# US 11,027,252 B2 · Reactor for continuous production of graphene and 2D inorganic compounds > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 11,027,252 B2 - Document ID: US11027252B2 - Status: Granted - Kind: B2 - Application number: 16/654,654 - Filed: 2019-10-16 - Published: 2021-04-22 - Granted: 2021-06-08 - Earliest claimed: 2019-10-16 - Assignees: Global Graphene Group, Inc. - Applicants: Nanotek Instruments, Inc. - Inventors: Yi-jun Lin; Hsuan-Wen Lee; Aruna Zhamu; Bor Z. Jang - Web page: https://patentgrep.com/patent/US11027252B2 ## CPC - B01J 8/10: moved by stirrers or by rotary drums or rotary receptacles {or endless belts} - C01B 32/19: by exfoliation - B01J 8/085: {Feeding reactive fluids (for solid material, see B01J8/0015)} - B01J 8/087: {Heating or cooling the reactor} - B01J 19/0006: {Controlling or regulating processes (controlling or regulating in general G05)} - B01J 19/0066: {Stirrers (mixing per se B01F)} - B01J 19/0093: {Microreactors, e.g. miniaturised or microfabricated reactors (laboratory containers with capillary fluid transport in microfabricated channels or chambers B01L3/5027)} - B01J 19/1881: {externally, i.e. the mixture leaving the vessel and subsequently re-entering it} - B01J 19/1887: {forming a thin film} - C01B 19/007: {Tellurides or selenides of metals (C01B19/002 takes precedence)} - C01B 21/0648: {After-treatment, e.g. grinding, purification (transformation of hexagonal into cubic or wurtzitic boron nitride C04B35/5831)} - C01B 32/192: starting from graphitic oxides - C01B 32/198: Graphene oxide - C01B 32/22: Intercalation - C01G 31/00: Compounds of vanadium - C01G 33/00: Compounds of niobium - C01G 35/00: Compounds of tantalum - C01G 39/06: Sulfides - C01G 41/00: Compounds of tungsten - B01J 2208/00203: Coils - B01J 2208/00212: Plates; Jackets; Cylinders - B01J 2208/00769: Details of feeding or discharging - B01J 2208/00858: Moving elements - B01J 2219/0009: Coils - B01J 2219/00094: Jackets - C01B 2204/02: Single layer graphene - C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram - C01P 2002/82: by IR- or Raman-data - C01P 2006/12: Surface area - B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS - C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C} - C01G: COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts or peroxyacids C01B15/00; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium, or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds containing nitrogen, other non-metals and metal C01B21/082}; metal amides C01B21/092; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanamide C01C3/16; thiocyanates C01C3/20) - C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS ## Abstract Provided is a continuous reactor system for producing graphene or an inorganic 2-D compound, the reactor comprising: (a) a first body comprising an outer wall and a second body comprising an inner wall, wherein the inner wall defines a bore and the first body is configured within the bore and a motor is configured to rotate the first and/or second body; (b) a reaction chamber between the outer wall of the first body and the inner wall of the second body; (c) a first inlet and a second inlet disposed at first end of the reactor and in fluid communication with the reaction chamber; (d) a first outlet and a second outlet disposed downstream from the first inlet, the outlets being in fluid communication with the reaction chamber; and (e) a flow return conduit having two inlets/outlets in fluid communication with two ends of the reactor. ## Claims ### Claim 1 A continuous reactor or reactor system for producing graphene or an inorganic 2-D compound, said reactor comprising: A) a first body comprising an outer wall and a second body comprising an inner wall, wherein the inner wall defines a bore and the first body is configured within the bore and wherein a motor is configured to rotate the first and/or second body at a rate of from 300 to 500 rpm; B) a reaction chamber being configured between the outer wall of the first body and the inner wall of the second body; C) a first inlet and a second inlet disposed at or near a first end of the reactor and being configured to be in fluid communication with the reaction chamber; D) a first outlet and a second outlet disposed downstream from said first and second inlet at or near a second end of the reactor, the first outlet and the second outlet being configured to be in fluid communication with the reaction chamber; and E) a flow return conduit having a first conduit inlet in fluid communication with the second outlet of the reactor and having a first conduit outlet in fluid communication with the second inlet of the reactor; wherein said reactor or reactor system is operated to receive a first stock of reactants, containing a graphitic material or an inorganic layered compound dispersed in a liquid medium, through the first inlet into the reaction chamber, driving the reactants downstream toward said first and second outlet and facilitating reactions between the reactants to produce a first product slurry, driving the first product slurry through the flow return conduit and the second inlet of the reactor to re-enter the reaction chamber, and further driving the first product slurry downstream toward the first and second outlet to form a second product slurry, which is discharged off the reaction chamber through the first outlet of the reactor or driven to flow through the conduit to return to the reaction chamber through the second inlet for at least another time, wherein the first body has a length and a diameter and the length-to-diameter ratio is no greater than 30. ### Claim 2 (depends on 1) The reactor or reactor system of claim 1, further comprising a pump to drive the first or second product slurry through the conduit back to the reaction chamber. ### Claim 3 (depends on 1) The reactor or reactor system of claim 1, further comprising a pump configured to inject the first stock of reactants into the reaction chamber. ### Claim 4 (depends on 1) The reactor or reactor system of claim 1, wherein the outer wall of the first body defines a cylindrical body. ### Claim 5 (depends on 1) The reactor or reactor system of claim 1, wherein the inner wall of the second body defines a cylindrical bore. ### Claim 