WO2019000030A1 - Appareil et méthode de génération d'oxygène et de conversion ou de stockage d'énergie - Google Patents

Appareil et méthode de génération d'oxygène et de conversion ou de stockage d'énergie Download PDF

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Publication number
WO2019000030A1
WO2019000030A1 PCT/AU2018/050645 AU2018050645W WO2019000030A1 WO 2019000030 A1 WO2019000030 A1 WO 2019000030A1 AU 2018050645 W AU2018050645 W AU 2018050645W WO 2019000030 A1 WO2019000030 A1 WO 2019000030A1
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Prior art keywords
oxygen
reduction
reactor
oxidation
res
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Ceased
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PCT/AU2018/050645
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English (en)
Inventor
Behdad Moghtaderi
Cheng Zhou
Hui Song
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Infratech Industries Pty Ltd
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Infratech Industries Pty Ltd
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Priority claimed from AU2017902481A external-priority patent/AU2017902481A0/en
Application filed by Infratech Industries Pty Ltd filed Critical Infratech Industries Pty Ltd
Priority to AU2018293554A priority Critical patent/AU2018293554A1/en
Publication of WO2019000030A1 publication Critical patent/WO2019000030A1/fr
Anticipated expiration legal-status Critical
Priority to AU2024202999A priority patent/AU2024202999A1/en
Ceased legal-status Critical Current

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Classifications

    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN  A CARRIER GAS OR AIR 
    • F23C10/00—Fluidised bed combustion apparatus
    • 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
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/18—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles
    • B01J8/24—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles according to "fluidised-bed" technique
    • B01J8/26—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles according to "fluidised-bed" technique with two or more fluidised beds, e.g. reactor and regeneration installations
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
    • C01B13/02—Preparation of oxygen
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
    • C01B13/02—Preparation of oxygen
    • C01B13/08—Preparation of oxygen from air with the aid of metal oxides, e.g. barium oxide, manganese oxide
    • C01B13/086—Preparation of oxygen from air with the aid of metal oxides, e.g. barium oxide, manganese oxide with manganese oxide
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN  A CARRIER GAS OR AIR 
    • F23C2900/00—Special features of, or arrangements for combustion apparatus using fluid fuels or solid fuels suspended in air; Combustion processes therefor
    • F23C2900/99008—Unmixed combustion, i.e. without direct mixing of oxygen gas and fuel, but using the oxygen from a metal oxide, e.g. FeO
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E20/00—Combustion technologies with mitigation potential
    • Y02E20/34—Indirect CO2mitigation, i.e. by acting on non CO2directly related matters of the process, e.g. pre-heating or heat recovery

Definitions

  • the present invention relates to an apparatus and method for producing oxygen and energy conversion or storage and in particular relates to a chemical looping- based oxygen production and energy conversion apparatus and method.
  • the invention has been developed primarily for the production of oxygen and energy conversion or storage for domestic, industrial, medical, emergency service and military applications.
  • thermo-chemical energy storage is a key technology for managing the balance between energy demand and supply, which is an important element for the successful transition towards a low-carbon economy. Storing energy as economically as possible is the key challenge faced by thermo-chemical energy storage technologies.
  • thermo-chemical energy storage technology employs a chemical looping based redox energy storage (RES) system, which simultaneously produces and, where possible, to stores heat, electricity, and/or oxygen.
  • RES redox energy storage
  • a first aspect of the invention provides an apparatus for generating oxygen, comprising a reduction reactor, an oxidation reactor fluidly connected to the reduction reactor so that oxygen carrier particles can be transferred between the reduction reactor and the oxidation reactor, an outlet conduit arranged to transfer an oxygen enriched mixture from the reduction reactor to an oxygen storage unit, wherein the reduction reactor is located at least partially within the oxidation reactor.
  • the reduction reactor is located within the oxidation reactor.
  • the reduction reactor is located adjacent the bed of the oxidation reactor. In another embodiment, the reduction reactor is located partly within the bed of the oxidation reactor. In a further embodiment, the reduction reactor is located within the bed of the oxidation reactor.
  • the reduction reactor is a fluidised bed reactor.
  • the oxidation reactor is a fluidised bed reactor.
  • one or more transfer conduits fluidly connect the reduction reactor and the oxidation reactor.
  • the reduction reactor, the oxidation reactor, and the outlet conduit form an integrated chemical looping air separation unit.
  • a second aspect of the invention provides a method for generating oxygen, comprising:
  • the heat generated by the oxidation process is used to maintain the reduction process at the higher temperature.
  • the reduction process is carried out 100 e to 150 e C higher than the oxidation process.
  • the temperature of the reduction process is at least 900 e C. In other embodiments, the temperature of the reduction process is between 900 e C and 1 ,150 e C. In one embodiment, the temperature of the reduction process is between 900 e C and 950 e C. In another embodiment, the temperature of the reduction process is between 1 ,000 e C and 1 ,050 e C. In a further embodiment, the temperature of the reduction process is between 1 ,100 e C and 1 ,150 e C. In one preferred embodiment, the temperature of the reduction process is around 950 e C.
  • the temperature of the oxidation process is at least 800 e C. In other embodiments, the temperature of the oxidation process is between 800 e C and 1 ,000 e C.
  • the reduction process is carried out in a first chamber exposed to the oxidation process.
  • the oxidation process is carried out in a second chamber, the first chamber being located at least partly within the second chamber. In another embodiment, the first chamber being located within the second chamber.
