Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
DETAILED ACTION
Response to Arguments
Applicant's arguments filed 2/9/2026 have been fully considered but they are not persuasive.
Regarding the applicant’s argument that Johnson does not teach wherein an active solid particle terminal velocity is within 10% of an inert solid particle terminal velocity, the examiner disagrees. Johnson states “In the preferred form of this invention, the powdered mass is maintained in a reactor substantially larger than the volume occupied by the mass itself in the fluidized condition” (column 3, line 43 emphasis added). This suggests that the whole powdered mass is fluidized together and must therefore have a substantially similar terminal velocity. If the terminal velocities of the particles were too different, some of the mass would be fluidized and some of the mass would be carried away by the fluidizing fluid and thus not maintained in the reactor.
Regarding the applicant’s argument regarding the use of In re Aller, the examiner points out that the cited text from the cited case law appears to be directed to the assumption of obviousness in overlapping ranges and not routine optimization. The applicant additionally argues that Johnson does not teach that including distinct inert particles would impact operation of the reactor system. The examiner disagrees. Johnson states “It may also be desirable to maintain the metal oxide on a suitable inert material as a support or carrier, or it may be desirable to have such inert material present in the reaction zone itself as separate particles from the oxides of manganese, as a diluent. This inert material may serve as a heat carrier and also may serve in aiding in the suspension and fluidization of the metal oxide” (column 4, line 70). Therefore, including the inert particles effects the result of aiding in suspension and fluidization.
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claims 1-6, 8, 9, 13, 15, 16, and 18-20 are rejected under 35 U.S.C. 103 as being unpatentable over Lewis (US 2607670 A), hereinafter Lewis, in view of Johnson (US 2656255 A), hereinafter Johnson.
Regarding claims 1 and 8, Lewis discloses a chemical looping system, comprising:
a reducer reactor including active solid particles (“In operation, hydrocarbon oxidizer 10 contains a dense bed 12 of titanium dioxide having a particle size of about 200-300 mesh fluidized” column 4, line 32 and “Returning new to oxidizer 10, a partially converted product gas which may still contain up to about 10% or more of unconverted methane is withdrawn from level L10 and passed substantially at the temperature and pressure of oxidizer 10 through line 48 to cleanup oxidizer 50” column 5, line 30),
wherein the active solid particles include a metal oxide (“While certain metal oxides which are reduced to metals such as ferrous oxide, cuprous oxide, and the like, are useful for the process, other suitable oxides are the higher oxides of metals which are capable of forming both higher and lower oxides. Typical for the latter oxides are ferric oxide, cupric oxide, vanadium pentoxide, stannic oxide, titanium dioxide, various manganese oxides and mixtures of these oxides. The oxides of titanium, preferably those promoted with a composite containing a major proportion of iron oxide and minor proportions of nickel oxide and chromium oxide are of particular advantage for the present invention because they have been found to possess satisfactory activity and selectivity to form CO and H2” column 3, line 55);
wherein the active solid particles are capable of cycling between a reduction reaction and an oxidation reaction (“reduced metal oxide is withdrawn from said conversion zone, regenerated with air in the form of a dense, turbulent, fluidized mass of solids in a regeneration zone at an oxidizing temperature and returned to said conversion zone” claim 3);
wherein the active solid particles have a particle size of 0.05 mm - 5 mm (200 mesh is 0.074 mm); and
a combustor reactor in fluid communication with the reducer reactor, the combustor reactor configured to receive active solid particles from the reducer reactor (“Metal oxide regenerator 30 is arranged in an elevated position with respect to oxidizer 10 and contains a dense bed 32 of reduced metal oxide in the state of reoxidation” column 4, line 46).
