen cleaning, separate and gathering-device particularly a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing.
Background technology
Hydrogen has clean, efficient with it, high heating value, eco-friendly feature, become the most promising new forms of energy of 21 century.Although Hydrogen Energy also has the long period apart from extensive use, significant for solving the energy problem facing in human kind sustainable development to its research and development.Convert solar energy into Hydrogen Energy and can form a kind of eucyclic energy system.Scientist has depicted a kind of desirable Hydrogen Energy system: utilize decomposing water with solar energy, then by fuel cell by produce H
2and O
2carry out electrochemical reaction, produce electric energy; Product water can be used as again the raw material of solar hydrogen making.Whole system has realized perfect circulation, and to environment without any pollution.The key issue of restriction solar energy photocatalytic hydrogen manufacturing is at present, the development of efficient, feasible light-catalyzed reaction system and exploitation.The development that light-catalyzed reaction system is put and the difficult point of exploitation have two: the one, and advanced Salar light-gathering technology; The 2nd, efficient photo catalysis reactor.Solar energy is inexhaustible, is desirable clean energy resource, but its energy density is low, dispersion and the drawbacks limit such as unstable it is carried out to scale utilization.Solar-energy light collector, especially, with the appearance of the solar condensing device of High Precision Automatic tracking sun function, makes the efficient utilization of solar energy become possibility.On this basis, if can develop the novel photocatalysis reactor that is different from traditional tubular type photo catalysis reactor, the easily shortcoming such as sedimentation in reactant liquor of the insufficient and catalyst of sunshine after the utilization that overcomes traditional tubular type photo catalysis reactor focuses on, will increase substantially the efficiency of solar energy photocatalytic hydrogen manufacturing.
With the solar condensing device of High Precision Automatic tracking sun function, because thereby the function with the real-time tracking sun can maximally utilise solar energy, successfully be applied in field of solar thermal power generation by domestic and international many families, in Europe with domesticly have a large-scale demonstration plant.At present at home and abroad, the example solar condensing device with High Precision Automatic tracking sun function and photocatalysis hydrogen production being coupled yet there are no formal report.On the other hand, novel photocatalysis reactor has obtained sufficient employing in photocatalysis to degrade organic matter technology, and the still traditional tubular type photo catalysis reactor mainly adopting at present in photochemical catalyzing and pollutant hydrogen producing technology.This tubular reactor has following shortcoming: (1), due to the restriction of external surface area, traditional tubular type photo catalysis reactor light-receiving area is limited, has greatly limited the utilization to focusing on rear sunshine; (2) structure of traditional tubular type photo catalysis reactor is relatively simple, be easy to cause photochemical catalyst to settle down from reactant liquor, not only seriously affect the efficiency of photocatalysis hydrogen production, and had influence on widely the stability of light-catalyzed reaction owing to resulting in blockage.
Retrieving and consult the relevant data such as document and patent finds, there are at present much reports about photochemical catalyzing and pollutant and reforming biomass hydrogen preparation reaction, but these systems are due to the restriction of the conditions such as experimental provision, the simple solar condensing device of general employing, and do not adopt the solar condensing device with High Precision Automatic tracking sun function, can not fully and efficiently utilize solar energy.In photocatalysis field, the application of novel photocatalysis reactor is mainly confined in the reaction of photocatalysis to degrade organic matter pollutant, and utilizes the informal report of experiment of novel photocatalysis reactor reaction decomposition water and pollutant and reforming biomass hydrogen preparation.
Bibliography: CN101033058A2007.9.12; CN100515924C2009.7.22; CN101973519A2011.2.16; CN102151534A2011.8.17; KR20110066335A2011.6.17; JP10218601A1998.8.18.
Summary of the invention
The invention discloses a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing.Utilize this covering device can directly, efficiently and stably realize continuous solar photochemical catalyst decomposition water and pollutant and reforming biomass hydrogen preparation, and can realize separation, purification, detection and the collection to generated gas.
Technical scheme of the present invention is achieved in that
The charging aperture of the fluid reservoir of institute of the present invention development device is connected with feed pump, and its top has charge door; First fluid reservoir top exit is connected with filter, connects successively subsequently gas chromatograph, flowmeter and gas bottle; Fluid reservoir outlet at bottom connects circulating pump, circulating pump is connected to one end of photo catalysis reactor, and the other end of photo catalysis reactor is connected to the top of fluid reservoir; On liquid storage tank skin, be respectively equipped with temp probe and precision pressure gauge; And be connected with nitrogen cylinder at the outlet at bottom place of fluid reservoir.