  • the oxygen depleted air from the oxidation process is passed through a heat exchanger to transfer heat to an incoming gas added to the oxidation process.
  • the oxygen enriched mixture from the reduction process is passed through a heat exchanger to transfer heat to a fuel for the reduction process.
  • a fluid medium is passed through a heat exchanger to receive heat from the chemical looping process and drive a turbine. More preferably, the fluid medium comprises water and steam is generated to drive the turbine to generate electricity. Alternatively, the fluid medium is directed to a temperature control system for heating or cooling.
  • the oxygen separated from the oxygen enriched mixture is transferred to an oxygen consumption unit.
  • the oxygen carrier particles comprise metal oxides. More preferably, the metal oxides comprise at least one of Cu, Mn and Co based metal oxides. In one embodiment, the metal oxides comprise mono-bi-metallic oxide sorbents or composites, such as perovkites and the like. In other embodiments, the metal oxides are selected from the group comprising Mn0 2 , Mn 2 0 3 , Mn 3 0 4 , CoO, Co 3 0 4 , CuO, Cu 2 0 and mixed metal oxides.
  • a third aspect of the invention provides a system for generating oxygen and storing energy, the system comprising the apparatus of the first aspect and an oxygen separating unit for separating oxygen from the oxygen enriched mixture.
  • the system further comprises the oxygen storage unit fluidly connected to the oxygen separating unit.
  • the oxygen storage unit controllably releases oxygen.
  • the oxygen storage unit has a valve to controllably release oxygen.
  • the oxygen separating unit comprises a condenser for condensing the oxygen-enriched mixture to separate the oxygen, the condenser being fluidly connected to the outlet conduit.
  • the system further comprises a compressor for compressing the oxygen, the compressor being fluidly connected to the condenser.
  • the oxygen separating unit comprises a heat exchanger for exchanging heat between the oxygen-enriched mixture and incoming gas into the reduction reactor.
  • the system comprises a heat exchanger for exchanging heat between air from an air supply and oxygen depleted air from the oxidation reactor.
  • the combustion unit combusts coal in a coal-fired power plant.
  • the combustion unit comprises a furnace. In other embodiments, the combustion unit comprises a boiler.
  • Figure 1 is a schematic drawing of an apparatus and system for energy conversion or storage and oxygen production according to one embodiment of the invention
  • Figure 2 is a schematic drawing of the apparatus of Figure 1 in a RES configuration
  • Figure 3 is a schematic drawing of a process simulation of the RES
  • Figure 4 is a schematic drawing of another process simulation of the RES configuration of Figure 2;
  • Figure 5 is a schematic drawing of a further process simulation of the RES configuration of Figure 2;
  • Figure 6 is a schematic drawing of the apparatus of Figure 1 in an alternative RES configuration
  • Figure 7 is a graph of expander power production minus compressor power consumption against the compressor outlet pressure for RES unit of Figure 6;
  • Figure 8 is a graph comparing the net present values off the RES units of Figures 2 and 6 with conventional and advanced CASU units against the cost of oxygen.
  • the embodiments of the invention are in general directed to a RES system and in particular to providing a chemical looping energy on demand system (CLES), which is a technology for poly-generation of power, heating, cooling, hot water, oxygen and hydrogen.
  • CLES chemical looping energy on demand system
  • the CLES technology has been developed for use in a diverse range of applications such as:
  • CLAS chemical looping air separation
  • the oxidation half-cycle is typically carried out under normal air whilst the reduction half-cycle is usually accomplished in the presence of steam.
  • the energy input to the CLES is primarily used to support the endothermic reduction phase of the redox reaction while the hot gases generated during the oxidation phase are expanded through a power turbine-generator set for production of electricity.
  • the waste heat from the exhaust of the turbine is used to produce other products (heat, hot water, cooling using an absorption chiller, hydrogen through either electrolysis of chemical reactions).
  • the energy on demand mode the energy input from natural gas (or diesel fuel, bio-diesel, or similar fuels) is converted to power, heating, cooling, hot water, oxygen and hydrogen on a continuous basis.
  • natural gas or diesel fuel, bio-diesel, or similar fuels
  • the use of natural gas is preferred as it has one third of greenhouse gas emissions when compared with other types of solid fuels like coal.
  • the CLES technology operates in a batch mode whereby the off-peak and hence cheap electricity (from renewable sources such as wind or solar or from conventional power plants) is used during off-peak hours to carry out the reduction of the metal oxide particles. During this endothermic process oxygen is produced which can be either stored or utilised.
  • the apparatus 1 comprises a reduction reactor 2 and an oxidation reactor 3 fluidly connected so that oxygen carrier particles 4a, 4b (in this embodiment in the form of metal oxide particles) can be transferred between the reactors 2, 3.
  • An outlet conduit 5 is arranged transfer an oxygen-enriched mixture from the reduction reactor 2 to an oxygen storage unit 6.
  • Both the reduction reactor 2 and the oxidation reactor 3 are fluidised bed reactors.
  • the reduction reactor 2 and the oxidation reactor 3 can be any other type of chemical reactor, such as a fixed-bed or spouted-bed reactor.