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Lewis does not disclose:
the reducer reactor including inert solid particles, wherein the inert solid particles comprise a refractory material, wherein the refractory material includes
S
i
0
2
,
A
l
2
0
3
,
C
a
O
,
M
g
O
, aluminosilicates, kaolin, mullite, alumina-zirconia-silica,
C
a
A
l
2
0
4
, or
C
a
A
l
4
0
7
;
wherein the inert solid particles are not reactants in either the reduction reaction or the oxidation reaction;
wherein the inert solid particles have a particle size of 0.05 mm - 5 mm;
wherein an active solid particle terminal velocity is within 10% of an inert solid particle terminal velocity;
wherein an active particle density is no more than 40% greater, or no more than 40% less than, an inert particle density;
wherein a ratio of inert solid particles to active solid particles is 0.25:1 to 1:1;
the combustor reactor configured to receive inert solid particles from the reducer reactor.
However, Johnson teaches:
the reducer reactor including inert solid particles (“It may also be desirable to maintain the metal oxide on a suitable inert material as a support or carrier, or it may be desirable to have such inert material present in the reaction zone itself as separate particles from the oxides of manganese, as a diluent. This inert material may serve as a heat carrier and also may serve in aiding in the suspension and fluidization of the metal oxide” column 4, line 70),
the reducer reactor including inert solid particles, wherein the inert solid particles comprise a refractory material, wherein the refractory material includes
S
i
0
2
,
A
l
2
0
3
,
C
a
O
,
M
g
O
, aluminosilicates, kaolin, mullite, alumina-zirconia-silica,
C
a
A
l
2
0
4
, or
C
a
A
l
4
0
7
(“Such inert materials suitable as diluents or carriers comprise silica, alumina, magnesia, bentonite type clays as "Filtrol" and "Super-Filtrol" (acid treated bentonite), and various materials known to those skilled in the art” column 5, line 3);
wherein the inert solid particles are not reactants in either the reduction reaction or the oxidation reaction (“inert”);
wherein the inert solid particles have a particle size of 0.05 mm - 5 mm (“If present as separate particles in admixture with the oxygen carrier, the inert material is of a size within the ranges previously discussed with reference to the manganese oxide” column 5, line 8 and “A highly desirable powdered oxide of manganese for use in this invention comprises about 15 per cent between 0 and 20 microns, about 20 per cent between 20 and 40 microns, about 30 per cent between about 40 and 60 microns, about 25 per cent between 60 and 80 microns, and not over 10 per cent above 80 microns” column 3, line 35);
wherein an active solid particle terminal velocity is within 10% of an inert solid particle terminal velocity (“In the preferred form of this invention, the powdered mass is maintained in a reactor substantially larger than the volume occupied by the mass itself in the fluidized condition” column 3, line 43 suggests that the whole powdered mass is fluidized together and must therefore have a substantially similar terminal velocity);
wherein an active particle density is no more than 40% greater, or no more than 40% less than, an inert particle density (At least magnesia and alumina have densities no more than 40% greater and no more than 40% less than manganese oxide);
the combustor reactor configured to receive inert solid particles from the reducer reactor (“Reduced contact material is oxidized in reactor 41 and is removed from the bottom thereof by means of standpipe 48 and returned to the bottom of reducing reactor 26 by introduction into conduit 24” column 9, line 18).
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In view of Johnson’s teachings, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the invention to include the inert solid particles as is taught in Johnson, in the chemical looping system disclosed by Lewis because Johnson states “This inert material may serve as a heat carrier and also may serve in aiding in the suspension and fluidization of the metal oxide.” Therefore, including the inert material taught by Johnson will improve heat carrying and fluidization of the metal oxide of Lewis.
Lewis, as modified by Johnson, does not explicitly disclose wherein a ratio of inert solid particles to active solid particles is 0.25:1 to 1:1. However, it has been held that “[w]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See MPEP §2144.05(II)(A) (quoting In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). Although, it has been further held that "[a] particular parameter must first be recognized as a result-effective variable, i.e. a variable which achieves a recognized result, before determination of the optimum or workable ranges of said variable might be characterized as routine experimentation. Refer to MPEP §2144.05(II)(B)(quoting In re Antonie, 559 F.2d 618, 195 USPQ 6 (CCPA 1977). In this case, Johnson teaches inert solid particles, but does not specifically recite the ratio of inert solid particles to the active solid particles. Achieving 0.25:1 to 1:1 is a results-effective variable because Johnson states that the inert solid particles aid in suspension. Accordingly, it would have been obvious to one of ordinary skill in the art at the time the invention was made to modify the ratio, because the selection of ratio to achieve improved suspension constitutes the optimization of design parameters, which fails to distinguish the claim.