Photo catalysis reactor is mainly made up of shaft type solar focusing device and serpentine coil formula reactor two parts: shaft type solar focusing device is formed (or being only made up of Linear Parabolic face concentrator) by Linear Parabolic face concentrator and auto sun-tracking system, and serpentine coil formula reactor is placed on the position, center spot place at linear parabola focalizer.The sunshine temperature focusing on due to shaft type solar focusing device is higher, in order not affect the carrying out of light-catalyzed reaction, around serpentine coil formula reactor, adds cooling circulating water.After multiple photo catalysis reactors are arranged side by side together, can connect successively by pvc pipe import and the outlet of each serpentine coil formula reactor string, so just arbitrarily increase and decrease the quantity of photo catalysis reactor according to designing requirement.In addition, utilize pvc pipe to connect successively import 20 and the outlet 21 of many cover cooling circulating waters, just can realize many cover photo catalysis reactors and share a set of recirculated cooling water device.
Serpentine coil formula reactor is made up of quartz or pyrex Pyrex glass.
The middle part of fluid reservoir is cylindrical, and top and bottom are circular arc.
Tool of the present invention has the following advantages:
1, because fluid reservoir of the present invention top has charge door, can be used for adding catalyst in reaction system; In addition,, in order to ensure fully to mix between the reactant liquor in added catalyst and fluid reservoir, fluid reservoir top is with direct current generator and paddle;
2, because fluid reservoir top exit of the present invention passes through filter at first, successively connect gas chromatograph, gas flowmeter and gas bottle thereafter, can utilize like this filter to take off hydrogen sulfide and the steam of carrying secretly in product hydrogen, thereby avoid above-mentioned sour gas to gas chromatograph, flowmeter and be collected in the corrosiveness of gas bottle;
3, the shaft type solar focusing device that the present invention adopts is mainly formed (or being only made up of Linear Parabolic face concentrator) by Linear Parabolic face concentrator and auto sun-tracking system.Because shaft type solar focusing device has adopted auto sun-tracking system, so just can the real-time tracking sun, improve light-catalyzed reaction efficiency thereby maximally utilise sunshine;
4, the chief component of photo catalysis reactor that the present invention adopts is serpentine coil formula reactor, when reactant liquor and catalyst stream are during through serpentine coil formula reactor, under the solar energy effect focusing on, realizes hydrogen production by water decomposition at shaft type solar focusing device.Because serpentine coil formula reactor is to be processed by elongated glass tube dish system, its less glass tube caliber and bending structure of spiraling, can ensure well that catalyst mixes fully with reactant liquor, and do not occur that catalyst separates from reactant liquor, the phenomenon of sedimentation, greatly improve the stability of reaction.In addition, this serpentine coil formula reactor is compared with traditional tubular reactor, and surface area can increase by 3 to 5 times, so just can further increase light-catalysed reaction efficiency by the illuminating area that has improved reactor;
5, the present invention is adding cooling circulating water device around serpentine coil formula reactor.The sunshine temperature focusing on due to shaft type solar focusing device is higher, in order not affect the carrying out of light-catalyzed reaction, around serpentine coil formula reactor, install cooling circulating water device additional, so just a large amount of heats can be taken away, thereby guarantee light-catalyzed reaction can be carried out under suitable reaction temperature.Meanwhile, cooling circulating water device, also with sewage draining exit, can regularly be discharged the dirt in cooling circulating water device thus.In addition, utilize pvc pipe to connect successively import and the outlet of many cover cooling circulating waters, just can realize many cover photo catalysis reactors and share a set of recirculated cooling water device.
This reaction system is utilizing under the prerequisite of sunshine to greatest extent, can realize again the abundant mixing of catalyst and reactant liquor, there is cost reasonable, reaction rate is high, easy to operate and stable advantage, the present invention is not only applicable to photochemical catalyzing and pollutant and reforming biomass hydrogen preparation reaction, is applicable to photocatalysis degradation organic contaminant and photo catalytic reduction CO yet
2in field.
Brief description of the drawings
Fig. 1 is total schematic diagram of a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing of the present invention;
Fig. 2 is the schematic diagram of the photo catalysis reactor of a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing of the present invention.