  • the reduction reactor 2 is located within the oxidation reactor 3. That is, the reduction reactor 2 is contained within or inside the oxidation reactor 3. However, it will be appreciated that in other embodiments, the reduction reactor 2 may be located partly within the oxidation reactor 3. Also, in the present embodiment, the reduction reactor 2 is substantially smaller in size than the oxidation reactor 3. In any event, this "twin reactor" configuration is a unique design developed by the inventors.
  • the reduction and oxidation reactors 2, 3 are fluidly connected by an inlet conduit 7 and an outlet conduit 8.
  • the inlet conduit 7 transfers the oxygen carrier particles 4a from the oxidation reactor 3 to the interior of the reduction reactor 2, where they undergo a reduction reaction to release or generate oxygen, as described in more detail below.
  • the outlet conduit 8 transfers oxygen-depleted carrier particles 4b from the reduction reactor 2 to the oxidation reactor 3 and are replenished with oxygen in the oxidation reaction and ready to be transferred to the reduction reactor 2.
  • the reduction reactor 2 is embedded in the bed 9 of the oxidation reactor 3. By this configuration, an outer surface 10 of the reduction reactor 2 is maintained at a temperature almost the same as that of the bed temperature of the oxidation reactor 3. This arrangement minimises the overall heat losses and as such leads to higher overall thermal efficiencies. Given its high temperature, the outer surface of the reduction reactor 2 becomes very critical in maintaining the correct temperature gradient and thus driving force for the reduction reaction.
  • the reduction reactor 2 may be located adjacent to or partly within the bed of the oxidation reactor 3, instead of within the bed.
  • the apparatus 1 in Figure 1 is incorporated into a system 20 for generating oxygen and storing energy.
  • the system 10 comprises a conduit 21 that delivers water from a condenser 22 and a pump 23 (as well as an optional water supply 24 to provide additional made up water) to a heat exchanger 25 to generate steam that is then delivered by conduit 26 as a gas stream into the reduction reactor 2.
  • the reduction reactor outlet 5 transfers an oxygen-enriched gas mixture produced by the reduction reaction in the reduction reactor 2 to the heat exchanger 25 to provide the heat that generates the steam.
  • the now cooler oxygen-enriched gas mixture passes to the condenser 22 via a conduit 27, where oxygen is remove and transferred by the conduit 28 to the oxygen storage unit 6 for future use as oxygen or to generate energy.
  • the heat generated during the oxidation of the metal oxides in the oxidation reactor 3 is completely extracted by the inlet air flow and is transferred to another heat exchanger 30 via a conduit 31 .
  • the cooler gases then pass to a cooler unit 32 via a conduit 33 before being exhausted out of a discharge line 34.
  • a water supply line 35 may be used to heat water in the cooler unit 32, which can then be used for various purposes via a conduit 36.
  • Air is also from an air supply (not shown) can be delivered by a pump 37 via and a conduit 37 to the heat exchanger 30 to preheat and compress the air.
  • a conduit 39 takes the preheated compressed hot air to a booster 40 where it is superheated to a high temperature before entering into a turbine (in this embodiment, an indirectly fired gas turbine, such as a hot air turbine 42) via a conduit 43 for the purpose of increasing power generation efficiency.
  • the superheated air expands through the turbine 42 and produces both heat and power.
  • the waste gas from the turbine 42 is then taken by a conduit 44 to the cooler unit 32 and/or to the oxidation reactor 3 to fuel the oxidation reaction.
  • the system 20 involves metal oxide oxygen carrier particles 4a, 4b being continuously circulated between the oxidation reactor 3 and the reduction reactor 2.
  • the metal oxide particles 4b undergo reduction reaction at temperatures about 950 e C in the presence of a sweep gas (steam in this case) and produces oxygen-enriched gas mixture.
  • the reduction reactor 2 is indirectly heated either by combustion of a fuel such as natural gas or diesel in the energy on demand mode or by electrical heating (joule heating) in the energy storage mode. The same energy sources are used to generate the required quantities of steam from the water derived from the condenser 22.
  • the oxygen-enriched stream passes through the heat exchanger 25 so that the heat content of the gases can be recycled for preheating the inlet stream of steam entering the heat exchanger 25 via the conduit 21 .
  • Pure oxygen is then produced and stored by further condensing the oxygen-enriched stream in the condenser 22 and the later compressed in an oxygen compressor (not shown) before being stored in the oxygen storage tank 6.
  • the condensate from the condenser 22 is recycled back to the reduction loop via the pump 24 so that the water usage in the system 20 (as part of a power plant) can be kept at minimum.
  • the reduced metal oxide oxygen carrier particles then pass from the reduction reactor 2 via the outlet conduit 8 and on the way to the oxidation reactor 3 are oxidised in the presence of the exhaust air exiting the hot air turbine 42 incoming via the conduit 44.
  • the makeup water from the water supply 23 may be needed in the condenser 22 with possible blow-off being discharged via a line 45 to a drain system (not shown).
  • a drain system not shown
  • the combustion product gas from the turbine 42 and the reduced air exiting the oxidation reactor 3 are joined together via conduits 33 and 44 and enter the cooler unit 32. Waste heat can be recycled from these exhaust gas streams in the cooler unit as discussed above and used for HVAC applications.
  • additional energy inputs 50, 51 , 52 may also be provided to the oxidation reactor 3, reduction reactor 2 and the booster 40, respectively, to assist in supplying sufficient energy/heat to drive the oxidation, reduction and superheating processes.
