WO2009103548A2 - Method for treating exhaust gas streams during the processing of biogenic gas streams - Google Patents

Method for treating exhaust gas streams during the processing of biogenic gas streams Download PDF

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Publication number
WO2009103548A2
WO2009103548A2 PCT/EP2009/001226 EP2009001226W WO2009103548A2 WO 2009103548 A2 WO2009103548 A2 WO 2009103548A2 EP 2009001226 W EP2009001226 W EP 2009001226W WO 2009103548 A2 WO2009103548 A2 WO 2009103548A2
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Prior art keywords
catalyst
biogas
characterized
exhaust gas
exhaust
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PCT/EP2009/001226
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German (de)
French (fr)
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WO2009103548A3 (en )
Inventor
Hans-Christoph Schwarzer
Hans-Georg Anfang
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Süd-Chemie AG
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    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10LFUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/10Working-up natural gas or synthetic natural gas
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10LFUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00Technologies for the production of fuel of non-fossil origin
    • Y02E50/30Fuel from waste
    • Y02E50/34Methane
    • Y02E50/343Methane production by fermentation of organic by-products, e.g. sludge

Abstract

The invention relates to a method for producing biogas from crude biogas, wherein an exhaust gas stream occurring during the processing of crude biogas is treated using a catalyst. Furthermore, the invention relates to the use of a catalyst for treating an exhaust gas stream occurring during the production of biogas.

Description

A process for treating exhaust streams in the workup of biogenic gas streams

The invention relates to a process for producing biogas from crude gas, wherein a is treated in the processing of raw biogas applicable exhaust stream with a catalyst. The invention further relates to the use of a catalyst for the treatment of a obtained in the production of biogas exhaust stream.

Biogas is a mixture of the main components methane and carbon dioxide and formed during the anaerobic fermentation of organic material. In contrast to the aerobic composting process is the absence of air. The fermentation process takes place in nature for. B. place in the rumen of cattle, in bog or marsh areas or in rice fields.

Table 1 shows a typical composition of biogas.

Table 1: Typical Composition of biogas

Figure imgf000003_0001
The industrial production of biogas is realized in particular biogas plants. Typical starting materials for this are,. B. manure (z. B. slurry) and energy crops (renewable resource). The technical basis for the production and use of biogas are repeatedly described in the literature and prior art. Good reviews are for. (:; 978-3922964599: 3922964591 ISBN-13 ISBN-10 Ökσbuch publisher) to find as in the book "Biogas Practice" by Heinz Schulz.

In principle, there are various energy and chemical use and exploit ways of biogas. The oldest and simplest Nutzungsweg is the direct combustion to generate heat.

The current technical main use is the motorized conversion into electricity and heat. In this case, an internal combustion engine is fed with biogas and operated with the generated kinetic energy of a generator for power generation. The combustion process obtained in the comparison waste heat is the one hand fed back to the fermentation process as a necessary process heat for the fermentation and / or used in cogeneration / CHP systems.

Current main purpose of a biogas plant, is the generation of electricity and the supply to the public network. Biogas power can be different than electricity from wind and solar plants permanently fed into a power grid and thus cover basic loads in the power supply.

Further possibilities for use of biogas are for. B. the energy generation in fuel cells (z. B. MCFC systems, "CFC-solutions") and the production of synthesis gas with DA up following synthesis steps such as. For example, a methanol synthesis or Fischer-Tropsch synthesis.

A frequently discussed in recent times use path is biogas upgrading to natural gas. The thus produced "Bicmethan" ( "Bioerdgas") may be locally connected or supplied and used in the natural gas grid. According to German Biogas Association. V. could in future be covered in Germany alone, up to 20% of natural gas consumption on biomethane. So that the gas can be easily fed into a natural gas network, in addition to CO 2 other accompanying substances also have to be removed permanently. The quality requirements for the production of natural gas are substitut in the DVGW G260, set 261 and 262nd

All use paths of biogas require a different intensive treatment (gas purification) of the raw biogas for subsequent use. The gas can be purified for example by the removal of the unwanted components. Several methods can be combined. Often at least a separation method for gas processing is required. This can basically be realized by the following methods [DGMK Conference Report 2002-2; ISBN 3-931850-91-9, pp 37-44, Schulte-Schulze Berndt]:

-Druckwasserwäsche

-Aminwäsche (depressurized and pressure-operated) -Membranverfahren

-kombiniertes membrane washing method -CO 2 liquefaction adsorption process

-Druckwechseladsorption over activated carbon and / or carbon molecular sieve A detailed description of methods for the treatment of raw biogas to Bioerdgas as well as the possible use of exhaust gas streams can be found in EP 1634946 Al ( "environmentally friendly process for obtaining natural biogas").

