# US 10,308,516 B2 · Zeolite production method > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 10,308,516 B2 - Document ID: US10308516B2 - Status: Granted - Kind: B2 - Application number: 14/990,431 - Filed: 2016-01-07 - Published: 2016-04-28 - Granted: 2019-06-04 - Earliest claimed: 2013-07-09 - Assignees: Mitsubishi Chemical Corporation; The University of Tokyo - Applicants: Mitsubishi Chemical Corporation; The University of Tokyo - Inventors: Tatsuya Okubo; Toru Wakihara; Zhendong Liu; Takahiko Takewaki; Kazunori Oshima; Daisuke Nishioka - Web page: https://patentgrep.com/patent/US10308516B2 ## CPC - C01B 39/54: Phosphates, e.g. APO or SAPO compounds - B01J 8/085: {Feeding reactive fluids (for solid material, see B01J8/0015)} - B01J 8/087: {Heating or cooling the reactor} - B01J 19/243: {spirally, concentrically or zigzag wound} - B01J 29/06: Crystalline aluminosilicate zeolites; Isomorphous compounds thereof - B01J 29/70: of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 - B01J 29/7015: {CHA-type, e.g. Chabazite, LZ-218} - B01J 29/763: {CHA-type, e.g. Chabazite, LZ-218} - B01J 29/83: Aluminophosphates [APO compounds] - B01J 29/85: Silicoaluminophosphates [SAPO compounds] - C01B 39/02: 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 - C01B 39/04: using at least one organic template directing agent, e.g. an ionic quaternary ammonium compound or an aminated compound - C01B 39/10: the replacing atoms being {at least} phosphorus atoms - C01B 39/46: Other types characterised by their X-ray diffraction pattern and their defined composition {(C01B39/023, C01B39/026, C01B39/06 take precedence)} - C01B 39/48: using at least one organic template directing agent - B01J 2208/00106: by indirect heat exchange - B01J 2208/00168: with heat exchange elements outside the bed of solid particles - B01J 2208/00283: involving reactant liquids - B01J 2208/00752: Feeding - B01J 2208/065: Heating or cooling the reactor - B01J 2219/00099: the reactor being immersed in the heat exchange medium - 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 ## Abstract Provided is a method for continuous production of zeolite in which a starting material is continuously supplied to a tubular reactor to produce an aluminophosphate zeolite that contains, in the framework structure, at least aluminum atoms and phosphorus atoms or an aluminosilicate zeolite having 5≤SiO2/Al2O3≤2000. The tubular reactor is heated using a heat medium; a ratio (volume)/(lateral surface area) of the volume (inner capacity) to the lateral surface area of the tubular reactor is 0.75 cm or smaller; and seed crystals are added to the starting material. Through using a small-diameter tubular reactor and heating with a heat medium, it becomes possible to heat sufficiently the entirety of a starting material (zeolite precursor gel) in a short time, and to allow reaction to proceed at a high rate. The occurrence of irregular pressure fluctuations during continuous production of the zeolite can be prevented by adding seed crystals. ## Claims ### Claim 1 A method for continuous production of zeolite, wherein a starting material is continuously supplied to a tubular reactor to produce an aluminophosphate zeolite that contains, in a framework structure, at least aluminum atoms and phosphorus atoms or an aluminosilicate zeolite having 5≤SiO2/Al2O3≤2000, the starting material comprises a zeolite precursor gel, the tubular reactor is heated using a heat medium, a ratio (volume)/(lateral surface area) of the volume (inner capacity) to the lateral surface area of the tubular reactor is 0.75 cm or smaller, and seed crystals and a template are added to the starting material. ### Claim 2 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein after heating of the starting material that is supplied into the tubular reactor, the zeolite precursor gel is further added to an intermediate product in the tubular reactor, so as to come into contact with the starting material after heating. ### Claim 3 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein the zeolite structure of the zeolite, as established by IZA, is AFI. ### Claim 4 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein the zeolite structure of the zeolite, as established by IZA, is CHA. ### Claim 5 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein the starting material is aged for 2 hours or longer. ### Claim 6 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein the framework density of the zeolite ranges from 12.0 T/1,000 Å3 to 17.5 T/1,000 Å3. ### Claim 7 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein the zeolite comprises a transition metal. ### Claim 8 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein the tubular reactor comprises an independent tubular reactor having an openable and closable lid; the starting material is supplied to the tubular reactor and the lid is closed; thereafter, the tubular reactor is heated by being placed in the heat medium; and thereafter, the tubular reactor is retrieved from the heat medium, the lid is opened, and a product is retrieved. ### Claim 9 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein the tubular reactor comprises an independent tubular reactor having an openable and closable lid; the starting material is supplied to the tubular reactor and the lid is closed; thereafter, the tubular reactor is heated by being placed in the heat medium; and thereafter, the tubular reactor is retrieved from the heat medium, the lid is opened, a product is retrieved, and the product is kept at a lower temperature than during reaction. ### Claim 10 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein in case of production of aluminophosphate zeolite, the zeolite precursor gel contains an aluminum source and a phosphorus source, and in case of production of aluminosilicate zeolite, the zeolite precursor gel contains an aluminum source and a silicon source. ### Claim 11 (depends on 1) The method for continuous production of zeolite according to claim 1, wherein an average particle size of the seed crystals is in a range of 0.1 μm or greater and 100 μm or smaller. ### Claim 12 A method for continuous production of zeolite, wherein a starting material is supplied into a tubular reactor, followed by heating the tubular reactor with a heat medium, to produce an aluminophosphate zeolite that contains, in a framework structure, at least aluminum atoms and phosphorus atoms or an aluminosilicate zeolite having 5≤SiO2/Al2O3≤2000 (molar ratio), wherein a diameter of the tubular reactor is set to be equal to or smaller than 3 cm, the starting material comprises a zeolite precursor gel, and seed crystals and a template are added to the starting material.