  • the arrangement of the reduction reactor 2 inside the oxidation reactor 3 ensures that the heat generated from the oxidation reaction in the oxidation reactor 3 maintains the reduction reactor 2 at a higher temperature than the oxidation reactor 3 due to the additional supply of heat from the incoming steam from the conduit 26.
  • the arrangement of the reduction reactor 2 inside the oxidation reactor 3 ensures that the heat generated from the oxidation reaction in the oxidation reactor 3 maintains the reduction reactor 2 at a higher temperature than the oxidation reactor 3 due to the additional supply of heat from the incoming steam from the conduit 26.
  • the CLES system is able to reallocate excess power at off-peak hours for the use in peak-hours period by its storage feature.
  • the reduction reactor 2 and the oxidation reactor 3 function independently in a batch operation mode.
  • the power at off-peak time heats both the reduction reactor 2 and the oxidation reactor 3 to desired temperature levels; an adequate temperature in the reduction reactor 2 for facilitating the oxygen release and a suitable bed temperature retained for the oxidation reactor 3.
  • the oxidation reactor 3 is maintained at a temperature as low as the oxidation reaction of oxygen carrier particles is restricted or hardly occurs by a small amount of power from off peak hours.
  • the oxygen carrier particles are intermittently exchanged between the reduction reactor 2 and the oxidation reactor 3. All the solid particles in the reduction reactor 2 undergoes the reduction reaction to release oxygen until completion, during which no exchange of oxygen carrier particles occurs between the reduction reactor 2 and the oxidation reactor 3. Subsequent discharge of the reduced particles from the reduction reactor 2 to the oxidation reactor 3 is
  • the bed temperature of oxidation reactor 3 in the CLES system is slightly elevated to stimulate the oxidation reaction, and once oxidation has started, a significant amount of heat will be released for power generation to meet the incremental demand of electricity.
  • the oxidation reactor 3 in comparison to the reduction reactor 2 for a few reduction steps could proceed during off-peak period whereas only one oxidation step can be achieved during peak hours.
  • the benefit of the design using the reduction reactor at least partly (and preferably fully) within the oxidation reactor is that there is a minimisation of the system heat loss and a maximisation of the efficiency of the redox reaction.
  • the reaction thermodynamics at equilibrium the oxygen partial pressure is higher at high temperatures. Hence, larger quantities of oxygen can be stripped from normal air (with an oxygen partial pressure of 0.21 ) if the oxidation reaction is carried out at lower temperatures.
  • larger quantities of oxygen can be released by the metal oxide particles. In the embodiment of the invention this is achieved by placing the reduction reactor 2 within the oxidation reactor 3 to achieve these higher temperatures. More importantly, a much lower quantity of steam (and hence, a substantial reduction in input energy) is required for the reduction reaction, allowing much smaller reduction reactors to be used, which in turn lowers the cost in capital expenditure and maintenance.
  • temperatures during the redox reaction inspired the inventors to design the process in which the reduction reaction is carried out at temperatures higher than those for oxidation reaction. Preferably, these temperatures are about 100 e C to 150 e C higher than the oxidation reaction temperature. This unique approach is quite different from conventional redox based chemical looping air separation methods where oxidation temperature is always maintained at higher levels than reduction temperatures.
  • Oxygen as a key component in the basic oxygen furnace for steel production, is currently produced from cryogenic air separation unit (CASU) in large quantity, which is an energy intensive process (0.43 kWh/Nm 3 ).
  • CASU cryogenic air separation unit
  • the oxygen usage in the basic oxygen furnace was estimated to be 50 Nm 3 per tonne of steel production.
  • the annual oxygen requirement can be greater than 44 million Nm 3 , which requires greater than 19 million kWh of electricity per year (or ⁇ $4 million/year of electricity).
  • the embodiment of the invention may be employed as a less energy intensive option for oxygen production in order to reduce the energy penalty associated with plant oxygen demand.
  • the CLES system and, in particular, the apparatus 1 is adapted for use in a RES configuration (which for ease of convenience will be referred to as a RES unit 100), which acts as an energy storage facility to help balance the electricity/thermal consumption and demand of the steelmaking plant.
  • the REST unit 100 comprises the apparatus 1 (taking the form of the twin reactor 102 having the reduction reactor inside the oxidation reactor as described above) fluidly connected to heat exchangers 103, 104, a condenser 105 and a steam turbine 106 (instead of an indirectly fired gas turbine).
  • a reduction loop 1 10 is formed by a conduit 1 1 1 connecting the twin reactor 102 to the heat exchanger 4 and condenser 5, and a conduit 12 connected the apparatus 1 to an input gas supply 13 described in more detail below.
  • An oxidation loop 1 15 is formed by a conduit 1 16 connecting the twin reactor 102 to the heat exchanger 103 and an air supply 1 17, and a conduit 1 18 connecting the twin reactor 102 to a discharge conduit 1 19.
  • Valves 120, 121 close off the reduction loop 1 10 from the twin reactor 102 while valves 122, 123 close off the oxidation loop 1 15 from the twin reactor 102.
  • the twin reactor 102 can be operated to performed oxidation or reduction separately.
  • the oxidation process is performed continuously whenever the oxidation loop 1 15 formed or opened and the reduction loop 1 10 is closed off.
  • the reduction process is performed continuously whenever the reduction loop 1 10 is opened and the oxidation loop 1 15 is closed off.
  • the reduction loop 1 10 is formed by closing valves 122, 123 to seal off the oxidation loop 1 15 and opening valves 120, 121 to enable gas to flow through the conduits 1 1 1 , 1 12.
