US20130118059A1 - Process for conversion of a cellulosic material - Google Patents

Process for conversion of a cellulosic material Download PDF

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Publication number
US20130118059A1
US20130118059A1 US13/677,124 US201213677124A US2013118059A1 US 20130118059 A1 US20130118059 A1 US 20130118059A1 US 201213677124 A US201213677124 A US 201213677124A US 2013118059 A1 US2013118059 A1 US 2013118059A1
Authority
US
United States
Prior art keywords
equal
product
catalyst
catalytic cracking
organic solvent
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Abandoned
Application number
US13/677,124
Other languages
English (en)
Inventor
Jean Paul Lange
Colin John Schaverien
Nicolaas Wilhelmus Joseph WAY
Johan Willem Gosselink
John William Harris
Andries Quirin Maria BOON
Andries Hendrik Janssen
Leticia ESPINOSA ALONSO
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Shell USA Inc
Original Assignee
Shell Oil Co
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Shell Oil Co filed Critical Shell Oil Co
Publication of US20130118059A1 publication Critical patent/US20130118059A1/en
Assigned to SHELL OIL COMPANY reassignment SHELL OIL COMPANY ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: HARRIS, JOHN WILLIAM, BOON, ANDRIES QUIRIN MARIA, SCHAVERIEN, COLIN JOHN, ESPINOSA ALONSO, Leticia, GOSSELINK, JOHAN WILLEM, WAY, NICOLAAS WILHELMUS JOSEPH, JANSSEN, ANDRIES HENDRIK, LANGE, JEAN-PAUL
Abandoned legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
    • C10G1/006—Combinations of processes provided in groups C10G1/02 - C10G1/08
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/02—Liquid carbonaceous fuels essentially based on components consisting of carbon, hydrogen, and oxygen only
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
    • C10G1/002—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal in combination with oil conversion- or refining processes
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
    • C10G1/04—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal by extraction
    • C10G1/042—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal by extraction by the use of hydrogen-donor solvents
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/14—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts
    • C10G11/18—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts according to the "fluidised-bed" technique
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G3/00—Production of liquid hydrocarbon mixtures from oxygen-containing organic materials, e.g. fatty oils, fatty acids
    • C10G3/50—Production of liquid hydrocarbon mixtures from oxygen-containing organic materials, e.g. fatty oils, fatty acids in the presence of hydrogen, hydrogen donors or hydrogen generating compounds
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P30/00—Technologies relating to oil refining and petrochemical industry
    • Y02P30/20—Technologies relating to oil refining and petrochemical industry using bio-feedstock