Each separation method has various advantages and disadvantages. Allen separation method, however, is inherent in that after separation of the biogas containing main gas stream containing a high methane gas content - that is higher than the Riobiogas - (depending on the selectivity of the separation process), a remaining gas flow is obtained, the so-called exhaust gas stream or partial gas stream containing methane in lesser includes concentration and can contain other hydrocarbons, CO, H 2, NH 3, NO x and O 2.

A typical process route for the production of biogas from crude biogas is shown in the diagram in Figure 1, also the occurrence of an exhaust gas stream (partial gas stream) is illustrated.

Often these partial gas streams enter (see Figure 1) as an exhaust gas into the atmosphere. Because components Non- controlling this gas stream to health and umweitschädlich (eg methane is one of the greenhouse gases and is a factor of 21 more damaging than CO 2 rated), the untreated discharge into the environment should be avoided.

In addition, the exhaust flow through the components included a calorific value that would not be used in direct release into the environment.

In EP 1634946 Al is described, for example, such as the methane content can be varied in this exhaust gas flow through a modification of the separation process. The aim is to adjust the exhaust gas stream in its composition that a combustible composition is produced which can be used thermally (by burning), for example for the production of raw biogas (z. B. for the heating of a fermenter). This umweitschädiiches methane is less discharged from the exhaust stream as exhaust gas into the environment. A disadvantage of this method, however, is that caused by the combustion of the exhaust gas stream of sulfur oxides and nitrogen oxides, which will continue to be discharged to the environment.

The object of the present invention is thus to provide a method in which the exhaust gas stream is freed of harmful components and also the Strom in exhaust energy contained can be used.

The object is achieved by a method for the production of biogas from crude gas, comprising the steps of

a) preparing raw biogas, b) Aufbereitens of the raw biogas by separating a biogas containing main gas stream by means of a separation process, and c) separating a resulting in the preparation of the raw biogas exhaust stream

and which is characterized in that the exhaust gas stream is treated with a catalyst.

The provision of the raw biogas can according to the known in the prior art method, for example, anaerobic fermentation in an industrial biogas plant occur.

Similarly, all known in the prior art separation processes for the preparation of the raw biogas can be used. These include the pressure water wash, the amine scrubbing (normally operated and pressure), the membrane process, a combined membrane-washing method, the CO 2 liquefaction, the adsorption or pressure swing adsorption over active carbon and / or a carbon molecular sieve. Through this process, the biogas can be effectively separated from raw biogas. What remains is a partial gas stream, commonly referred to as off-gas, which in addition to residual methane, further components such. B. contains other hydrocarbons, CO, H 2, NH 3, NO x and O 2.

According to the invention the exhaust gas stream is treated with a catalyst. This means that the exhaust stream is passed over the catalyst, whereby a reaction heat is generated which can be reused.

Preferably, the catalyst used is a talysator Oxidationska-. The catalyst may consist of one or more layers, which may be the same or different. Preferably, the oxidation catalyst is a monolithic catalyst, such as metal and ceramic honeycomb. Further preferably, the catalyst is a foam or a bulk catalyst, for example a shell catalyst, a solid material or an extrudate, wherein various geometric shapes and dimensions are possible. The catalysts may be coated with one or more layers and washcoat containing one or more noble metals and / or metal oxides and / or mixtures thereof as active components.

Usually the catalyst is so constructed that a catalytically active compound is present as a coating on a suitable carrier. Preferably, the catalytically active layers are based on aluminum, cerium, tungsten, titanium, iron, silicon and zirconium oxide, or combinations of the above, which additionally catalytically active precious metals and / or catalytically active metal oxides of Fe, Cu which may contain Mn thereof, or combinations thereof. Suitable noble metals are preferably selected from the group consisting of platinum, palladium, rhodium, copper, silver and ruthenium.

