BR112016028226B1 - Processo para preparação de um material zeolítico, material zeolítico sintético e uso de material zeolítico sintético - Google Patents

Processo para preparação de um material zeolítico, material zeolítico sintético e uso de material zeolítico sintético Download PDF

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Publication number
BR112016028226B1
BR112016028226B1 BR112016028226-4A BR112016028226A BR112016028226B1 BR 112016028226 B1 BR112016028226 B1 BR 112016028226B1 BR 112016028226 A BR112016028226 A BR 112016028226A BR 112016028226 B1 BR112016028226 B1 BR 112016028226B1
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Brazil
Prior art keywords
zeolitic material
range
present
cha
compounds
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BR112016028226-4A
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English (en)
Portuguese (pt)
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BR112016028226A2 (pt
Inventor
Mathias Feyen
Jeff Yang
Roger Ruetz
Ulrich Müller
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Basf Se
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Publication of BR112016028226A2 publication Critical patent/BR112016028226A2/pt
Publication of BR112016028226B1 publication Critical patent/BR112016028226B1/pt

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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
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/7015—CHA-type, e.g. Chabazite, LZ-218
    • 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
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
    • 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
    • B01J20/16—Alumino-silicates
    • B01J20/18—Synthetic zeolitic molecular sieves
    • 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
    • B01J20/30—Processes for preparing, regenerating, or reactivating
    • B01J20/305—Addition of material, later completely removed, e.g. as result of heat treatment, leaching or washing, e.g. for forming pores
    • B01J20/3057—Use of a templating or imprinting material ; filling pores of a substrate or matrix followed by the removal of the substrate or matrix
    • 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
    • B01J20/30—Processes for preparing, regenerating, or reactivating
    • B01J20/3085—Chemical treatments not covered by groups B01J20/3007 - B01J20/3078
    • 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
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/7049—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing rare earth elements, titanium, zirconium, hafnium, zinc, cadmium, mercury, gallium, indium, thallium, tin or lead
    • B01J29/7065—CHA-type, e.g. Chabazite, LZ-218
    • 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
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
    • B01J29/723—CHA-type, e.g. Chabazite, LZ-218
    • 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
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
    • B01J29/76—Iron group metals or copper
    • B01J29/763—CHA-type, e.g. Chabazite, LZ-218
    • 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
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
    • 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
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/40—Catalysts, in general, characterised by their form or physical properties characterised by dimensions, e.g. grain size
    • 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
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/70—Catalysts, in general, characterised by their form or physical properties characterised by their crystalline properties, e.g. semi-crystalline
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/0009—Use of binding agents; Moulding; Pressing; Powdering; Granulating; Addition of materials ameliorating the mechanical properties of the product catalyst
    • B01J37/0018—Addition of a binding agent or of material, later completely removed among others as result of heat treatment, leaching or washing,(e.g. forming of pores; protective layer, desintegrating by heat)
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/024—Multiple impregnation or coating
    • B01J37/0246—Coatings comprising a zeolite
    • 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
    • B01J39/00—Cation exchange; Use of material as cation exchangers; Treatment of material for improving the cation exchange properties
    • B01J39/02—Processes using inorganic exchangers
    • 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
    • B01J39/00—Cation exchange; Use of material as cation exchangers; Treatment of material for improving the cation exchange properties
    • B01J39/08—Use of material as cation exchangers; Treatment of material for improving the cation exchange properties
    • B01J39/14—Base exchange silicates, e.g. zeolites
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B39/00—Compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites; Their preparation; After-treatment, e.g. ion-exchange or dealumination
    • C01B39/02—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof; Direct preparation thereof; Preparation thereof starting from a reaction mixture containing a crystalline zeolite of another type, or from preformed reactants; After-treatment thereof
    • C01B39/46—Other types characterised by their X-ray diffraction pattern and their defined composition
    • C01B39/48—Other types characterised by their X-ray diffraction pattern and their defined composition using at least one organic template directing agent
    • 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
    • B01J2220/00—Aspects relating to sorbent materials
    • B01J2220/40—Aspects relating to the composition of sorbent or filter aid materials
    • B01J2220/42—Materials comprising a mixture of inorganic materials
    • 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
    • B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
    • B01J2229/10—After treatment, characterised by the effect to be obtained
    • B01J2229/18—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself
    • B01J2229/186—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself not in framework positions
    • 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
    • B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
    • B01J2229/30—After treatment, characterised by the means used
    • B01J2229/42—Addition of matrix or binder particles
    • 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
    • B01J2235/00—Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties
    • B01J2235/05—Nuclear magnetic resonance [NMR]
    • 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
    • B01J2235/00—Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties
    • B01J2235/10—Infrared [IR]
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00—Crystal-structural characteristics
    • C01P2002/80—Crystal-structural characteristics defined by measured data other than those specified in group C01P2002/70
    • C01P2002/82—Crystal-structural characteristics defined by measured data other than those specified in group C01P2002/70 by IR- or Raman-data
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00—Crystal-structural characteristics
    • C01P2002/80—Crystal-structural characteristics defined by measured data other than those specified in group C01P2002/70
    • C01P2002/86—Crystal-structural characteristics defined by measured data other than those specified in group C01P2002/70 by NMR- or ESR-data