Definitions

  • the organic solvent may preferably comprise one or more non-polar hydrocarbon compounds(s), which one or more non-polar hydrocarbon compound(s) preferably is/are a hydrocarbon compound having a polarity of log P in the range from +5 to +10, more preferably in the range from +7 to +8.
  • the catalyst is an acid catalyst.
  • the acid catalyst for use in liquefaction step to the invention may be any acid catalyst known in the art to be suitable for liquefying of cellulosic material.
  • the acid catalyst may be a Brönsted acid or a Lewis acid.
  • the acid catalyst may be a homogeneous catalyst or a heterogeneous catalyst.
  • the acid catalyst is a homogeneous or finely dispersed heterogeneous catalyst, most preferably the acid catalyst is a homogeneous catalyst.
  • the acid catalyst remains liquid and stable under the liquefaction conditions and preferably it is sufficiently strong to effect cleavage of the covalent linkages and dehydration of the cellulosic material.
  • the liquefaction process according to the invention can be carried out batch-wise, semi-batch wise and continuously.
  • the liquefied product(s) may comprise monomeric and/or oligomeric compounds and optionally excess water produced during the liquefaction process. From the liquefied product a product containing monomeric and oligomeric compounds may be separated. Also part of the liquefied product may be separated for recycling to the liquefaction step as organic solvent.
  • the co-solvent is an organic co-solvent such as a petroleum oil or a fraction of a petroleum oil
  • the liquefaction step comprises hydrogenating of the one or more liquefied products
  • the petroleum oil or a fraction of the petroleum oil may suitably also be hydrogenated. This may be advantageous during the catalytic cracking step.
  • a mixture of the liquefied product(s) and a first hydrocarbon co-feed (which may for example be the organic solvent when the organic solvent is chosen from the described fluid hydrocarbon co-feeds) is supplied to a riser reactor at a first location and a second fluid hydrocarbon co-feed is supplied to the riser reactor at a second location downstream of the first location.
  • a first hydrocarbon co-feed which may for example be the organic solvent when the organic solvent is chosen from the described fluid hydrocarbon co-feeds
  • the internal riser reactor is an essentially vertical essentially tube-shaped reactor, that may have an essentially vertical upstream end located outside a vessel and an essentially vertical downstream end located inside the vessel.
  • the vessel is suitably a reaction vessel suitable for catalytic cracking reactions and/or a vessel that comprises one or more cyclone separators and/or swirl tubes.
  • the internal riser reactor may be especially advantageous in the catalytic cracking step as it may be less prone to plugging, thereby increasing safety and hardware integrity.
  • the one or more product fractions and/or the one or more hydrotreated product fractions and/or any fractions derived therefrom can conveniently be used as a biofuel component.
  • a biofuel component may conveniently be blended with one or more other components to produce a biofuel.
  • examples of such one or more other components include anti-oxidants, corrosion inhibitors, ashless detergents, dehazers, dyes, lubricity improvers and/or mineral fuel components, but also conventional petroleum derived gasoline, diesel and/or kerosene fractions.
  • the first and second total product were combined.
  • methyl-tetrahydrofuran m-THF, 400 grams
  • the mixture of methyl-tetrahydrofuran and total products was stirred for 10 minutes at room temperature (20° C.) and subsequently filtered over a P3 glass filter to produce a filtrate and a filter cake.
  • the feed mixture of final liquefied product and fluid hydrocarbon co-feed When compared with a feed consisting of 100 wt % fluid hydrocarbon co-feed, the feed mixture of final liquefied product and fluid hydrocarbon co-feed is more reactive.
  • the feed mixture of final liquefied product and fluid hydrocarbon co-feed shows a similar yield of valuable products (gasoline, light cycle oil and LPG) and a similar coke yield when compared to the reference feed.
  • Detailed results are provided in Table 1.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Wood Science & Technology (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
US13/677,124 2011-11-14 2012-11-14 Process for conversion of a cellulosic material Abandoned US20130118059A1 (en)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
EPEP11189049.7 2011-11-14
EP11189049 2011-11-14
EP12190054 2012-10-25
EPEP12190054.2 2012-10-25

Publications (1)

Publication Number Publication Date
US20130118059A1 true US20130118059A1 (en) 2013-05-16

Family

ID=47215545

Family Applications (1)

Application Number Title Priority Date Filing Date
US13/677,124 Abandoned US20130118059A1 (en) 2011-11-14 2012-11-14 Process for conversion of a cellulosic material

Country Status (8)

Country Link
US (1) US20130118059A1 (enrdf_load_stackoverflow)
EP (1) EP2780433A1 (enrdf_load_stackoverflow)
CN (1) CN104011177A (enrdf_load_stackoverflow)
AU (1) AU2012338868A1 (enrdf_load_stackoverflow)
BR (1) BR112014011506A2 (enrdf_load_stackoverflow)
CA (1) CA2855584A1 (enrdf_load_stackoverflow)
IN (1) IN2014DN03435A (enrdf_load_stackoverflow)
WO (1) WO2013072391A1 (enrdf_load_stackoverflow)