6 (depends on 1) The reactor or reactor system of claim 1, wherein the first body has a length and a diameter and the length-to-diameter ratio is from 3 to 20. ### Claim 7 (depends on 1) The reactor or reactor system of claim 1, wherein the first body and/or second body independently comprise a stainless-steel alloy, an austenitic stainless steel, an austenitic chromium-nickel stainless steel, a super duplex stainless steel alloy, polytetrafluoroethylene (PTFE), glass coated metal, borosilicate glass, PTFE-coated metal, nickel-chromium-molybdenum-tungsten alloy, stainless steel with silicon, a Ni—Fe—Cr— Mo alloy, a Ni—Cr—Mo alloy, an alloy, lead, high silicon cast iron, cast iron, ductile iron, or a combination thereof. ### Claim 8 (depends on 1) The reactor or reactor system of claim 1, further comprising a cooling jacket or cooling coil in at least partial surrounding relation to the second body. ### Claim 9 (depends on 1) The reactor or reactor system of claim 1, further comprising a heating jacket or heating coil in at least partial surrounding relation to the second body. ### Claim 10 (depends on 1) The reactor or reactor system of claim 1, further comprising at least a stock reservoir, the stock reservoir in fluid contact with the first inlet. ### Claim 11 (depends on 1) The reactor or reactor system of claim 1, further comprising one or more additional inlet(s), the one or more additional inlet(s) in fluid communication with the reaction chamber, and the one or more additional inlet(s) being configured in a longitudinal position between the first inlet and the first outlet. ### Claim 12 (depends on 1) The reactor or reactor system of claim 1, wherein the continuous reactor has a flow from the first inlet to the first outlet, the flow being a vortex flow. ### Claim 13 (depends on 12) The reactor or reactor system of claim 12, wherein the vortex flow is a toroidal vortex flow. ### Claim 14 (depends on 1) The reactor or reactor system of claim 1, wherein the continuous reactor is configured to produce a toroidal vortex flow. ### Claim 15 (depends on 13) The reactor or reactor system of claim 13, wherein the toroidal vortex flow comprises a plurality of non-axisymmetric toroidal vortices. ### Claim 16 (depends on 1) The reactor or reactor system of claim 1, wherein the continuous reactor is a continuous Couette-Taylor reactor. ### Claim 17 (depends on 1) The reactor or reactor system of claim 1, wherein the continuous reactor comprises a reactor chamber into which the first stock is injected; the reactor chamber being configured between an outer wall of a first cylindrical body and the inner wall of a second cylindrical body or bore, one or both of the first and second cylindrical bodies rotating around the axis thereof. ### Claim 18 (depends on 1) The reactor or reactor system of claim 1, wherein the first and second cylindrical bodies are rotating in opposite directions. ### Claim 19 (depends on 1) The reactor or reactor system of claim 1, wherein the liquid medium contains an acid selected from sulfuric acid, nitric acid, phosphoric acid, or a combination thereof, wherein at least 80% of the graphene sheets within product slur, which is not sent to an inlet, are single layer graphene sheets. ### Claim 20 (depends on 1) The reactor or reactor system of claim 1, wherein the graphitic material is selected natural graphite, artificial graphite, highly oriented pyrolytic graphite (HOPG), meso-carbon micro-bead (MCMB), carbon fiber, graphite fiber, carbon nano-fiber, graphite nano-fiber, multi-walled carbon nano-tube, soft carbon, hard carbon, activated carbon, meso-phase pitch, needle coke, coal, graphite oxide, graphite halogenide, hydrogenated graphite, nitrogenated graphite, or a combination thereof. ### Claim 21 A continuous reactor or reactor system for producing an inorganic 2-D compound, said reactor comprising: A) a first body comprising an outer wall and a second body comprising an inner wall, wherein the inner wall defines a bore and the first body is configured within the bore and wherein a motor is configured to rotate the first and/or second body; B) a reaction chamber being configured between the outer wall of the first body and the inner wall of the second body; C) a first inlet and a second inlet disposed at or near a first end of the reactor and being configured to be in fluid communication with the reaction chamber; D) a first outlet and a second outlet disposed downstream from said first and second inlet at or near a second end of the reactor, the first outlet and the second outlet being configured to be in fluid communication with the reaction chamber; and E) a flow return conduit having a first conduit inlet in fluid communication with the second outlet of the reactor and having a first conduit outlet in fluid communication with the second inlet of the reactor; wherein said reactor or reactor system is operated to receive a first stock of reactants, containing an inorganic layered compound dispersed in a liquid medium, through the first inlet into the reaction chamber, driving the reactants downstream toward said first and second outlet and facilitating reactions between the reactants to produce a first product slurry, driving the first product slurry through the flow return conduit and the second inlet of the reactor to re-enter the reaction chamber, and further driving the first product slurry downstream toward the first and second outlet to form a second product slurry, which is discharged off the reaction chamber through the first outlet of the reactor or driven to flow through the conduit to return to the reaction chamber through the second inlet for at least another time, wherein the inorganic layered compound is selected from boron nitride (h-BN), HfS2, tungsten disulfide (WS2), NiTe2, VSe2, WSe2, molybdenum disulfide (MoS2), MoSe2, MoTe2, TaS2, RhTe2, PdTe2, NbS2, NbSe2, NbTe2, TaSe2, Bi2Se3, Bi2Te3, or a combination thereof. ### Claim 22 (depends on 1) The reactor or reactor system of claim 1, wherein said liquid medium further comprises a surfactant. ### Claim 23 (depends on 1) The reactor or reactor system of claim 1, further comprising a cooling jacket or cooling coil and/or a heating jacket or heating coil in at least partial surrounding relation to the second body.