Below in conjunction with accompanying drawing, technology contents of the present invention is described in further detail:
Detailed description of the invention
As shown in Figure 1, be connected with feed pump 7 with the charging aperture of the fluid reservoir 3 of direct current generator 12 and paddle 13; Fluid reservoir 3 top exits pass through filter 15 at first, connect successively thereafter gas chromatograph 4, gas flowmeter 5 and gas bottle 6; Fluid reservoir 3 outlet at bottoms connect circulating pump 8, circulating pump 8 are connected to one end of photo catalysis reactor 1, and the other end of photo catalysis reactor 1 is connected to fluid reservoir 3; Fluid reservoir 3 walls are provided with temp probe 10 and precision pressure gauge 11.Above-mentioned parts are connected with silicone tube by vacuum glass valve, pvc pipe 14, reactive moieties, cyclic part, monitoring part and reinforced and the output section of constituent apparatus.
Reactive moieties: formed by photo catalysis reactor 1, light-catalyzed reaction is carried out in serpentine coil formula reactor 17, when reactant liquor and catalyst stream are during through serpentine coil formula reactor 17, under the sunshine effect focusing at shaft type solar focusing device 2, realize hydrogen production by water decomposition.Shaft type solar focusing device 2 forms (or being only made up of Linear Parabolic face concentrator) by Linear Parabolic face concentrator and auto sun-tracking system two parts.Serpentine coil formula reactor 17 adopts the good quartz of light transmission or pyrex (Pyrex) glass to be made.
Cyclic part: under the drive of circulating pump 8, be mixed with the hydrogen producing in the reaction solution of catalyst and course of reaction flows in the sealing and circulating loop being made up of serpentine coil formula reactor 17, pvc pipe 14, vacuum glass valve, circulating pump 8 and fluid reservoir 3, product hydrogen in fluid reservoir 3 because of after Action of Gravity Field natural separation, take off through filter 15 hydrogen sulfide and the steam in product hydrogen, carried secretly at first, and then be collected in gas bottle 6 through flowmeter 5.
Monitoring part: formed by temp probe 10, precision pressure gauge 11 and flowmeter 5 and gas-chromatography 4, can Real-Time Monitoring closed circuit in temperature, the pressure of reaction system and the output of hydrogen of reaction solution.
Feed in raw material and output section: formed by the charge door 16 on the fluid reservoir 3 with direct current generator 12 and paddle 13, feed pump 7, fluid reservoir 3, filter 15 and gas bottle 6.Before reacting, add after reactant liquor to fluid reservoir 3 by feed pump 7, in fluid reservoir 3, add required catalyst by charge door 16, under the effect of direct current generator 12 and paddle 13, catalyst and reactant liquor are fully mixed.On the other hand, the hydrogen generating in course of reaction, takes off through filter 15 hydrogen sulfide and the steam in product hydrogen, carried secretly at first, and then is collected in gas bottle 6 through flowmeter 5.
Fig. 2 is the schematic diagram of the photo catalysis reactor of a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing of the present invention.Shaft type solar focusing device 2 is mainly formed (or being only made up of Linear Parabolic face concentrator) by Linear Parabolic face concentrator and auto sun-tracking system, is provided with serpentine coil formula reactor 17 at the center spot place of linear parabola focalizer.The sunshine temperature focusing on due to shaft type solar focusing device is higher, in order not affect the carrying out of light-catalyzed reaction, around serpentine coil formula reactor 17, adds cooling circulating water device.Cooling circulating water device adds sewage draining exit 22, can regularly dirt in cooling-cycle device be discharged thus.After arranged together multiple photo catalysis reactors, each serpentine coil formula reactor 17 connects charging aperture 18 and outlet 19 successively by pvc pipe 14, forms the closed circuit of a sealing.Meanwhile, utilize pvc pipe 14 to connect successively import 20 and the outlet 21 of serpentine coil formula reactor 17 cooling circulating water device around, many like this cover photo catalysis reactors can use a set of recirculated cooling water device.
The reactant liquor preparing is inputted in fluid reservoir 3 through the charging aperture on tank skin by feed pump 7, drops into required catalyst subsequently by charge door 16, under the effect of direct current generator 12 and paddle 13, catalyst and reactant liquor is fully mixed; Open nitrogen cylinder 9, to passing into a large amount of nitrogen in whole system to discharge air wherein, avoid a large amount of air react with the hydrogen generating and affect safety, also can prevent that catalyst is oxidized simultaneously and affect catalytic activity; ON cycle pump 8 makes the reactant liquor that is fully mixed with catalyst be circulated to serpentine coil reactor 17 through the outlet at bottom of fluid reservoir 3, and light-catalyzed reaction occurs therein; Product gas enters fluid reservoir 3 together with being mixed with the reactant liquor of catalyst, wherein product gas is discharged by fluid reservoir 3 top exits, first take off through filter 15 hydrogen sulfide and the steam in product hydrogen, carried secretly, then after being detected by gas chromatograph 4, flow through flowmeter 5 again and be collected in gas bottle 6, the reactant liquor that is mixed with catalyst is again circulated and is participated in reaction by the outlet at bottom of fluid reservoir 3.