Regarding claim 2, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 1, wherein the metal oxide is iron oxide (
F
e
2
O
3
), copper oxide (
C
u
O
), nickel oxide (
N
i
O
), manganese oxide (
M
n
2
0
3
), cerium oxide (
C
e
O
2
), cobalt oxide (
C
o
3
0
4
), tungsten oxide (
W
O
3
), vanadium oxide (
V
2
0
5
), calcium and iron oxide (
C
a
2
F
e
2
O
5
), or combinations thereof (“While certain metal oxides which are reduced to metals such as ferrous oxide, cuprous oxide, and the like, are useful for the process, other suitable oxides are the higher oxides of metals which are capable of forming both higher and lower oxides. Typical for the latter oxides are ferric oxide, cupric oxide, vanadium pentoxide, stannic oxide, titanium dioxide, various manganese oxides and mixtures of these oxides. The oxides of titanium, preferably those promoted with a composite containing a major proportion of iron oxide and minor proportions of nickel oxide and chromium oxide are of particular advantage for the present invention because they have been found to possess satisfactory activity and selectivity to form CO and H2” column 3, line 55).
Regarding claim 3, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 2, wherein the metal oxide is
C
u
O
,
M
n
2
0
3
,
C
o
3
0
4
,
F
e
2
O
3
,
N
i
O
, or
C
e
O
2
(“While certain metal oxides which are reduced to metals such as ferrous oxide, cuprous oxide, and the like, are useful for the process, other suitable oxides are the higher oxides of metals which are capable of forming both higher and lower oxides. Typical for the latter oxides are ferric oxide, cupric oxide, vanadium pentoxide, stannic oxide, titanium dioxide, various manganese oxides and mixtures of these oxides. The oxides of titanium, preferably those promoted with a composite containing a major proportion of iron oxide and minor proportions of nickel oxide and chromium oxide are of particular advantage for the present invention because they have been found to possess satisfactory activity and selectivity to form CO and H2” column 3, line 55).
Regarding claim 4, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 1, wherein the active solid particles further comprise a support comprising lithium (Li), beryllium (Be), boron (B), sodium (Na), magnesium (Mg), aluminum (Al), silicon (Si), potassium (K), calcium (Ca), scandium (Sc), titanium (Ti), vanadium (V), chromium (Cr), manganese (Mn), cobalt (Co), zinc(Zn), gallium (Ga), germanium (Ge), rubidium (Rb), yttrium (Y), zirconium (Zr), niobium (Nb), molybdenum (Mo), cadmium (Cd), indium (In), tin (Sn), antimony (Sb), caesium (Cs), barium (Ba), lanthanum (La), cerium (Ce), thorium (Th), and combinations thereof (“The metal oxides may be supported on carriers such as kieselguhr, alumina, silica gel, bentonites, etc., which increase the active surface of the metal oxides” column 3, line 72).
Regarding claim 5, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 4, wherein the support is SiO2, MgO, A1203, TiO2, SiC, or a combination thereof (“The metal oxides may be supported on carriers such as kieselguhr, alumina, silica gel, bentonites, etc., which increase the active surface of the metal oxides” column 3, line 72).
Regarding claim 6, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 4.
