Catalytic effects of oxygen carrier based chemical-looping reforming of CH4 with CO2

Patent metadata

Field	Value
Publication number	US-10478807-B2
Application number	US-201715607954-A
Country	US
Kind code	B2
Filing date	May 30, 2017
Priority date	May 11, 2015
Publication date	Nov 19, 2019
Grant date	Nov 19, 2019

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.

First claim

What is claimed:

1. A method of carbon dioxide sequestration, comprising the steps of:
introducing a gaseous feed mixture comprising carbon dioxide (CO 2 ) into a reactor; and
performing carbon dioxide sequestration according to reaction R1, reaction R2, and reaction R3:
MO+CH 4 →M+2H 2 +CO  (R1)

MO+CO 2 →MO+CO  (R2)

CH 4 +CO 2 →2H 2 +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.

2. The method of claim 1 , wherein the metal comprises at least one of Fe and Al.

3. The method of claim 1 , wherein the metal oxide comprises Fe 2 O 3 —Al 2 O 3 .

4. The method of claim 1 , wherein the rare earth oxide catalyst comprises CeO 2 and La 2 O 3 .

5. The method of claim 1 , wherein the rare earth oxide catalyst comprises a perovskite crystallographic structure comprising a formula: La x Ce 1-x FeO 3 wherein said x is a range from 0 to 1.

6. The method of claim 1 , wherein the rare earth oxide catalyst comprises a perovskite crystallographic structure comprising a formula: La x Ce 1-x FeO 3-δ , wherein said x is a range from 0 to 1, and wherein said 6 is a value indicative of oxygen consumed by oxidation.

7. A method of carbon dioxide sequestration, comprising the steps of:
introducing gaseous carbon dioxide (CO 2 ) into a first reactor; and
introducing methane (CH 4 ) into a second reactor, wherein the first reactor and second reactor are in gaseous communication with each other; and
performing carbon dioxide (CO 2 ) sequestration according to reaction R1, reaction R2, and reaction R3:
MO+CH 4 →M+2H 2 +CO  (R1)

MO+CO 2 →MO+CO  (R2)

CH 4 +CO 2 →2H 2 +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.

8. The method of claim 7 , wherein the rare earth oxide catalyst comprises a perovskite crystallographic structure comprising a formula: La x Ce 1-x FeO 3 wherein said x is a range from 0 to 1.

9. The method of claim 7 , wherein the rare earth oxide catalyst comprises a perovskite crystallographic structure comprising a formula: La x Ce 1-x FeO 3-δ , wherein said x is a range from 0 to 1, and wherein said δ is a value indicative of oxygen consumed by oxidation.

10. A method of enhancing a reactivity of Fe 2 O 3 -Al 2 O 3 toward CH 4 oxidation and enhancing an oxygen releasing rate for improving kinetics, comprising the steps of:
introducing a gaseous feed mixture comprising carbon dioxide (CO 2 ) into a reactor containing a dual component perovskite crystallographic structure La x Ce 1-x FeO 3 , wherein said x is a range from 0 to 1; and
performing oxidation or partial oxidation in the reactor.

11. 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
⁢

Assignees

• Univ Wyoming

Inventors

• Fan Maohong
• Tang Mingchen

Classifications

• B01J37/035

  Precipitation on carriers · CPC title

• C01B2203/1088

  Non-supported catalysts · CPC title

• B01J37/32

  Freeze drying, i.e. lyophilisation · CPC title

• B01J37/0036

  Grinding · CPC title

• B01J23/002

  Mixed oxides other than spinels, e.g. perovskite · CPC title