Embodiment 1: the parameter that sets the High Precision Automatic tracking solar system on shaft type solar focusing device, make it can the real-time tracking sun, the width of the Linear Parabolic face concentrator on shaft type solar focusing device is 0.5 meter, and length is 4 meters, and the width of its focal beam spot producing is 0.10m.Serpentine coil formula reactor adopts thin glass tube totally 50 meters of long being processed that external diameter is 0.006 meter for 0.008 meter, internal diameter, and the external diameter of serpentine coil formula reactor is that 0.08 meter, length are 4 meters.In system, adding catalyst CdS concentration is 1.0g/L, and reaction solution is deionized water, and cumulative volume is 12L.Reactant liquor cycle rate is 60.2mL/min, at direct solar radiation amount average out to 480W/m
2condition under, this covering device can be realized continous-stable and produce hydrogen, average hydrogen-producing speed is 0.66L/h.
Embodiment 2: the parameter that sets the High Precision Automatic tracking solar system on shaft type solar focusing device, make it can the real-time tracking sun, the width of the Linear Parabolic face concentrator on shaft type solar focusing device is 0.5 meter, and length is 4 meters, and the width of its focal beam spot producing is 0.10m.Serpentine coil formula reactor adopts thin glass tube totally 50 meters of long being processed that external diameter is 0.006 meter for 0.008 meter, internal diameter, and the external diameter of serpentine coil formula reactor is that 0.08 meter, length are 4 meters.In system, adding catalyst CdS concentration is 1.0g/L, and reaction solution is Na
2s and Na
2sO
3mixed solution, concentration is 0.5mol/L, cumulative volume is 12L.Reactant liquor cycle rate is 60.2mL/min, at direct solar radiation amount average out to 480W/m
2condition under, this covering device can be realized continous-stable and produce hydrogen, average hydrogen-producing speed is 2.4L/h.
Embodiment 3: the parameter that sets the High Precision Automatic tracking solar system on shaft type solar focusing device, make it can the real-time tracking sun, the width of the Linear Parabolic face concentrator on shaft type solar focusing device is 0.5 meter, and length is 4 meters, and the width of its focal beam spot producing is 0.10m.Serpentine coil formula reactor adopts thin glass tube totally 50 meters of long being processed that external diameter is 0.006 meter for 0.008 meter, internal diameter, and the external diameter of serpentine coil formula reactor is that 0.08 meter, length are 4 meters.In system, adding catalyst P 25 concentration is 2.0g/L, and reaction solution is methanol solution, and concentration is 5.0mol/L, and cumulative volume is 12L.Reactant liquor cycle rate is 60.2mL/min, at direct solar radiation amount average out to 480W/m
2condition under, this covering device can be realized continous-stable and produce hydrogen, average hydrogen-producing speed is 2.2L/h.
Claims (8)
1. one kind is utilized the reaction unit of solar energy photocatalytic hydrogen manufacturing, it is characterized in that: this device mainly comprises shaft type solar focusing device (2) and photo catalysis reactor (1), and photo catalysis reactor (1) is placed in the center spot place of the solar light focusing of shaft type solar focusing device (2).
2. according to photo catalysis reactor claimed in claim 1 (1), it is characterized in that:
The chief component of this photo catalysis reactor (1) is serpentine coil formula reactor (17), it is processed by quartz ampoule or Pyrex glass pipe dish system elongated, printing opacity, and one end of serpentine coil formula reactor (17) is provided with charging aperture (18), the other end is provided with outlet (19); This serpentine coil formula reactor (17) is placed in a cool cycles water receptacle printing opacity, airtight, this cool cycles water receptacle is provided with cool cycles water inlet (20) and outlet (21), and being provided with sewage draining exit (22) thereon, this cool cycles water receptacle is made up of quartz or the Pyrex glass of printing opacity.