Lewis, as modified by Johnson, does not explicitly disclose wherein the weight percentage of the support is between 1 wt% and 99 wt% of the active solid particle. However, it has been held that “[w]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See MPEP §2144.05(II)(A) (quoting In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). Although, it has been further held that "[a] particular parameter must first be recognized as a result-effective variable, i.e. a variable which achieves a recognized result, before determination of the optimum or workable ranges of said variable might be characterized as routine experimentation. Refer to MPEP §2144.05(II)(B)(quoting In re Antonie, 559 F.2d 618, 195 USPQ 6 (CCPA 1977). In this case, Lewis discloses a support, but does not specifically recite the percentage of the active particle that it comprises. Achieving between 1 wt% and 99 wt% of the active solid particle is a results-effective variable because Lewis states that the support increases the active surface of the metal oxide. Accordingly, it would have been obvious to one of ordinary skill in the art at the time the invention was made to modify the percentage, because the selection of percentage to achieve increased active surface constitutes the optimization of design parameters, which fails to distinguish the claim.
Regarding claim 9, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 1, wherein the reducer reactor further comprises second active solid particles, where the second active solid particles comprise different metal oxide than the active solid particles (“The oxides of titanium, preferably those promoted with a composite containing a major proportion of iron oxide and -minor proportions of nickel oxide and chromium-oxide are of particular advantage for the present invention” column 3, line 63).
Regarding claim 13, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 1, wherein the active solid particles have an active particle density ranging from 1000 to 5000 kg/m3 (One or more of the active particles disclosed by Lewis has a density within the claimed range; and
wherein the inert solid particles have an inert particle density ranging from 1000 to 5000 kg/m3 (One or more of the inert particles taught by Johnson has a density within the claimed range).
Regarding claim 15, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 1, wherein the reducer reactor is arranged as a co-current moving bed, a counter-current moving bed, a fluidized bed, a fixed bed, a gas switching fixed bed, a rotary kiln, or a downer; and wherein the combustor reactor is arranged as a co-current moving bed, a counter-current moving bed, a fluidized bed, a fixed bed, a gas switching fixed bed, a rotary kiln, a downer, or a riser (“a dense, turbulent, fluidized mass of finely divided metal oxide” column 2, line 34).
Regarding claim 16, Lewis discloses a method of operating a chemical looping system, the method comprising:
providing active solid particles to a reducer reactor (“In operation, hydrocarbon oxidizer 10 contains a dense bed 12 of titanium dioxide having a particle size of about 200-300 mesh fluidized” column 4, line 32 and “Returning new to oxidizer 10, a partially converted product gas which may still contain up to about 10% or more of unconverted methane is withdrawn from level L10 and passed substantially at the temperature and pressure of oxidizer 10 through line 48 to cleanup oxidizer 50” column 5, line 30),
wherein the active solid particles include a metal oxide (“While certain metal oxides which are reduced to metals such as ferrous oxide, cuprous oxide, and the like, are useful for the process, other suitable oxides are the higher oxides of metals which are capable of forming both higher and lower oxides. Typical for the latter oxides are ferric oxide, cupric oxide, vanadium pentoxide, stannic oxide, titanium dioxide, various manganese oxides and mixtures of these oxides. The oxides of titanium, preferably those promoted with a composite containing a major proportion of iron oxide and minor proportions of nickel oxide and chromium oxide are of particular advantage for the present invention because they have been found to possess satisfactory activity and selectivity to form CO and H2” column 3, line 55);
wherein the active solid particles are capable of cycling between a reduction reaction and an oxidation reaction (“reduced metal oxide is withdrawn from said conversion zone, regenerated with air in the form of a dense, turbulent, fluidized mass of solids in a regeneration zone at an oxidizing temperature and returned to said conversion zone” claim 3);
wherein the active solid particles have a particle size of 0.05 mm - 5 mm (200 mesh is 0.074 mm);