  • the reduction loop 1 10 is operated during the off-peak hours of electricity usage (i.e. at night time), where the metal oxide oxygen carrier particles in the fluidised bed of the twin reactor 102 undergo a reduction reaction in the presence of the input gas, which in this case is a sweep gas added via the conduit 1 13 from the gas source supply 1 12.
  • the sweep gas in this case is H 2 0, but in other embodiments, the sweep gas can be any inert gas (examples may include C0 2 , argon or helium) that can be easily separated by membrane or any separation method after the reduction step to produce pure oxygen stream.
  • the reduction process consumes relatively cheap electricity (or thermal energy originating from carbon-based fuels) using an electric heater or boiler and produces an oxygen-enriched stream primarily containing oxygen and water that passes from the twin reactor 102 through the conduit 1 1 1 and valve 121 to the heat exchanger 104. In the heat exchanger 104, waste heat from the stream is recycled to preheat the incoming water before it is fed into the twin reactor 102.
  • the produced oxygen is purified from the oxygen-enriched stream by the condenser 5, which condenses the oxygen-enriched stream to separate oxygen from water and thus producing pure oxygen.
  • the pure oxygen is then sent for downstream use and/or storage.
  • the condensate comprising mostly of water is then recycled from the condenser 105 via a conduit 130 back to the reduction loop 1 10 by joining the incoming water in the conduit 1 12, through the valve 120 and heat exchanger 104, and then to the twin reactor 102.
  • the RES unit 1 00 is then moved to the oxidation process by closing the valves 1 20, 121 and opening valves 122, 1 23 to form the oxidation loop 1 1 5.
  • the oxidation process in the oxidation loop 1 1 5 is performed during the peak hours (i.e. at day time), where the reduced metal oxide oxygen carrier particles in the fluidised bed 109 are now oxidised in the presence of air which is introduced by the valve 122 from the air supply 1 17.
  • the air is preheated by a waste stream conveyed by the discharge conduit 1 19 via the heat exchanger 103.
  • the oxidation process in the twin reactor 102 generates heat that can be extracted by different ways such as gas (steam or air), liquid (organic or inorganic) and solids (sand or ceramic).
  • heat is extracted by using a separate conduit 135 carrying water from a water supply 138 to embedded water tubes (not shown) in the twin reactor 102 to produce hot water or steam for heat and/or power generation purposes.
  • the hot water or steam is directed to the turbine 106 via a conduit 140 to produce electricity.
  • the oxygen depleted air (also called reduced air) comprising mostly of nitrogen N 2 is removed from the twin reactor 102 as the waste stream via the discharge conduit 1 19.
  • the waste stream passes through the heat exchanger 1 03 to preheat the incoming air and then is discharged to the ambient environment through an outlet 145.
  • the method and apparatus 1 or twin reactor 102 may use different oxygen carrier particles for oxygen production, such as ⁇ 2 ⁇ 2 ⁇ 3,
  • the process uses a variety of other suitable oxygen carrier particles.
  • the RES unit 170 used C0O/C03O4 and CuO/Cu 2 0 as the oxygen carrier particles due to their high oxygen transport capacity (OTC) and reactivity.
  • OTC oxygen transport capacity
  • the RES unit 100 does not require external heating since the heat produced in the oxidation reactor 3 is usually sufficient to provide the necessary heat required in the reduction reactor 2.
  • NGCC Natural gas combined cycle
  • RES unit 100 The integration between a RES unit 100 and an integrated steelmaking plant can become quite mutually beneficial.
  • oxygen, steam, heat, and electricity (90% derived from coal, excluding oxygen) are being used in the integrated steelmaking plant.
  • the RES process has the ability to deliver all of these energy and gas products.
  • the significant amount of heat demand in the reduction reactor of the RES unit 100 can be supplemented by direct/indirect firing of either on-site coal, natural gas, or the waste gases of the steelmaking process (e.g. COG and BFG).
  • the low-cost off-peak electricity can also be used for this purpose via joule heating.
  • the energy contained in the above forms can be said to be temporarily stored in the reduction reactor 2 of the twin reactor 102. This energy can then be released from the oxidation reactor 3 whenever they are required.
  • Such an energy storage concept is also applicable to many other industrial processes where energy storage is found advantageous, such as coal plants, solar plants and wind farms.
  • the RES unit 100 When joule heating is employed using the low-cost and sometimes wasted off- peak electricity, the RES unit 100 then acts as an off-peak electricity storage "tank" to absorb as much off-peak electricity generation as possible from coal-fired power plants. This can be quite beneficial for the coal-fired power plants as it allows them to run more frequently on full loads with greater generation efficiency.
  • coal-fired power plants are normally operating at partial loads during low demand periods, which is highly inefficient and contributes to a great amount of greenhouse gas emissions.
  • the stored low-cost off-peak electricity can be regenerated for on-site uses during the peak periods when the electricity price is doubled or even tripled. This concept, however, suffers from potentially significant energy losses during the electricity regeneration process, namely -2/3 losses during the heat-to-electricity conversion.
  • the heat released from the RES unit 100 could be used to either generate steam via the existing boiler to offset the plant steam usage, or provide heat for numerous on-site heating purposes, e.g. furnace preheating, reheating of steel, reheating of fuel before entering to a hot stove, heating of facilities and etc.
