US-12617675-B1 - Systems and methods of pyrolyzing hydrocarbons

US12617675B1US 12617675 B1US12617675 B1US 12617675B1US-12617675-B1

Abstract

Systems and methods of pyrolyzing gaseous hydrocarbons include a reaction chamber and a plenum in fluid communication therewith. A light source directs electromagnetic radiation through a window into the reaction chamber. A first recirculation conduit connected between an offtake and an intake of the reaction chamber recirculates to the intake of the reaction chamber a portion of an aerosol product from the offtake of the reaction chamber. A filter operatively associated with the offtake of the reaction chamber receives un-recirculated amounts of the aerosol product and produces a retentate that includes particulate matter removed from the aerosol product. First and second gas separators operatively associated with the filter separate hydrogen and unreacted hydrocarbons from a filtrate of the filter. A second recirculation conduit connected between the second gas separator and the intake of the plenum recirculates unreacted hydrocarbons from the filtrate to the plenum.

Inventors

Patrick J. Panzarino

Assignees

Plan Beta LLC

Dates

Publication Date: 20260505
Application Date: 20250806

Claims (20)

1 . A method of pyrolyzing a hydrocarbon reactant material to produce hydrogen, comprising: introducing the hydrocarbon reactant material into an intake of a plenum operatively associated with a reaction chamber, the reaction chamber defining a plurality of apertures therein that are in fluid communication with the plenum so that the hydrocarbon reactant material in the plenum is introduced into the reaction chamber at multiple locations; introducing a particulate material into an intake of the reaction chamber, the particulate material mixing with the hydrocarbon reactant material from the plenum to form an aerosol; exposing the aerosol to electromagnetic radiation sufficient to raise the temperature of the particulate material to a level sufficient to initiate pyrolyzation of the gaseous hydrocarbon reactant material to produce an aerosol product; withdrawing the aerosol product via an offtake of the reaction chamber; recirculating a portion of the withdrawn aerosol product to the intake of the reaction chamber, the recirculated portion of the aerosol product mixing with additional quantities of the gaseous hydrocarbon reactant material from the plenum, the recirculated portion of the aerosol product comprising the particulate material that is introduced into the intake of the reaction chamber; filtering non-recirculated portions of the aerosol product to produce a filtrate substantially devoid of particulate matter; separating a first gas constituent from the filtrate, the first gas constituent comprising hydrogen; separating a second gas constituent from the filtrate, the second gas constituent comprising unreacted amounts of the gaseous hydrocarbon reactant material; recirculating the separated second gas constituent to the inlet of the plenum; and diffusing the hydrocarbon reactant material through a porous felt material positioned adjacent the plurality of apertures defined by the reaction chamber.
2 . The method of claim 1 , further comprising cooling the filtrate before performing at least one of said separating the first gas constituent and said separating the second gas constituent.
3 . The method of claim 2 , further comprising filtering the cooled filtrate to remove additional amounts of particulate matter retained in the filtrate before performing at least one of said separating the first gas constituent and said separating the second gas constituent.
4 . The method of claim 1 , wherein said introducing the particulate material into the intake of the reaction chamber comprises introducing a particulate seed material into the intake of the reaction chamber; and wherein said method further comprises terminating said providing the particulate seed material into the intake of the reaction chamber after said recirculating the portion of the withdrawn aerosol product to the intake of the reaction chamber.
5 . The method of claim 4 , wherein said introducing the particulate seed material into the reaction chamber comprises introducing carbon particles into the reaction chamber.
6 . The method of claim 5 , wherein said introducing carbon particles into the reaction chamber comprises introducing carbon particles having a D50 particle size less than about 100 μm.
7 . The method of claim 1 , further comprising introducing a catalyst material into the intake of the reaction chamber.
8 . The method of claim 7 , wherein said introducing a catalyst material into the intake of the reaction chamber comprises introducing a catalyst material comprising one or more selected from the group consisting of carbon black, activated carbon, Fe 3 O 4 , Fe 2 O 3 , FeO, and CoFeNi oxide into the intake of the reaction chamber.
9 . The method of claim 1 , wherein said introducing the hydrocarbon reactant material into the intake of the plenum comprises introducing natural gas into the intake of the plenum.
10 . The method of claim 1 , wherein said introducing the hydrocarbon reactant material into the intake of the plenum comprises introducing methane gas into the intake of the plenum.