providing a carbonaceous feedstock to the reducer reactor (“Natural gas, preferably preheated to a temperature of about 800°-100° F., is supplied through line 14” column 4, line 39), wherein the reduction reaction includes the carbonaceous feedstock and the active solid particles and generates a first product gas stream (“Product gas consisting predominantly of CO and H2 and containing mere traces of unconverted hydrocarbon and relatively small amounts of CO2 and H2O is withdrawn from oxidizer 50 through line 54” column 5, line 53), where lattice oxygen is transferred from the active solid particles to the carbonaceous feedstock, thereby generating reduced active solid particles (“finely divided metal oxide capable of oxidizing hydrocarbons to carbon monoxide and hydrogen” column 2, line 35); and
providing the reduced active solid particles, and oxidizing agent to a combustor reactor, the combustor reactor in fluid communication with the reducer reactor and configured to receive the reduced active solid particles from the reducer reactor, wherein the oxidation reaction includes the reduced active solid particles and the oxidizing agent to replenish the lattice oxygen (“Metal oxide regenerator 30 is arranged in an elevated position with respect to oxidizer 10 and contains a dense bed 32 of reduced metal oxide in the state of reoxidation” column 4, line 46 and “Any metal or metal oxide fines carried from oxidizer 10 to oxidizer 50 by the gas passing through line 48 are sintered and agglomerated in oxidizer 50 so that the large particles formed will drop out of the gas and collect in the bottom of oxidizer 50 from which they may be removed continuously or periodically through line 53, to be returned through line 35 to regenerator 30, preferably after grinding to the desired particle size” column 5, line 43) and generate a second product gas stream (“Residual air containing about 95-100% nitrogen is withdrawn from level L30 through a gas solids separator, such as cyclone 33 provided with solids return pipe 37, and then through line 43” column 5, line 20).
Lewis does not disclose:
providing inert solid particles to the reducer reactor,
wherein the inert solid particles comprise a refractory material; and
wherein the inert solid particles are not reactants in either the reduction reaction or the oxidation reaction;
wherein the inert solid particles have a particle size of 0.05 mm - 5 mm;
wherein an active solid particle terminal velocity is within 10% of an inert solid particle terminal velocity;
wherein an active particle density is no more than 40% greater, or no more than 40% less than, an inert particle density;
wherein a ratio of inert solid particles to active solid particles is 0.25:1 to 1:1;
providing the inert solid particles to the combustor reactor, the combustor reactor configured to receive the inert particles from the reducer reactor.
However, Johnson teaches:
providing inert solid particles to the reducer reactor (“It may also be desirable to maintain the metal oxide on a suitable inert material as a support or carrier, or it may be desirable to have such inert material present in the reaction zone itself as separate particles from the oxides of manganese, as a diluent. This inert material may serve as a heat carrier and also may serve in aiding in the suspension and fluidization of the metal oxide” column 4, line 70),
wherein the inert solid particles comprise a refractory material (“Such inert materials suitable as diluents or carriers comprise silica, alumina, magnesia, bentonite type clays as "Filtrol" and "Super-Filtrol" (acid treated bentonite), and various materials known to those skilled in the art” column 5, line 3); and
wherein the inert solid particles are not reactants in either the reduction reaction or the oxidation reaction (“inert”);
wherein the inert solid particles have a particle size of 0.05 mm - 5 mm (“If present as separate particles in admixture with the oxygen carrier, the inert material is of a size within the ranges previously discussed with reference to the manganese oxide” column 5, line 8 and “A highly desirable powdered oxide of manganese for use in this invention comprises about 15 per cent between 0 and 20 microns, about 20 per cent between 20 and 40 microns, about 30 per cent between about 40 and 60 microns, about 25 per cent between 60 and 80 microns, and not over 10 per cent above 80 microns” column 3, line 35);
wherein an active solid particle terminal velocity is within 10% of an inert solid particle terminal velocity (“In the preferred form of this invention, the powdered mass is maintained in a reactor substantially larger than the volume occupied by the mass itself in the fluidized condition” column 3, line 43 suggests that the whole powdered mass is fluidized together and must therefore have a substantially similar terminal velocity);
wherein an active particle density is no more than 40% greater, or no more than 40% less than, an inert particle density (At least magnesia and alumina have densities no more than 40% greater and no more than 40% less than manganese oxide);
providing the inert solid particles to the combustor reactor, the combustor reactor configured to receive the inert particles from the reducer reactor (“Reduced contact material is oxidized in reactor 41 and is removed from the bottom thereof by means of standpipe 48 and returned to the bottom of reducing reactor 26 by introduction into conduit 24” column 9, line 18).