The catalytically active layer is preferably (pient INCI wetness method) in the form of a washcoat by impregnation, spraying or eye applied that contains the catalytically active substances, in particular the metals. The metals (metal) are usually applied in the form of their nitrates, chlorides, sulfates, sulfites, acetates, etc., or complex compounds of these metals. Of course, the corresponding oxides in the form of slurries can be used.

After application of the washcoat is typically carried out by a drying or calcination, followed by addition finally a metal or noble metal doping of the washcoat surface, be configured with other catalytically active metals or their compounds, such as nitrates, chlorides, sulfates, sulfites, acetates or complex compounds can.

Likewise, the oxidation catalyst is a zeolite or a zeolithähnliches material or may be a support material can be coated with the zeolite or zeolite-like material. Also preferred within the meaning of this invention is a combination of a zeolite or zeolite-like material with an oxidation catalyst, as described above.

The zeolite is preferably selected from a group of zeolites with the topologies AEL, BEA, CHA, EUO, FAO, FER, KFI, LTA, LTL, MAZ, MOR, MEL, MTW, LEV, OFF, TON and MFI.

The term "zeolite" is in the context of the present invention as defined by the International Mineralical Association (DS Coombs et al., Canadian Mineralogist, 35, 1979, 1571) a crystalline substance from the group of aluminum silicates with a spatial network structure of the general formula

M n + [(AlO 2 J x (SiO 2 Jy] XH 2 O

understood that consist 4 tetrahedra of SiO 4 / AlO, which are linked by common oxygen atoms to form a regular three dimensional network.

The ratio of Si / Al = y / x is always> 1 according to the so-called. "Loewenstein rule", prohibiting the occurrence of two neighboring adjacent negatively charged A10 4 tetrahedra. The focus is at a low Si / Al ratio, although more exchange sites for metal available, the zeolite is, however, increasingly thermally unstable.

The zeolite structure contains voids, channels, which are characteristic of each zeolite. The zeolites are classified according to their topology in various structures. The Zeo- lithgerüst includes open cavities in the form of channels and cages, which are normally occupied by water molecules and additional framework cations that can be exchanged. Of an aluminum atom an excess negative charge which is compensated by these cations. The interior of the pore system represents the catalytically active surface. The more aluminum and the less silicon contains a zeolite, the denser is the negative charge in its lattice and the more polar its inner surface. The pore size and structure is determined by parameters in the manufacture, that use or type of templates, pH, pressure, temperature, presence of seed crystals, by the Si / Al ratio that most of the catalytic character of a zeolite accounts. By the presence of divalent or trivalent cations as tetrahedral center in the zeolite, the zeolite receives a negative charge in the form of so-called. Anion sites in the vicinity thereof of the corresponding cation positions are located. The negative charge is compensated for by the inclusion of cations in the pores of the zeolite material. The zeolites, a distinction is based primarily on the geometry of the cavities, which are formed by the rigid network / SiO 4 AlO 4 tetrahedra. The inputs to the cavities are formed by 8, 10 or 12 rings, the skilled person speaks from narrow, medium and large pore zeolites. Certain zeolites exhibit a uniform structural assembly, z. For example, the ZSM-5 or MFI topology, with linear or zigzag-shaped extending passages, in other larger cavities join behind the pore openings, for example. B. in the Y or zeolite A, with the FAO topologies and LTA.

Preferably, the zeolite is a metal exchanged zeolite, more preferably an Fe-zeolite. The zeolite or the zeo- lithähnliche material may also be coated with a precious metal or doped. Suitable noble metals are also preferably selected from the group consisting of platinum, palladium, rhodium, copper, silver and ruthenium. The manufacturing method of metal-exchanged zeolites, for example the solid or liquid phase exchange, are known in the art. Likewise, the method for coating or doping of zeolites are known to those skilled in precious metals.

The present invention thus describes a combined process for the production of biogas from crude gas, which consists of a separation process and a downstream process, said to be removed from the separation process by catalytic oxidation at the downstream process harmful and environmentally hazardous components of the Abgasteil- current, and wherein the at the oxidation heat released for further use is available.

A schematic overview of the process of the invention can be seen in FIG. 2

Surprisingly, it was found that it is not necessary in the inventive process, to achieve a certain concentration of methane in the exhaust stream, since no combustible composition of the exhaust stream is required for this procedure. This means that the methane yield in the main gas flow is maximum.