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Geology (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Silicates, Zeolites, And Molecular Sieves (AREA)
  • Catalysts (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)
BR112016028226-4A 2014-06-05 2015-06-03 Processo para preparação de um material zeolítico, material zeolítico sintético e uso de material zeolítico sintético BR112016028226B1 (pt)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
EP14171324 2014-06-05
EP14171324.8 2014-06-05
PCT/EP2015/062377 WO2015185625A2 (en) 2014-06-05 2015-06-03 Cha type zeolitic materials and methods for their preparation using combinations of cycloalkyl- and tetraalkylammonium compounds

Publications (2)

Publication Number Publication Date
BR112016028226A2 BR112016028226A2 (pt) 2017-08-22
BR112016028226B1 true BR112016028226B1 (pt) 2021-10-26

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BR112016028226-4A BR112016028226B1 (pt) 2014-06-05 2015-06-03 Processo para preparação de um material zeolítico, material zeolítico sintético e uso de material zeolítico sintético

Country Status (12)

Country Link
US (1) US10315924B2 (enExample)
EP (1) EP3152162B1 (enExample)
JP (1) JP6698555B2 (enExample)
KR (1) KR102410485B1 (enExample)
CN (1) CN106660024B (enExample)
BR (1) BR112016028226B1 (enExample)
CA (1) CA2951064C (enExample)
MX (1) MX379278B (enExample)
PL (1) PL3152162T3 (enExample)
RU (1) RU2678676C2 (enExample)
WO (1) WO2015185625A2 (enExample)
ZA (1) ZA201608280B (enExample)

Families Citing this family (20)