In view of Johnson’s teachings, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the invention to include the inert solid particles as is taught in Johnson, in the method disclosed by Lewis because Johnson states “This inert material may serve as a heat carrier and also may serve in aiding in the suspension and fluidization of the metal oxide.” Therefore, including the inert material taught by Johnson will improve heat carrying and fluidization of the metal oxide of Lewis.
Lewis, as modified by Johnson, does not explicitly disclose wherein a ratio of inert solid particles to active solid particles is 0.25:1 to 1:1. However, it has been held that “[w]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See MPEP §2144.05(II)(A) (quoting In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). Although, it has been further held that "[a] particular parameter must first be recognized as a result-effective variable, i.e. a variable which achieves a recognized result, before determination of the optimum or workable ranges of said variable might be characterized as routine experimentation. Refer to MPEP §2144.05(II)(B)(quoting In re Antonie, 559 F.2d 618, 195 USPQ 6 (CCPA 1977). In this case, Johnson teaches inert solid particles, but does not specifically recite the ratio of inert solid particles to the active solid particles. Achieving 0.25:1 to 1:1 is a results-effective variable because Johnson states that the inert solid particles aid in suspension. Accordingly, it would have been obvious to one of ordinary skill in the art at the time the invention was made to modify the ratio, because the selection of ratio to achieve improved suspension constitutes the optimization of design parameters, which fails to distinguish the claim.
Regarding claim 18, Lewis, as modified by Johnson, discloses the method according to claim 16, further comprising:
providing steam, carbon dioxide (C02), or a combination thereof, to the reducer reactor (“steam superheated to a similar temperature may be added through line 16” column 4, line 41);
wherein the carbonaceous feedstock is coal, biomass, natural gas, shale gas, biogas, or petroleum coke (“hydrocarbon gases such as natural gas, methane, etc.” column 2, line 33);
wherein the first product gas stream includes one or more of: unconverted gaseous fuel, unconverted volatile components of solid feedstocks, hydrogen (H2), carbon monoxide (CO), C02 and steam (“Product gas consisting predominantly of CO and H2 and containing mere traces of unconverted hydrocarbon and relatively small amounts of CO2 and H2O is withdrawn from oxidizer 50 through line 54” column 5, line 53);
wherein the oxidizing agent includes at least one of: steam, carbon dioxide (C02), and air (“air, preferably preheated to about 800°-1000° F., and supplied through line 34” column 4, line 50); and
wherein the second product gas stream includes one or more of: hydrogen (H2), steam, carbon monoxide (CO), carbon dioxide (C02), nitrogen (N2), and oxygen (02) (“Residual air containing about 95-100% nitrogen is withdrawn from level L30 through a gas solids separator, such as cyclone 33 provided with solids return pipe 37, and then through line 43” column 5, line 20).
Regarding claim 19, Lewis, as modified by Johnson, discloses the method according to claim 16, wherein the reducer reactor and the combustor reactor are operated at a temperature of 600 °C to 1300 °C and at a pressure of 0.5 atm to 50 atm (“Operating temperatures for titanium dioxide may be about 1500°- 1900° F., preferably about 1600° F. in regenerator 30 and about 1400°-1600° F., preferably about 1500° F. in oxidizer 10” column 5, line 11 and “Oxidizer 10 may be maintained at an elevated pressure of, say, about- 75-200 lbs. per square inch, preferably 100-150 lbs. per square inch, while regenerator 30 is kept at a lower pressure, preferably at about atmospheric to 50 lbs. per square inch” column 4, line 58).