Further advantages of the inventive method:

• The exhaust contains less harmful components;

• The heat can be used;

• Compared with the thermal combustion no nitrogen oxides and / or sulfur oxides are formed;

• Compared with the thermal combustion is no support - gas firing is necessary ( "flameless poor gas burner");

• There is no elaborate control requirements depending on the exhaust gas flow composition or the volume flow, which is caused by the cyclic operation of the separation process, it is necessary;

• The catalyst is used as a heat reservoir for balancing these cyclic fluctuations (minimal need for regulation).

In addition, the catalysts defined above can also be used to (for example, during the combustion in a gas engine) to clean the exhaust gas streams arising in the use of the biogas produced, and also to remove as overall sundheitsschädliche and environmentally hazardous components.

In addition, the catalysts defined above can also be used to clean the production both of the raw biogas exhaust streams (such as heating of the fermentation) and to remove as also harmful and environmentally hazardous components.

In addition, the catalysts defined above can also be used to purify the exhaust gas streams produced during the production, purification or use of a biogenic gas (for example, by gasification of organic (bio) mass) and to remove as also harmful and environmentally hazardous components.

Likewise, the scope of the invention include a biogas plant, which is suitable for carrying out the method according to the invention and at least one catalyst, as described above, comprising. Preferably, the catalyst is arranged in the exhaust line of the accumulating in the preparation of the raw biogas exhaust gas.

According to a further preferred embodiment, an additional catalyst is disposed in an exhaust system of a obtained in the fermentation bioreactor in the exhaust gas (for example, in the generation of heat for the fermentation accumulating exhaust gas or in the fermentation accumulating biogenic waste gas).

According to an even further preferred embodiment of the invention, an additional catalyst resulting in an exhaust line of an in the use of the produced biogas (combustion) the exhaust gas is arranged. For example, the methane content after natural gas or biogas operated stationary engines (for example in combined heat and power) is typically below 3000 ppm (equivalent to about 0.3 vol .-%). The oxygen content is .-% at about 8-12 vol. Order to allow sufficient definitely oxygen for the catalytic or thermal oxidation Total available. A catalyst is preferably used, which consists of a ceramic and / or metal support, which comprises a washcoat based on alumina and platinum as active component. The platinum concentration is preferably in the range of 1.0 to 1.5 g / l honeycomb volume. Thus, CO reductions in the exhaust gas of 70% can be achieved up to 90%.

The catalysts for the respective exhaust lines may be the same or different. Preferably, the catalytic converters are adapted to the respective use. For example, the catalyst that is obtained in an exhaust system of the in the use of the produced biogas (combustion) the exhaust gas preferably is high temperature stable, since the heat generated in the combustion of biogas can produce an exhaust gas with a temperature of more than 400 0 C.

Through the combination of several catalysts ensures that thermal energy for biogas production is always sufficiently available. Excess thermal energy, which is obtained by the use of one or more catalysts, for example, can be collected in hot water tanks or for other purposes (eg. For example, for electricity generation) are used.

The invention will now be described with reference to some embodiments which are not to be understood as limiting the scope of the invention in detail.

EXAMPLES Example 1:

A catalyst composition for the purification of the obtained in the production of biogas partial gas flow (exhaust gas flow):

It was used with a ceramic support, a catalyst was coated with a washcoat based on alumina with platinum and palladium as active components.

The total precious metal concentration was 3 g / l, 4 g / l and 5 g / 1 of honeycomb volume.

Example 2:

A catalyst composition for the purification of the obtained in the production of biogas partial gas flow (exhaust gas flow):

It was used with a metal support, a catalyst was coated with a washcoat based on alumina with platinum and palladium as active component.

The total precious metal concentration was 3 g / l, 4 g / l and 5 g / 1 of honeycomb volume.

Example 3:

A catalyst composition for the purification of an exhaust gas stream which is obtained in the combustion of the biogas in a stationary engine:

It was used with a ceramic carrier is a catalyst comprising a washcoat based on alumina and platinum as active component. The platinum concentration was in the range of 1.0 and 1.5 g / l honeycomb volume.

Example 4:

A catalyst composition for purifying an exhaust gas - stream which is obtained in the combustion of the biogas in a stationary engine:

It was used with a metallic carrier is a catalyst comprising a washcoat based on alumina and platinum as active component. The platinum concentration was in the range of 1.0 and 1.5 g / l honeycomb volume. Thus CO reductions in exhaust gas were achieved by 90%.