  • the produced steam can be used for the treatment of semi-finished products, powering pump/compressors, facility heating, and electricity generation.
  • the energy for steam production in an integrated steelmaking plant has been estimated to be up to 10% of the total energy consumption.
  • the generated electricity can be used for producing compressed air, pumping, rolling steel, rolling mills, driving conveyors and fans, and powering materials handling equipment and other ancillary processes. It has been estimated that 13% of the energy consumption in iron and steel making process was in the form of electricity, the production of which accounted for an even higher percentage (-33%) of the total raw energy and fuel usage. Therefore, using a RES process to simultaneously produce oxygen, steam, heat, and electricity is expected to generate great synergies, reducing energy intensity and providing cost benefits for the iron and steel industry.
  • FIG. 3 shows the overall processes involved with the intermittent operational mode, where the CLAS process 150 receives air and water as inputs 152 and produces reduced (oxygen depleted) air 153 and an oxygen enriched stream 155 that passes through two cooling stages 156, 157 (to exchange heat with the incoming air and water) before undergoing oxygen separation at 160.
  • the pure oxygen produced at 163 is then sent for use in either industrial or medical applications while the water that remains is recycled at 165.
  • FIG. 4 another exemplary RES unit 170 is illustrated and comprises the twin reactor 102 schematically illustrated for clarity as separate reduction and oxidation reactors 172, 173.
  • air from the air supply 1 17 is passed through an air compressor 168 before entering the oxidation reactor 173 and then the oxygen depleted air passes through a booster 166 and a hot air turbine 167 before being discharged via outlet 145.
  • air from the air supply 1 17 is passed through an air blower 180 before passing through the heat exchanger 103 for preheating before entering the oxidation reactor 173 and oxygen depleted air is then removed via outlet 145.
  • the reduction loop 1 10 involves the water being pumped into the reactor 172 via a pump 175 from a water supply source 177 and heat exchangers 179 being used to generate steam from the oxygen enriched stream 155 for power generation prior to being sent to the condenser or other oxygen separation unit.
  • the RES unit 170 has the mineral/metal oxide particles transferred between the reduction and oxidation reactors 172, 173.
  • the reactors 172, 173 are connected to pass the oxygen carrier particles as described above between each other to create the chemical looping process.
  • the RES unit 170 was simulated to operate the oxidation reactor 173 and reduction reactor 172 intermittently during peak and off-peak periods, respectively. In this mode, no oxygen but only electricity is produced during the peak period. That is, during the period in which the oxidation process is performed, no oxygen is produced by the oxidation reactor 173 in the RES unit 170. Rather, only electricity is generated with the oxidation process enriches the oxygen-depleted carrier particles with oxygen for subsequent use in the reduction process.
  • the intermittent operation of the RES unit 70 would require at least 2.7 standard RES units to be built and operating during the 9 hour off-peak period (approximately from 10pm to 7am in the night phase) to be able to produce enough oxygen (i.e. a total of 120,000 m 3 ) for a full day load.
  • 45,000m 3 is consumed during the same off-peak period while the rest (being 75,000m 3 ) is stored in an oxygen tank (such as the tank 6 of Figure 1 ) and consumed during the next 15-hour peak period (during the day phase), all at a constant consumption rate of 5,000 m 3 /hr. It is contemplated that this arrangement of 2.7 standard RES units is capable of meeting the oxygen requirements of a steelmaking plant for producing 1 00 tonnes per hour of steel.
  • Table 2 shows the operating conditions, material requirements, energy demands, and energy and oxygen production for the standard RES unit 170 using CuO as the oxygen carrier particles. These parameters are shown for three different reduction reaction temperatures, namely 1040°C, 1077°C, and 1 102°C, which correspond to low (25%), medium (50%), and high (75%) levels of oxygen partial pressures of the product stream (i.e. the oxygen enriched stream). It can be seen in Table 2 that as the oxygen partial pressure increases from 25% to 75% the minimum water requirement of the RES process is reduced significantly from 10,300 kg/hr to 1 ,200 kg/hr (or by 88%).
  • the oxygen production of the process was found to be around 5,000 m 3 /hr with an oxygen purity of 96% before the oxygen compression process.
  • the oxygen purity can be increased further to 99.9% depending on the targeted applications by further compressing the gases, enhancing the oxygen-water separation process and other oxygen purification processes.
  • Table 3 gives the main technical analysis results for the standard RES unit 170 using CoO as the oxygen carrier particles.
  • the analysis was performed for the same levels of oxygen partial pressures as those in Table 2 above but at lower temperatures, namely 894°C, 913°C, and 925°C. From Table 3, it can be seen that the minimum water and air requirements as well as the later cooling demand requirements for oxygen-water separation are almost the same as those of the copper case in Table 2 above. This is because that the two cases share the same oxygen production rate and same oxygen partial pressure in the production (oxygen enriched) stream. However, the minimum required inventory of cobalt oxide is 51 % greater than that of copper oxide given the same oxygen production capacity. The heating demand of the reduction reaction for the cobalt oxide oxygen carrier particles was also found to be greater than that of the copper oxide oxygen carrier particles.
  • a specific power demand of the RES unit 170 of about 0.08 kWh/m 3 was found consistent for all examined scenarios after taking into account the electrical energy demand, the recoverable energy production, and any energy losses of the process. This number represents a significant energy discount at about 81 - 92% when compared with the typical specific power demands of large CASU units at 0.43-0.55 kWh/m 3 of oxygen and small-medium scale PSA processes at 0.8-1 kWh/m 3 of oxygen.