Cited By (25)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20130247449A1 (en) * 2011-11-14 2013-09-26 Shell Oil Company Process for conversion of a cellulosic material
US20140227161A1 (en) * 2013-02-11 2014-08-14 American Science And Technology Corporation System and method for extraction of chemicals from lignocellulosic materials
WO2014210150A1 (en) * 2013-06-26 2014-12-31 Ensyn Renewables, Inc. Systems and methods for renewable fuel
US9102889B2 (en) 2011-12-12 2015-08-11 Ensyn Renewables, Inc. Fluidized catalytic cracker riser quench system
US9175235B2 (en) 2012-11-15 2015-11-03 University Of Georgia Research Foundation, Inc. Torrefaction reduction of coke formation on catalysts used in esterification and cracking of biofuels from pyrolysed lignocellulosic feedstocks
WO2015172208A1 (en) * 2014-05-12 2015-11-19 Katholieke Universiteit Leuven Ku Leuven Research & Development Biphasic solvent catalytic process for the direct production of light naphtha from carbohydrate-containing feedstock.
US9347005B2 (en) 2011-09-13 2016-05-24 Ensyn Renewables, Inc. Methods and apparatuses for rapid thermal processing of carbonaceous material
US9382283B2 (en) 2014-08-01 2016-07-05 American Science And Technology Corporation Oxygen assisted organosolv process, system and method for delignification of lignocellulosic materials and lignin recovery
US9422478B2 (en) 2010-07-15 2016-08-23 Ensyn Renewables, Inc. Char-handling processes in a pyrolysis system
US9441887B2 (en) 2011-02-22 2016-09-13 Ensyn Renewables, Inc. Heat removal and recovery in biomass pyrolysis
US9670413B2 (en) 2012-06-28 2017-06-06 Ensyn Renewables, Inc. Methods and apparatuses for thermally converting biomass
US9809564B2 (en) 2006-04-03 2017-11-07 Pharmatherm Chemicals, Inc. Thermal extraction method and product
US9951278B2 (en) 2010-05-20 2018-04-24 Ensyn Renewables, Inc. Processes for controlling afterburn in a reheater and for controlling loss of entrained solid particles in combustion product flue gas
US10041667B2 (en) 2011-09-22 2018-08-07 Ensyn Renewables, Inc. Apparatuses for controlling heat for rapid thermal processing of carbonaceous material and methods for the same
US10066168B2 (en) 2010-05-12 2018-09-04 Shell Oil Company Process for liquefying a cellulosic material and its products
RU2674018C1 (ru) * 2016-11-21 2018-12-04 Бейджинг Хуаши Юнайтед Энерджи Технолоджи энд Девелопмент Ко., Лтд. Способ производства лёгкого масла путем сжижения биомассы
US10337726B2 (en) 2015-08-21 2019-07-02 Ensyn Renewables, Inc. Liquid biomass heating system
US10400175B2 (en) 2011-09-22 2019-09-03 Ensyn Renewables, Inc. Apparatuses and methods for controlling heat for rapid thermal processing of carbonaceous material
US10400176B2 (en) 2016-12-29 2019-09-03 Ensyn Renewables, Inc. Demetallization of liquid biomass
EP3575383A1 (en) * 2018-05-28 2019-12-04 Total Research & Technology Feluy Biphasic solvent catalytic process for the production of mono-oxygenated molecules from a bio-feedstock comprising carbohydrates
EP3575384A1 (en) * 2018-05-28 2019-12-04 Total Research & Technology Feluy Biphasic solvent catalytic process for the production of mono-oxygenated molecules from a bio-feedstock comprising carbohydrates and use of said mono-oxygenated molecules in a fluid catalytic cracking process
WO2020068820A1 (en) 2018-09-25 2020-04-02 Exxonmobil Research And Engineering Company Co-processing hydrothermal liquefaction oil and co-feed to produce biofuels
WO2020118134A2 (en) 2018-12-07 2020-06-11 Exxonmobil Research And Engineering Company Processes for polymerizing internal olefins and compositions thereof
WO2020205708A1 (en) 2019-04-01 2020-10-08 Exxonmobil Research And Engineering Company Processes for polymerizing alpha-olefins, internal olefins and compositions thereof
EP3741828A1 (en) * 2019-05-23 2020-11-25 Vertoro B.V. Fluid catalytic cracking process of crude lignin oil (clo)

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EP2886628A1 (en) 2013-12-18 2015-06-24 Shell International Research Maatschappij B.V. Process for washing a biologically derived feed
SE544501C2 (en) * 2020-09-18 2022-06-21 Rise Res Institutes Of Sweden Ab Process for one-step conversion of lignocellulosic material to hydrocarbon products and catalyst for use in said process
IT202200007589A1 (it) 2022-04-15 2023-10-15 Pabif Srl Processo ed apparato per la produzione di acido levulinico da cellulosa ricavata da biomasse

