# US 10,478,807 B2 · Catalytic effects of oxygen carrier based chemical-looping reforming of CH4 with CO2 > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 10,478,807 B2 - Document ID: US10478807B2 - Status: Granted - Kind: B2 - Application number: 15/607,954 - Filed: 2017-05-30 - Published: 2017-12-14 - Granted: 2019-11-19 - Earliest claimed: 2015-05-11 - Applicants: University of Wyoming - Inventors: Maohong Fan; Mingchen Tang - Web page: https://patentgrep.com/patent/US10478807B2 ## CPC - B01J 23/83: with rare earths or actinides - B01J 23/002: {Mixed oxides other than spinels, e.g. perovskite} - B01J 37/035: {Precipitation on carriers} - B01J 37/32: Freeze drying, i.e. lyophilisation - C01B 3/061: by reaction of water with metal oxides - C01B 3/40: characterised by the catalyst - B01J 35/613: {10-100 m2/g} - B01J 37/0036: {Grinding} - B01J 2523/00: Constitutive chemical elements of heterogeneous catalysts - C01B 2203/1047: Group VIII metal catalysts - C01B 2203/1088: Non-supported catalysts - C01B 2203/1241: Natural gas or methane - Y02E 60/36: Hydrogen production from non-carbon containing sources, e.g. by water electrolysis - Y02P 20/52: using catalysts, e.g. selective catalysts - Y02P 30/00: Technologies relating to oil refining and petrochemical industry - B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS - C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C} - Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION - Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS ## Abstract The invention relates to CeO2 and La2O3 for catalyzing Fe2O3—Al2O3 based chemical-looping reforming of CH4 with CO2 (CL-DRM). The reaction performance of all the composite oxygen carriers was evaluated in a fixed-bed reactor at atmospheric pressure condition. The influencing factors, including temperature and time-on-stream (TOS) were investigated. The characteristics of the oxygen carriers were checked with Brunauer-Emmett-Teller (BET) analysis and X-ray diffraction (XRD). The reducibility of the composite materials was elucidated with temperature-programmed reduction by CH4 (CH4-TPR). Preliminary experimental observations suggest that the simultaneous presence of CeO2 and La2O3 can not only enhance the reactivity of Fe2O3—Al2O3 toward CH4 oxidation and its oxygen releasing rate for fast reaction kinetics, but also improve the reactivity of its reduced form toward CO2 splitting. ## Claims ### Claim 1 A method of carbon dioxide sequestration, comprising the steps of: introducing a gaseous feed mixture comprising carbon dioxide (CO2) into a reactor; and performing carbon dioxide sequestration according to reaction R1, reaction R2, and reaction R3: MO+CH4→M+2H2+CO (R1) MO+CO2→MO+CO (R2) CH4+CO2→2H2+2CO (R3) wherein said M is a metal, wherein said MO is a metal oxide, and wherein reaction R1 and reaction R2 further comprise a rare earth oxide catalyst. ### Claim 2 (depends on 1) The method of claim 1, wherein the metal comprises at least one of Fe and Al. ### Claim 3 (depends on 1) The method of claim 1, wherein the metal oxide comprises Fe2O3—Al2O3. ### Claim 4 (depends on 1) The method of claim 1, wherein the rare earth oxide catalyst comprises CeO2 and La2O3. ### Claim 5 (depends on 1) The method of claim 1, wherein the rare earth oxide catalyst comprises a perovskite crystallographic structure comprising a formula: LaxCe1-xFeO3 wherein said x is a range from 0 to 1. ### Claim 6 (depends on 1) The method of claim 1, wherein the rare earth oxide catalyst comprises a perovskite crystallographic structure comprising a formula: LaxCe1-xFeO3-δ, wherein said x is a range from 0 to 1, and wherein said 6 is a value indicative of oxygen consumed by oxidation. ### Claim 7 A method of carbon dioxide sequestration, comprising the steps of: introducing gaseous carbon dioxide (CO2) into a first reactor; and introducing methane (CH4) into a second reactor, wherein the first reactor and second reactor are in gaseous communication with each other; and performing carbon dioxide (CO2) sequestration according to reaction R1, reaction R2, and reaction R3: MO+CH4→M+2H2+CO (R1) MO+CO2→MO+CO (R2) CH4+CO2→2H2+2CO (R3) wherein said M is a metal, wherein said MO is a metal oxide, and wherein reaction R1 and reaction R2 further comprise a rare earth oxide catalyst. ### Claim 8 (depends on 7) The method of claim 7, wherein the rare earth oxide catalyst comprises a perovskite crystallographic structure comprising a formula: LaxCe1-xFeO3 wherein said x is a range from 0 to 1. ### Claim 9 (depends on 7) The method of claim 7, wherein the rare earth oxide catalyst comprises a perovskite crystallographic structure comprising a formula: LaxCe1-xFeO3-δ, wherein said x is a range from 0 to 1, and wherein said δ is a value indicative of oxygen consumed by oxidation. ### Claim 10 A method of enhancing a reactivity of Fe2O3-Al2O3toward CH4 oxidation and enhancing an oxygen releasing rate for improving kinetics, comprising the steps of: introducing a gaseous feed mixture comprising carbon dioxide (CO2) into a reactor containing a dual component perovskite crystallographic structure LaxCe1-xFeO3, wherein said x is a range from 0 to 1; and performing oxidation or partial oxidation in the reactor. ### Claim 11 (depends on 10) The method of claim 10, wherein the performing oxidation or partial oxidation in the reactor step is done according to reaction R1 and R2: La x ⁢ Ce 1 - x ⁢ FeO 3 + δ 1 4 ⁢ CH 4 → δ 1 4 ⁢ CO 2 + δ 1 2 ⁢ H 2 ⁢ O + La x ⁢ Ce 1 - x ⁢ FeO 3 - δ 1 , ( R1 ) La x ⁢ Ce 1 - x ⁢ FeO 3 + δ 2 ⁢ CH 4 → δ 2 ⁢ CO + 2 ⁢ δ 2 ⁢ H 2 + La x ⁢ Ce 1 - x ⁢ FeO 3 - δ 2 , ( R2 ) wherein said x is a range from 0 to 1, and wherein said δ is a value indicative oxygen consumed by oxidation.