  • Table 4 Overall performance comparison of the standard RES units using CuO and CoO as the oxygen carrier particles.
  • the low-grade, medium-grade, and high-grade heat refers to heat produced at temperatures ⁇ 100°C, 100°C - 600°C, and >600°C, respectively in general.
  • the indirect heating approach may be more appropriate for the current application, which uses solid/gaseous fuels as the indirect heating source for the reduction reaction without contaminating the oxygen product.
  • high purity oxygen product can be produced for direct uses in the basic oxygen furnace.
  • Table 5 shows the calculated requirements of coal, coke, COG, BFG, and natural gas if the RES unit 170 uses one of them as a supplementary indirect heating source.
  • Table 5 Individual fuel requirements of the standard RES units using CuO and CoO as the oxygen carrier particles based on a 100 tonne/hour steel making plant.
  • BFG alone may not be a suitable option for supplying heat for the reduction reactor due to its low flame temperature.
  • BFG can be better used by blending with other higher quality gases (e.g. COG/natural gas).
  • the intermittent operation of the RES unit 170 would require at least -2.7 standard units to be built.
  • Table 6 gives the performance of the 2.7 standard RES units for both the peak and off-peak periods.
  • the total electrical energy demands of these RES units using Cu-based oxygen carriers were found to be 321 -445 MWh (or 518-654 MWh for the CoO case) during the oxygen production period depending on the reduction reactor temperature.
  • This electrical energy could then be recovered during the peak period in the forms of low, medium, and, high-grade heat, of which the high-grade heat is converted into electricity and the rest can be used for heating/steam generation.
  • the oxygen being produced during the off-peak period at 120,000 m 3 can be consumed at a constant rate of 5000 m 3 /hr for both the peak and off-peak period via the use of an oxygen storage tank.
  • the low-grade, medium-grade, and high-grade heat refers to heat produced at temperatures ⁇ 100°C, 100°C - 600°C, and >600°C, respectively in general.
  • a hot air turbine can be implemented in the oxidation loop of the RES unit 170, as best shown in Figure 6.
  • This configuration is believed to improve the energy efficiency of the RES process.
  • the improvement or modification was made primarily in the oxidation loop 1 15, in which an air compressor 190 is added to compress the inlet air.
  • the compressed air then passed through the fluidised bed to be heated to a high temperature and exits as a depleted air.
  • An air expander 192 is added to the process for expanding the high -temperature and high- pressure depleted air and generating electricity. Part of the produced electricity can be used to drive the new compressor via a connecting rotating shaft 195.
  • the above concept mimics the operation of a gas turbine unit but differs in that (i) the compressed air is heated by reaction heat instead of a gaseous fuel, and (ii) reduced air is used in the expansion process rather than normal air. Such a modification is expected to yield more power generation than that could be produced from the unmodified RES process.
  • Table 7 sets out the possible changes of heat/power generation profile of the RES process (mainly the oxidation loop) due to the modification.
  • Table 7 Main changes of the heat/power profile of the oxidation loop due to the modification (for a standard RES unit using Cu-based oxygen carriers based on a 100 tonne/hour steel making plant).
  • a preliminary techno-economic feasibility of the RES unit 170 was assessed for a large-scale steelmaking plant of ⁇ 0.8 million tonnes per year. The cost was estimated based on the experience of a similar-scale RES unit that was constructed recently with an expected accuracy at -20% and + 20%. The hypothetical plant was assumed to have a continuous oxygen demand of 5,000 m 3 /h, which requires one standard RES unit under the continuous production mode or 2.7 RES units under the intermittent production mode.
  • Table 8 below shows the reactor parameters estimated according to the capacity of the RES unit 170 operating under the continuous production mode. It shows that the reduction reactor is much smaller than the oxidation reactor due to the lower gas flow rate.
  • Table 9 sets out preliminary reactor cost estimates for the RES unit 170 operating in both the intermittent and continuous production modes.
  • Table 9 Reactor cost estimates based on the fabrication costs of a similar- sized RES unit that was constructed recently Cost items Continuous production
  • Air flow -7.5 m 3 /s; pressure rise: 25 kPa; Power demand: 230 kW.
  • Table 10 sets out the capital cost of the RES unit 170 operating under the two production modes, compared with that of a CASU of the similar capacity.
  • the payback time of the total initial investment for RES unit 170 was found to vary between 1 .4 to 2.0 years without considering the cost saving from onsite oxygen production and merely 0.15 to 0.155 years if we consider the cost saving due to onsite oxygen production as a revenue (see Table 1 1 below). In contrast, the payback time of using CASU for oxygen production was found to be longer, at 0.57 to 0.60 year. Table 1 1 : Economic analysis of RES unit
  • the produced power at 88,800 kWh/day represents -5% of the average electricity
  • W c , RES, OP and W P denotes the amount of electricity being consumed during the off-peak period and that being produced during the peak period for the RES unit, respectively;
  • CoE op and CoE p denotes the electricity costs during the off-peak and peak time, respectively;
  • W c , CASU, OP and W c , CASU, P denotes the amount of electricity being consumed during the off-peak and peak periods for the CASU unit, respectively.
  • WCASU denotes the oxygen production cost of the CASU unit in terms of kWh per tonne of oxygen.