Claims

claims
1. A process for the production of biogas from crude gas, comprising the steps of
a) providing raw biogas, b) Aufbereitens of the raw biogas containing biogas by cutting off a main gas flow by means of a separation process, and c) separating a resulting in the preparation of the raw biogas exhaust gas stream, the exhaust stream contains residual methane,
characterized in that the exhaust gas stream is treated with an oxy dationskatalysator.
2. The method according to claim 1, characterized in that the exhaust gas stream also contains other hydrocarbons, CO, H 2, NH 3, NO x and O 2.
3. The method of claim 1 or 2, characterized in that the catalyst is in the form of a monolithic catalyst or as a bulk catalyst.
4. The method according to any one of claims 1 to 3, characterized in that the catalyst is coated with a washcoat.
includes 5. Method according to one of the preceding claims, characterized in that the catalyst is a noble metal and / or a metal oxide and / or a composite oxide.
6. The method according to any one of the preceding claims, characterized in that the exhaust stream after treatment is free of harmful components with the catalyst substantially.
7. The method according to any one of the preceding claims, characterized in that which is used in the treatment of the exhaust stream with a catalyst resulting thermal energy.
8. The method according to claim 7, characterized in that the thermal energy for the production of crude biogas is used.
Which contains residual methane 9. The use of a catalyst for the treatment of a obtained in the production of biogas exhaust stream with an oxidation catalyst.
10. Use according to claim 9, characterized in that the catalyst is in the form of a monolithic catalyst or as a bulk catalyst.
11. Use according to any one of claims 9 or 10, characterized in that the catalyst is coated with a washcoat.
12. Use according to any one of claims 9 to 11, characterized in that the catalyst comprises a noble metal and / or a metal oxide and / or a composite oxide.
13. Use according to any one of claims 9 to 12, characterized in that the treatment of the waste from the production of biogas exhaust gas stream comprises the reduction of harmful substances in the exhaust stream.
14. Use according to any one of claims 9 to 13, characterized in that the catalyst for treating the exhaust gas stream is part of a biogas plant.
PCT/EP2009/001226 2008-02-21 2009-02-20 Method for treating exhaust gas streams during the processing of biogenic gas streams WO2009103548A3 (en)

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DE102008010329.2 2008-02-21

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DE102010018703A1 (en) * 2010-04-29 2011-11-03 Messer Group Gmbh A method of operating an internal combustion engine and internal combustion engine

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE4142399A1 (en) * 1991-12-20 1993-06-24 Linde Ag Desulphurising bio-gas by selective catalytic oxidn. - followed by washing out the sulphur di:oxide in soda lye, is simple and ecologically compatible
DE19840691A1 (en) * 1998-08-24 2000-03-09 Wolfgang Tentscher Processing biogas and landfill gases to yield a carbon dioxide-containing by-product, useful for e.g. preservation of foodstuffs and as a blanketing/protective gas
EP1634946A1 (en) * 2004-09-13 2006-03-15 RÜTGERS CarboTech Engineering GmbH Environmentally safe process for generating biological natural gas

Family Cites Families (2)

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Publication number Priority date Publication date Assignee Title
DE10356276A1 (en) * 2003-11-28 2005-06-30 Tentscher, Wolfgang, Dr. Method for recovery of carbon dioxide from biogas comprises compressing biogas and treating product with regenerated absorption stream so that carbon dioxide and trace materials are removed to enrich absorption stream
EP1754695A1 (en) * 2005-08-17 2007-02-21 Gastreatment Services B.V. Process and apparatus for the purification of methane rich gas streams

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE4142399A1 (en) * 1991-12-20 1993-06-24 Linde Ag Desulphurising bio-gas by selective catalytic oxidn. - followed by washing out the sulphur di:oxide in soda lye, is simple and ecologically compatible
DE19840691A1 (en) * 1998-08-24 2000-03-09 Wolfgang Tentscher Processing biogas and landfill gases to yield a carbon dioxide-containing by-product, useful for e.g. preservation of foodstuffs and as a blanketing/protective gas
EP1634946A1 (en) * 2004-09-13 2006-03-15 RÜTGERS CarboTech Engineering GmbH Environmentally safe process for generating biological natural gas

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EP2250239A2 (en) 2010-11-17 application
DE102008010329A1 (en) 2009-09-03 application

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