11 . The method of claim 1 , wherein said exposing the aerosol to electromagnetic radiation comprises exposing the aerosol to light having wavelengths within the range of about 8 μm to about 15 μm.
12 . The method of claim 11 , wherein said exposing the aerosol to light having wavelengths within the range of about 8 μm to about 15 μm comprises exposing the aerosol to light having a wavelength of about 10.6 μm.
13 . The method of claim 1 , wherein said exposing is conducted at an absolute pressure in a range of about 0.5 bar to about 1.5 bar.
14 . The method of claim 13 , wherein said exposing is conducted at an absolute pressure of about 1 bar.
15 . The method of claim 1 , further comprising purging at least the reaction chamber and the plenum with nitrogen gas before said introducing the hydrocarbon reactant material into the plenum.
16 . Hydrogen gas produced by a method comprising: introducing a gaseous hydrocarbon reactant material into an intake of a plenum operatively associated with a reaction chamber, the reaction chamber defining a plurality of apertures therein that are in fluid communication the plenum so that hydrocarbon reactant material in the plenum is introduced into the reaction chamber at multiple locations; introducing a particulate material into an intake of the reaction chamber, the particulate material mixing with the gaseous hydrocarbon reactant material from the plenum to form an aerosol; exposing the aerosol to electromagnetic radiation sufficient to raise the temperature of the particulate seed material to a range of about 400° C. to about 1200° C. to pyrolyze the gaseous hydrocarbon reactant material to produce an aerosol product; withdrawing the aerosol product via an offtake of the reaction chamber; recirculating a portion of the withdrawn aerosol product to the intake of the reaction chamber, the recirculated portion of the aerosol product mixing with additional quantities of the gaseous hydrocarbon reactant material from the plenum, the recirculated portion of the aerosol product comprising the particulate material that is introduced into the intake of the reaction chamber; filtering non-recirculated portions of the aerosol product to produce a filtrate substantially devoid of particulate matter; separating hydrogen gas from the filtrate; and diffusing the hydrocarbon reactant material through a porous felt material positioned adjacent the plurality of apertures defined by the reaction chamber.
17 . The method of claim 1 , wherein the plurality of apertures defined by the reaction chamber extend along a length of the reaction chamber and wherein said introducing the hydrocarbon reactant material into the reaction chamber further comprises introducing the hydrocarbon reactant material into the reaction chamber at multiple locations along a length of the reaction chamber.
18 . The method of claim 17 , wherein said introducing the particulate material into the intake of the reaction chamber further comprises introducing the particulate material into an intake located at about a first end of the reaction chamber.
19 . The method of claim 18 , wherein said withdrawing the aerosol product via the offtake of the reaction chamber further comprises withdrawing the aerosol product via an offtake located at about a second end of the reaction chamber.
20 . A method of pyrolyzing a hydrocarbon reactant material to produce hydrogen, comprising: introducing the hydrocarbon reactant material into a reaction chamber at multiple locations, wherein said introducing comprises diffusing the hydrocarbon reactant material through a porous felt material provided within the reaction chamber; introducing a particulate material into an intake of the reaction chamber, the particulate material mixing with the hydrocarbon reactant material introduced via the multiple locations to form an aerosol; exposing the aerosol to electromagnetic radiation sufficient to raise the temperature of the particulate material to a level sufficient to initiate pyrolyzation of the gaseous hydrocarbon reactant material to produce an aerosol product; withdrawing the aerosol product via an offtake of the reaction chamber; recirculating a portion of the withdrawn aerosol product to the intake of the reaction chamber, the recirculated portion of the aerosol product mixing with additional quantities of the gaseous hydrocarbon reactant material introduced via the multiple locations, the recirculated portion of the aerosol product comprising the particulate material that is introduced into the intake of the reaction chamber; filtering non-recirculated portions of the aerosol product to produce a filtrate substantially devoid of particulate matter; separating a first gas constituent from the filtrate, the first gas constituent comprising hydrogen; separating a second gas constituent from the filtrate, the second gas constituent comprising unreacted amounts of the gaseous hydrocarbon reactant material; and recirculating the separated second gas constituent to the reaction chamber so that the separated second gas constituent is introduced into the reaction chamber via the multiple locations.