3. according to shaft type solar focusing device claimed in claim 1 (2), it is characterized in that: this shaft type solar focusing device (2) is by Linear Parabolic face concentrator and auto sun-tracking system forms or be only made up of Linear Parabolic face concentrator.
4. according to a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing claimed in claim 1, it is characterized in that:
The outlet (19) of the serpentine coil formula reactor (17) in the photo catalysis reactor (1) of this reaction unit is connected with fluid reservoir (3), and the charging aperture (18) of serpentine coil formula reactor (17) is connected with the material outlet of fluid reservoir (3) bottom through circulating pump (8); On the connecting line between charging aperture (18) and the fluid reservoir (3) of serpentine coil formula reactor (17), be provided with nitrogen inlet, nitrogen inlet is connected with nitrogen cylinder (9);
Reactant liquor storage tank is connected with fluid reservoir (3) through feed pump (7);
Fluid reservoir (3) is provided with charge door (16), is provided with stirring arm (13) in fluid reservoir (3), and stirring arm (13) is in transmission connection with direct current generator (12);
Fluid reservoir (3) top is provided with gas vent, and gas vent is connected with gas bottle (6) through pneumatic filter (15).
5. according to a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing claimed in claim 4, it is characterized in that:
The fluid reservoir (3) of this reaction unit is provided with temp probe (10), and fluid reservoir (3) top is provided with Pressure gauge (11).
6. according to a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing claimed in claim 4, it is characterized in that:
The connecting line of this reaction unit between pneumatic filter (15) and gas bottle (6) is provided with sample collection mouth and the gas flowmeter (5) of gas chromatograph, and the sample collection mouth of gas chromatograph is connected with the injection port of gas chromatograph (4).
7. according to a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing claimed in claim 4, it is characterized in that:
The cool cycles water inlet (20) of the cool cycles water receptacle of this reaction unit is connected with cool cycles water storage tank respectively with outlet (21), is provided with water circulating pump in the connecting line of cool cycles water receptacle and cool cycles water storage tank.
8. according to a kind of novel reaction device that utilizes solar energy photocatalytic hydrogen manufacturing claimed in claim 4, it is characterized in that:
The photo catalysis reactor of this reaction unit can be more than two or two, after more than two or two photo catalysis reactor (1) order is arranged, the charging aperture (18) of each serpentine coil formula reactor (17) and outlet (19) are connected in series successively by pvc pipe (14), the outlet (19) of the charging aperture (18) of the serpentine coil formula reactor (17) of first photo catalysis reactor (1) and the serpentine coil formula reactor (17) of the last photo catalysis reactor (1) is connected with fluid reservoir (3), forms the Matter Transfer loop of a sealing;
Simultaneously, utilize pvc pipe (14) connect successively cool cycles water receptacle cool cycles water inlet (20) and outlet (21), the outlet (21) of the import (20) of the cool cycles water receptacle of first photo catalysis reactor (1) and the cool cycles water receptacle of the last photo catalysis reactor (1) is connected with cool cycles water storage tank respectively, is provided with water circulating pump in the connecting line of cool cycles water receptacle and cool cycles water storage tank.
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| CN110697654A (en) * | 2019-11-07 | 2020-01-17 | 西安交通大学 | Continuous flow snake-shaped microchannel light-gathering photo-thermal coupling catalytic hydrogen production reaction device |
| CN111545149B (en) * | 2020-04-27 | 2021-07-13 | 西安交通大学 | High-concentration system for photocatalytic water decomposition reaction and using method thereof |
| CN111545149A (en) * | 2020-04-27 | 2020-08-18 | 西安交通大学 | High-concentration system for photocatalytic water decomposition reaction and using method thereof |
| CN112934146A (en) * | 2021-02-09 | 2021-06-11 | 江南大学 | Optical drive photocatalytic reactor and preparation method thereof |
| WO2022213145A1 (en) * | 2021-04-06 | 2022-10-13 | The University Of Adelaide | Photocatalytic apparatus |
| CN114214080A (en) * | 2021-12-20 | 2022-03-22 | 中国矿业大学 | Biomass conversion device based on solar energy |
| CN114904475A (en) * | 2022-05-27 | 2022-08-16 | 东北电力大学 | Vortex sample injection photocatalytic water decomposition hydrogen production device and turbine type sample injection method |
| CN114904475B (en) * | 2022-05-27 | 2023-07-21 | 东北电力大学 | Vortex sample injection photocatalytic water splitting hydrogen production device and turbine sample injection method |
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Application publication date: 20140618 |