Regarding claim 20, Lewis, as modified by Johnson, discloses the method according to claim 16, further comprising providing second active solid particles, the second active solid particles comprising a metal oxide different from the active solid particles (“While certain metal oxides which are reduced to metals such as ferrous oxide, cuprous oxide, and the like, are useful for the process, other suitable oxides are the higher oxides of metals which are capable of forming both higher and lower oxides. Typical for the latter oxides are ferric oxide, cupric oxide, vanadium pentoxide, stannic oxide, titanium dioxide, various manganese oxides and mixtures of these oxides. The oxides of titanium, preferably those promoted with a composite containing a major proportion of iron oxide and minor proportions of nickel oxide and chromium oxide are of particular advantage for the present invention because they have been found to possess satisfactory activity and selectivity to form CO and H2” column 3, line 55).
Claim 7 is rejected under 35 U.S.C. 103 as being unpatentable over Lewis, in view of Johnson, and further in view of Fan (US 20140295361 A1), hereinafter Fan361.
Regarding claim 7, Lewis, as modified by Johnson discloses the chemical looping system according to claim 1.
Lewis, as modified by Johnson, does not disclose wherein the active solid particles further comprise one or more dopants selected from: nickel (Ni), cobalt (Co), copper (Cu), scandium (Sc), titanium (Ti), vanadium (V), chromium (Cr), manganese (Mn), zinc (Zn), yttrium (Y), zirconium (Zr), niobium (Nb), molybdenum (Mo), technetium (Tc), ruthenium (Ru), rhodium (Rh), palladium (Pd), silver (Ag), cadmium (Cd), lutetium (Lu), hafnium (Hf), tantalum (Ta), tungsten (W), rhenium (Re), osmium (Os), iridium (Ir), platinum (Pt), and gold (Au).
However, Fan361 teaches wherein the active solid particles further comprise one or more dopants selected from: nickel (Ni), cobalt (Co), copper (Cu), scandium (Sc), titanium (Ti), vanadium (V), chromium (Cr), manganese (Mn), zinc (Zn), yttrium (Y), zirconium (Zr), niobium (Nb), molybdenum (Mo), technetium (Tc), ruthenium (Ru), rhodium (Rh), palladium (Pd), silver (Ag), cadmium (Cd), lutetium (Lu), hafnium (Hf), tantalum (Ta), tungsten (W), rhenium (Re), osmium (Os), iridium (Ir), platinum (Pt), and gold (Au) (“In one embodiment, the addition of dopants improved the methane oxidation rates of the oxygen carrying material, as shown in FIG. 6. The data of FIG. 6 was produced from an experiment wherein CH4 at 100 ml/min was contacted with the oxygen carrying material at about 900° C. In one embodiment, the dopants that may be oxides of ceria and/or zirconia” paragraph [0066]).
In view of Fan361’s teachings, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the invention to include the dopants as is taught in Fan, in the chemical looping system disclosed by Lewis because Fan361 states that dopants improve the methane oxidation rates. Therefore, including the support and dopants of Fan361 will improve methane oxidation rates in the system of Lewis.
Claims 11 and 17 are rejected under 35 U.S.C. 103 as being unpatentable over Lewis, in view of Johnson, and further in view of Fan (US 20090000194 A1), hereinafter Fan194.
Regarding claim 11, Lewis, as modified by Johnson, discloses the chemical looping system according to claim 1.
Lewis, as modified by Johnson, does not disclose an oxidizer reactor in fluid communication with the combustor reactor and the reducer reactor, the oxidizer reactor configured to receive active solid particles and inert solid particles from the combustor reactor.
However, Fan194 teaches an oxidizer reactor in fluid communication with the combustor reactor and the reducer reactor, the oxidizer reactor configured to receive active solid particles and inert solid particles from the combustor reactor (“Referring to the FIG. 5 embodiment, a third reactor 3 in form of a fluidized bed is utilized to recover the heat for further oxidation of the particles exiting the second reactor” [0061]).
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In view of Fan194’s teachings, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the invention to include an oxidizer reactor in fluid communication with the combustor reactor and the reducer reactor, the oxidizer reactor configured to receive active solid particles and inert solid particles from the combustor reactor as is taught in Fan194, in the system disclosed by Lewis because Fan194 states “FIG. 5 is a schematic illustration of another system for producing hydrogen from coal, wherein the system utilizes a third reactor for heat recovery according to one or more embodiments of the present invention” (paragraph [0015]). Therefore, including the third reactor will improve heat recovery in Lewis.