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US9809564B2 (en) 2006-04-03 2017-11-07 Pharmatherm Chemicals, Inc. Thermal extraction method and product
US10066168B2 (en) 2010-05-12 2018-09-04 Shell Oil Company Process for liquefying a cellulosic material and its products
US9951278B2 (en) 2010-05-20 2018-04-24 Ensyn Renewables, Inc. Processes for controlling afterburn in a reheater and for controlling loss of entrained solid particles in combustion product flue gas
US10563127B2 (en) 2010-05-20 2020-02-18 Ensyn Renewables, Inc. Processes for controlling afterburn in a reheater and for controlling loss of entrained solid particles in combustion product flue gas
US9422478B2 (en) 2010-07-15 2016-08-23 Ensyn Renewables, Inc. Char-handling processes in a pyrolysis system
US11028325B2 (en) 2011-02-22 2021-06-08 Ensyn Renewables, Inc. Heat removal and recovery in biomass pyrolysis
US9441887B2 (en) 2011-02-22 2016-09-13 Ensyn Renewables, Inc. Heat removal and recovery in biomass pyrolysis
US9347005B2 (en) 2011-09-13 2016-05-24 Ensyn Renewables, Inc. Methods and apparatuses for rapid thermal processing of carbonaceous material
US10400175B2 (en) 2011-09-22 2019-09-03 Ensyn Renewables, Inc. Apparatuses and methods for controlling heat for rapid thermal processing of carbonaceous material
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US10975315B2 (en) 2011-12-12 2021-04-13 Ensyn Renewables, Inc. Systems and methods for renewable fuel
US9422485B2 (en) 2011-12-12 2016-08-23 Ensyn Renewables, Inc. Method of trading cellulosic-renewable identification numbers
US9102888B2 (en) 2011-12-12 2015-08-11 Ensyn Renewables, Inc. Methods for renewable fuels with reduced waste streams
US9969942B2 (en) 2011-12-12 2018-05-15 Ensyn Renewables, Inc. Systems and methods for renewable fuel
US9102889B2 (en) 2011-12-12 2015-08-11 Ensyn Renewables, Inc. Fluidized catalytic cracker riser quench system
US9670413B2 (en) 2012-06-28 2017-06-06 Ensyn Renewables, Inc. Methods and apparatuses for thermally converting biomass
US9175235B2 (en) 2012-11-15 2015-11-03 University Of Georgia Research Foundation, Inc. Torrefaction reduction of coke formation on catalysts used in esterification and cracking of biofuels from pyrolysed lignocellulosic feedstocks
US10633606B2 (en) 2012-12-10 2020-04-28 Ensyn Renewables, Inc. Systems and methods for renewable fuel
US9365525B2 (en) * 2013-02-11 2016-06-14 American Science And Technology Corporation System and method for extraction of chemicals from lignocellulosic materials
US20140227161A1 (en) * 2013-02-11 2014-08-14 American Science And Technology Corporation System and method for extraction of chemicals from lignocellulosic materials
WO2014210150A1 (en) * 2013-06-26 2014-12-31 Ensyn Renewables, Inc. Systems and methods for renewable fuel
US10640719B2 (en) 2013-06-26 2020-05-05 Ensyn Renewables, Inc. Systems and methods for renewable fuel
US10407623B2 (en) 2014-05-12 2019-09-10 Katholieke Universiteit Leuven, K.U. Leuven Research & Development Biphasic solvent catalytic process for the direct production of light naphtha from carbohydrate-containing feedstock
WO2015172208A1 (en) * 2014-05-12 2015-11-19 Katholieke Universiteit Leuven Ku Leuven Research & Development Biphasic solvent catalytic process for the direct production of light naphtha from carbohydrate-containing feedstock.
US9382283B2 (en) 2014-08-01 2016-07-05 American Science And Technology Corporation Oxygen assisted organosolv process, system and method for delignification of lignocellulosic materials and lignin recovery
US10948179B2 (en) 2015-08-21 2021-03-16 Ensyn Renewables, Inc. Liquid biomass heating system
US10337726B2 (en) 2015-08-21 2019-07-02 Ensyn Renewables, Inc. Liquid biomass heating system
RU2674018C1 (ru) * 2016-11-21 2018-12-04 Бейджинг Хуаши Юнайтед Энерджи Технолоджи энд Девелопмент Ко., Лтд. Способ производства лёгкого масла путем сжижения биомассы
US10982152B2 (en) 2016-12-29 2021-04-20 Ensyn Renewables, Inc. Demetallization of liquid biomass
US10400176B2 (en) 2016-12-29 2019-09-03 Ensyn Renewables, Inc. Demetallization of liquid biomass
EP3575383A1 (en) * 2018-05-28 2019-12-04 Total Research & Technology Feluy Biphasic solvent catalytic process for the production of mono-oxygenated molecules from a bio-feedstock comprising carbohydrates
EP3575384A1 (en) * 2018-05-28 2019-12-04 Total Research & Technology Feluy Biphasic solvent catalytic process for the production of mono-oxygenated molecules from a bio-feedstock comprising carbohydrates and use of said mono-oxygenated molecules in a fluid catalytic cracking process
WO2020068820A1 (en) 2018-09-25 2020-04-02 Exxonmobil Research And Engineering Company Co-processing hydrothermal liquefaction oil and co-feed to produce biofuels
WO2020118134A2 (en) 2018-12-07 2020-06-11 Exxonmobil Research And Engineering Company Processes for polymerizing internal olefins and compositions thereof
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CN104011177A (zh) 2014-08-27
BR112014011506A2 (pt) 2017-05-09

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