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US10556801B2 (en) 2015-02-12 2020-02-11 Basf Se Process for the preparation of a dealuminated zeolitic material having the BEA framework structure
ES2821890T3 (es) 2015-05-04 2021-04-28 Basf Se Procedimiento de preparación de melonal
EP3380226B1 (en) 2015-11-27 2019-10-23 Basf Se Ultrafast high space-time-yield synthesis of metal-organic frameworks
EP3178788A1 (en) 2015-12-08 2017-06-14 Basf Se A tin-containing zeolitic material having a bea framework structure
WO2017100384A1 (en) 2015-12-09 2017-06-15 Basf Corporation Cha type zeolitic materials and methods for their preparation using combinations of cycloal-kyl- and ethyltrimethylammonium compounds
EP3473598A4 (en) * 2016-05-23 2020-03-18 Tosoh Corporation CHA TYPE ZEOLITE AND PRODUCTION METHOD THEREFOR
JP7301541B2 (ja) 2016-06-13 2023-07-03 ビーエーエスエフ コーポレーション 触媒複合体及びｎｏｘの選択接触還元におけるその使用方法
CN109923070A (zh) * 2016-09-30 2019-06-21 庄信万丰股份有限公司 采用氟化物源的新的沸石合成
EP3533762A4 (en) 2016-10-25 2019-11-20 JGC Catalysts and Chemicals Ltd. ZEOLITE OF CHABAZITE TYPE FOR SUBSTRATE COATING
MY190284A (en) * 2017-10-11 2022-04-12 Tosoh Corp Metal-containing cha-type zeolite and method for producing the same
EP3728120A1 (en) 2017-12-21 2020-10-28 Basf Se A fast batch process for preparing a zeolitic material having framework type cha
JP6526847B1 (ja) * 2018-01-12 2019-06-05 エヌ・イーケムキャット株式会社 排ガス浄化触媒及びその製造方法
CN110240179B (zh) * 2018-03-09 2021-05-07 国家能源投资集团有限责任公司 Sapo-34分子筛及其制备方法和应用
KR102697497B1 (ko) * 2018-08-02 2024-08-22 바스프 에스이 유기주형에 의해 로딩된 종정을 사용한 제올라이트 물질의 연속 합성 방법
WO2020109292A1 (en) 2018-11-27 2020-06-04 Basf Se Mechanochemical activation in zeolite synthesis
WO2020109290A1 (en) 2018-11-27 2020-06-04 Basf Se Solvent-free mechanochemical activation in zeolite synthesis
US20220097033A1 (en) * 2018-12-19 2022-03-31 Basf Se Cha type zeolitic materials and methods for their preparation
WO2020225409A1 (en) 2019-05-09 2020-11-12 Basf Se Process for a continuous synthesis of a cha zeolitic material from an emulsion
KR20220164536A (ko) * 2020-04-07 2022-12-13 바스프 에스이 새로운 프레임워크 구조 유형의 제올라이트 및 이의 제조
EP4259330A1 (en) 2020-12-09 2023-10-18 BASF Corporation Preparation process of scr catalyst comprising cu and fe-exchanged zeolite, said catalyst, system comprising said catalyst and exhaust gas treatment using such

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US8409546B2 (en) * 2009-11-24 2013-04-02 Basf Se Process for the preparation of zeolites having B-CHA structure
WO2011064186A1 (en) 2009-11-24 2011-06-03 Basf Se Process for the preparation of zeolites having cha structure
JP5895510B2 (ja) * 2010-12-22 2016-03-30 東ソー株式会社 チャバザイト型ゼオライト及びその製造方法、銅が担持されている低シリカゼオライト、及び、そのゼオライトを含む窒素酸化物還元除去触媒、並びに、その触媒を使用する窒素酸化物還元除去方法
US9636667B2 (en) * 2012-06-04 2017-05-02 Basf Se CHA-type zeolite materials and methods for their preparation using cycloalkyammonium compounds
BR112014030263B1 (pt) 2012-06-04 2021-11-03 Basf Se Processo para a preparação de um material zeolítico que tem uma estrutura framework do tipo cha que compreende yo2 e x2o3 , material zeolítico sintético e uso de um material zeolítico sintético

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RU2016152444A3 (enExample) 2018-11-26
RU2678676C2 (ru) 2019-01-30
CA2951064A1 (en) 2015-12-10
BR112016028226A2 (pt) 2017-08-22
ZA201608280B (en) 2020-05-27
WO2015185625A3 (en) 2016-02-04
MX379278B (es) 2025-03-11
US20180186648A1 (en) 2018-07-05
RU2016152444A (ru) 2018-07-09
KR20170013989A (ko) 2017-02-07
PL3152162T3 (pl) 2019-05-31
WO2015185625A2 (en) 2015-12-10
EP3152162B1 (en) 2018-12-12
CN106660024A (zh) 2017-05-10
JP2017518251A (ja) 2017-07-06
CA2951064C (en) 2022-08-30
CN106660024B (zh) 2020-07-24
EP3152162A2 (en) 2017-04-12
MX2016016060A (es) 2017-03-28
JP6698555B2 (ja) 2020-05-27
US10315924B2 (en) 2019-06-11
KR102410485B1 (ko) 2022-06-20

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