Regarding claim 17, Lewis, as modified by Johnson, discloses the method according to claim 16.
Lewis, as modified by Johnson, does not disclose:
providing the active solid particles from the combustor reactor to an oxidizer reactor;
providing an air stream to the oxidizer reactor, wherein the active solid particles are regenerated in the oxidizer reactor;
collecting a depleted air stream from the oxidizer reactor; and
providing the regenerated active solid particles to the reducer reactor.
However, Fan194 teaches:
providing the active solid particles from the combustor reactor to an oxidizer reactor (“Referring to the FIG. 5 embodiment, a third reactor 3 in form of a fluidized bed is utilized to recover the heat for further oxidation of the particles exiting the second reactor i.e. the metal oxide intermediates” paragraph [0061]);
providing an air stream to the oxidizer reactor, wherein the active solid particles are regenerated in the oxidizer reactor (Figure 5,
O
2
);
collecting a depleted air stream from the oxidizer reactor (Figure 5, MO); and
providing the regenerated active solid particles to the reducer reactor (“first reactor 1” paragraph [0061]).
In view of Fan194’s teachings, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the invention to include an oxidizer reactor in fluid communication with the combustor reactor and the reducer reactor, the oxidizer reactor configured to receive active solid particles and inert solid particles from the combustor reactor as is taught in Fan, in the method disclosed by Lewis because Fan194 states “FIG. 5 is a schematic illustration of another system for producing hydrogen from coal, wherein the system utilizes a third reactor for heat recovery according to one or more embodiments of the present invention” (paragraph [0015]). Therefore, including the third reactor will improve heat recovery in Lewis.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure:
Corner (US 2553551 A) Similar to the cited Lynch reference
Ksepko (WO 2011070450 A1) “Many possible oxygen carriers are known, including various compositions of copper, manganese, iron or nickel oxides used as active materials and aluminium oxide, titanium dioxide, zirconium dioxide used as an inert material. Inert materials are added at the amount from a few to a few dozen wt.% in relation to the active material, due to which the oxide carriers life is extended, inter alia via the reduction of their abrasion”
Siriwardane (US 20130316292 A1) “Disclosed here is an oxygen carrier comprised of a metal oxide and MgO promoter particles for the chemical looping combustion of a gaseous hydrocarbon at temperatures greater than about 725° C. The oxygen carrier maintains MgO as a discrete component over numerous redox cycles, and demonstrably improves the percentage combustion and oxygen utilization of the metal oxide”
Fan (US 20140295361 A1) “The mixture may then be modified to the given particle size range of about 0.5 mm to about 7 mm in diameter”
Fan (US 20160023190 A1) “In addition to the active mass, the oxygen carrying material may comprise a high-strength inert structure. As used herein, a high-strength inert structure is a solid framework structure of one or more materials that are inert to oxidation and reduction reactions, or substantially inert to oxidation and reduction reactions such as having a very low reactivity unsuitable for chemical looping systems” and “the oxygen carrying material may be in the form of a particle, such as a particle having a diameter of between about 0.5 mm and about 10 mm”
Main (US 2459444 A) “I improved the fluidizing characteristics of the powdered iron used in the fluid catalyst process for synthesizing hydrocarbons by mixing with the iron a quantity of a coarser or larger particle size powdered inert material such as silica gel”
Lewis (US 2623817 A) “an inert heat carrier having high total heat capacity in the process. This heat carrier makes it possible to use preheated air in the oxidation zone without any serious loss in capacity therein. This heated carrier is then conveyed to the reduction zone where it supplies heat for the endothermic reactions occurring therein”
Lewis (US 2671719 A) “In order to realize satisfactory heat transfer from the oxidation chamber to the reduction and reforming chambers, it is advantageous to use an inert heat carrier. When such a sand is employed, it will constitute between about 30 and 60% of the stream of circulating solid”
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