# US 10,870,582 B2 · Method of producing beta zeolite > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 10,870,582 B2 - Document ID: US10870582B2 - Status: Granted - Kind: B2 - Application number: 16/310,640 - Filed: 2017-06-13 - Published: 2019-06-13 - Granted: 2020-12-22 - Earliest claimed: 2016-06-17 - Assignees: Mitsui Mining & Smelting Co., Ltd.; The University of Tokyo - Applicants: Mitsui Mining & Smelting Co., Ltd.; The University of Tokyo - Inventors: Keiji Itabashi; Shanmugam Palani Elangovan; Tatsuya Okubo - Web page: https://patentgrep.com/patent/US10870582B2 ## CPC - C01B 39/46: Other types characterised by their X-ray diffraction pattern and their defined composition {(C01B39/023, C01B39/026, C01B39/06 take precedence)} - B01J 20/18: Synthetic zeolitic molecular sieves - B01J 20/28004: {Sorbent size or size distribution, e.g. particle size} - B01J 29/7007: {Zeolite Beta} - B01J 35/40: characterised by dimensions, e.g. grain size (in a colloidal state B01J35/23; crystallite size B01J35/77) - C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram - C01P 2004/61: Micrometer sized, i.e. from 1-100 micrometer - C01P 2004/62: Submicrometer sized, i.e. from 0.1-1 micrometer - C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C} - B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS - C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS ## Abstract Provided is a production method with which it is possible to produce beta zeolite at high purity by suppressing the generation of impurities by a seed crystal addition method that can reduce the environmental burden as much as possible, without using an organic structure-directing agent. This method for producing beta zeolite having a step that mixes and heats an organic-compound-free reaction mixture comprising a silica source, alumina source, alkali source, and water with beta zeolite seed crystals, wherein (I) beta zeolite synthesized without using an organic structure-directing agent and having 90% or more by volume of particles 10 μm or less in diameter in the particle size distribution by a laser diffraction scattering-type particle size distribution measurement method is used, (III) acid-treated zeolite in which the SiO2/Al2O3 ratio is 150 or less is prepared by (II) contact treatment with an acidic aqueous solution, and the acid-treated zeolite is used as the beta zeolite seed crystals. ## Claims ### Claim 1 A method of producing a beta zeolite comprising: mixing an organic compound-free reaction mixture containing a silica source, an alumina source, an alkaline source and water with a beta zeolite seed crystal and heating the resulting mixture, wherein (I) a beta zeolite which is synthesized without using an organic structure-directing agent and comprises particles having a particle size of 10 μm or less in an amount of 90% or more on a volume basis in the particle size distribution as determined by a laser diffraction/scattering particle size distribution measuring method, (II) the beta zeolite is subjected to contact treatment with an aqueous acidic solution, and thereby (III) an acid-treated zeolite having a SiO2/Al2O3 molar ratio of 150 or less is prepared and this is used as the beta zeolite seed crystal. ### Claim 2 (depends on 1) The method of producing a beta zeolite according to claim 1, wherein (1) and (2) below are used in combination as the beta zeolite seed crystal: (1) the acid-treated zeolite and (2) the beta zeolite which is synthesized without using an organic structure-directing agent, comprises particles having a particle size of 10 μm or less in an amount of 90% or more on a volume basis in the particle size distribution and is not subjected to contact treatment with an acidic aqueous solution. ### Claim 3 (depends on 1) The method of producing a beta zeolite according to claim 1, wherein (1) and (3) below are used in combination as the beta zeolite seed crystal: (1) the acid treated zeolite and (3) a calcined crystal of the beta zeolite synthesized using an organic structure-directing agent. ### Claim 4 (depends on 1) The method of producing a beta zeolite according to claim 1, wherein the reaction mixture has molar ratios described below: SiO2/Al2O3=8 or more and less than 40, Na2O/SiO2=0.05 or more and 0.3 or less and H2O/SiO2=5 or more and 50 or less. ### Claim 5 (depends on 1) The method of producing a beta zeolite according to claim 1, wherein the SiO2/Al2O3 molar ratio of the acid-treated zeolite is 100 or less. ### Claim 6 (depends on 1) The method of producing a beta zeolite according to claim 1, comprising preparing a solid-liquid mixture containing (i) below as the beta zeolite seed crystal and adding the solid-liquid mixture to the reaction mixture, wherein (i) is a beta zeolite which is synthesized without using an organic structure-directing agent, comprises particles having a particle size of 10 μm or less in an amount of 90% or more on a volume basis in the particle size distribution and is subjected to contact with an acidic aqueous solution. ### Claim 7 (depends on 6) The method of producing a beta zeolite according to claim 6, comprising using a solid-liquid mixture obtained by mixing (i) above and (ii) below as the beta zeolite seed crystal and adding the solid-liquid mixture to the reaction mixture, wherein (ii) is a beta zeolite which is synthesized without using an organic structure-directing agent, comprises particles having a particle size of 10 μm or less in an amount of 90% or more on a volume basis in the particle size distribution and is not subjected to contact with an acidic aqueous solution. ### Claim 8 (depends on 6) The method of producing a beta zeolite according to claim 6, comprising using a solid-liquid mixture obtained by mixing (i) above with (iii) below as the beta zeolite seed crystal and adding the solid-liquid mixture to the reaction mixture, wherein (iii) is a calcined crystal of beta zeolite synthesized using an organic structure-directing agent. ### Claim 9 (depends on 1) The method of producing a beta zeolite according to claim 1, wherein particles of the beta zeolite which is synthesized without using an organic structure-directing agent are sorting out by (A) a method of sorting out only crystal particles having a small particle size by adjusting a size of opening of filtration cloth used in filtration, (B) a method of sorting out by using a slurry in which crystals are dispersed and sorting out by sedimentation method, (C) a wet method, or (D) a dry method, prior to being subjected to the contact treatment.