Description

TECHNICAL FIELD The present invention relates to systems and methods for carrying out high-temperature dissociation reactions in general and more specifically to systems and methods of dissociating hydrocarbon reactant materials. BACKGROUND Various types of systems and methods of pyrolyzing or dissociating hydrocarbon reactant materials are well-known in the art and have been used for decades to produce hydrogen, hydrogen-containing gases, and carbon, for example. In the case of hydrocarbons, the dissociation reactions are conducted in the absence of oxygen, thereby eliminating or substantially reducing the production of carbon dioxide. Such systems generally involve a reactor for receiving the hydrocarbon reactant material and a means for heating the hydrocarbon reactant material within the reactor to initiate and maintain the pyrolyzation or dissociation reaction. The reaction is endothermic and requires a constant supply of energy to maintain the reaction. The energy may be provided from any of a wide range of sources, including electrically heated elements, electric arcs, flames, or radiant energy from solar or laser sources, for example. Many such reactors transfer heat to the reactants by convection and/or conduction, which may limit the types of materials that can be used for the reactors. Moreover, in the case of a convective reactor, a significant portion of the heat energy required for the continued pyrolyzation reaction may come from the reactor walls themselves. However, since the reactor walls are good reaction sites, dissociated carbon from the reaction tends to build up on the reactor walls, which results in reduced heat transfer and, in some reactor designs, even clogging of internal tubes. Such reactors also may be susceptible to thermal runaway. For example, during the pyrolysis of natural gas, the thermal conductivity of the gas phase may suddenly increase, often by an order of magnitude or more, depending on the composition of the gas. Because it is difficult to quickly control the temperature of a convective reactor, such reactors are prone to thermal runaway, which can result in explosions. Partly in an effort to address some of the drawbacks associated with convective reactors, several different types of fluid wall reactors have been developed. While such fluid wall reactors have proven effective in addressing some of these drawbacks associated with convective reactors, they have not proven to be a panacea. For example, many fluid wall reactors are complex and difficult to construct or may require the provision of substantial amounts of inert gases to be supplied during operation, thereby increasing costs. Consequently, there is a continuing need for systems and methods for pyrolyzing hydrocarbon reactant materials that solve some of the drawbacks associated with known systems and methods. SUMMARY One embodiment of a method of pyrolyzing a hydrocarbon reactant material according to the disclosed instrumentalities may include: Introducing the hydrocarbon reactant material into an intake of a plenum that is in fluid communication with a reaction chamber; introducing a particulate material into an intake of the reaction chamber, the particulate material mixing with the hydrocarbon reactant material from the plenum to form an aerosol; exposing the aerosol to electromagnetic radiation of sufficient energy to raise the temperature of the particulate material to a level sufficient to initiate pyrolyzation of the gaseous hydrocarbon reactant material and produce an aerosol product; withdrawing the aerosol product via an offtake of the reaction chamber; recirculating a portion of the withdrawn aerosol product to the intake of the reaction chamber, the recirculated portion of the aerosol product mixing with additional quantities of the gaseous hydrocarbon reactant material from the plenum, the recirculated portion of the aerosol product comprising the particulate material that is introduced into the intake of the reaction chamber; filtering non-recirculated portions of the aerosol product to produce a filtrate substantially devoid of particulate matter; separating a first gas constituent from the filtrate, the first gas constituent comprising hydrogen; separating a second gas constituent from the filtrate, the second gas constituent comprising unreacted amounts of the gaseous hydrocarbon reactant material; and recirculating the second gas constituent to the inlet of the plenum. Also disclosed is hydrogen gas produced by a method that includes: Introducing a gaseous hydrocarbon reactant material into an intake of a plenum that is in fluid communication with a reaction chamber; introducing a particulate material into an intake of the reaction chamber, the particulate material mixing with the gaseous hydrocarbon reactant material from the plenum to form an aerosol; exposing the aerosol to electromagnetic radiation sufficient to raise the carbon particulate seed material to a temperature in a range