  • Figure 8 shows the net present value of the RES unit compared to those of the conventional and advanced CASU units as a function of the cost of oxygen in cylinders. As it shows, at a high market cost of oxygen in cylinders (AUD 1 .28/m 3 and AUD
  • the scenario of AUD 0.64/m 3 refers to a 50% discount of the off-site purchase cost of oxygen in cylinders assuming the steel making plant made a long-term contract with the gas company.
  • the scenario of AUD 0/m 3 refers to the case that the cost saving due to the shift from off-site purchase to on-site oxygen production is excluded, and thus the NPV results correspond to the present value of the cumulative future payments for on-site oxygen production.
  • This amount for the RES unit 170 was found to be AUD 35 million and AUD 14 million less than those of the conventional and advanced CASU cases, respectively. In other words, the RES unit 170 can help save AUD 14 to 35 million in terms of oxygen production cost over the examined plant lifetime.
  • the RES unit 170 provides a cheaper option than CASU and helps saving millions of dollars for the industry.
  • Table 12 Cost saving of oxygen production in AUD million due to the employment of RES unit as opposed to the conventional CASU technology for a range of peak and off-peak electricity prices
  • the RES process when operating in the continuous production mode, was more economically attractive than the conventional CASU process, leading to an increased net present value by 7 to 1 1 % and a shortened payback period by 2.4 to 2.8 times.
  • the RES process when operating in the intermittent production mode, requires the ratio between the peak and off-peak electricity prices to be greater than 2.38 - 2.80 for it to become economically superior to CASU processes.
  • embodiments of the invention can be combined together and are not necessarily applied in isolation from each other.
  • the feature of a partly embedded reduction reactor in the oxidation reactor can be used instead of the fully embedded reduction reactor in the RES unit 170.
  • Similar combinations of two or more features from the above described embodiments or preferred forms of the invention can be readily made by one skilled in the art.
  • the invention By providing a unique reactor configuration of a reduction reactor at least partly within the oxidation reactor, the invention confers the advantages of being able to maintain the reduction reactor at a consistently higher temperature than the oxidation reactor. This in turn minimises heat loss, improving the efficiency of the redox reaction, further enhances the production of oxygen and reduces the amount of incoming steam to fuel the reduction reaction. All these advantages of the invention result in lower costs in capital expenditure and maintenance. Furthermore, since smaller reduction reactors are used that are at least partly within or fully within the oxidation reactor, the invention can be readily implemented to existing plants by replacing single reactors with the reactor configuration of the embodiments of the present invention. In all these respects, the invention represents a practical and commercially significant improvement over the prior art. [001 15] Although the invention has been described with reference to specific examples, it will be appreciated by those skilled in the art that the invention may be embodied in many other forms.

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Abstract

Un appareil (1) pour générer de l'oxygène comprend un réacteur de réduction (2) en communication fluidique avec et situé au moins partiellement à l'intérieur d'un réacteur d'oxydation (3), où des particules porteuses d'oxygène (4a, 4b) sont transférées entre les réacteurs de réduction et d'oxydation. Un conduit de sortie (5) transfère un mélange enrichi en oxygène du réacteur de réduction à une unité de stockage d'oxygène (6). Une méthode correspondante fournit un procédé de boucle chimique utilisant des particules porteuses d'oxygène transférées entre des processus de réduction et d'oxydation, où des particules porteuses appauvries en oxygène produites dans le processus de réduction sont transférées au et régénérées dans le processus d'oxydation. L'oxygène est séparé d'un mélange de gaz d'échappement produit dans le processus de réduction. Le processus de réduction est effectué à une température plus élevée que le processus d'oxydation. Un système (20) utilise l'appareil et un condenseur (22) pour condenser le mélange enrichi en oxygène à partir du conduit de sortie (6).
PCT/AU2018/050645 2017-06-27 2018-06-26 Appareil et méthode de génération d'oxygène et de conversion ou de stockage d'énergie Ceased WO2019000030A1 (fr)

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CN111747379A (zh) * 2020-06-29 2020-10-09 东北大学 一种基于太阳能光热的化学链连续制氧系统及方法
CN114588856A (zh) * 2022-03-24 2022-06-07 北京理工大学 一种耦合化学链循环的太阳能热化学制备燃料系统及方法
CN114623431A (zh) * 2022-03-21 2022-06-14 浙江大学 稳燃调峰系统及稳燃调峰方法
CN119253870A (zh) * 2024-09-27 2025-01-03 东南大学 一种太阳能辅助的化学链热泵储电系统

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WO2013040645A1 (fr) * 2011-09-23 2013-03-28 Newcastle Innovation Limited Séparation d'air en boucle chimique intégrée dans des centrales à oxygaz à grande échelle
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WO2013040645A1 (fr) * 2011-09-23 2013-03-28 Newcastle Innovation Limited Séparation d'air en boucle chimique intégrée dans des centrales à oxygaz à grande échelle
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Publication number Priority date Publication date Assignee Title
CN111747379A (zh) * 2020-06-29 2020-10-09 东北大学 一种基于太阳能光热的化学链连续制氧系统及方法
CN111747379B (zh) * 2020-06-29 2023-02-24 东北大学 一种基于太阳能光热的化学链连续制氧系统及方法
CN114623431A (zh) * 2022-03-21 2022-06-14 浙江大学 稳燃调峰系统及稳燃调峰方法
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