US 12,420,266 B2
Promoted mixed oxides for “low-temperature” methane partial oxidation in absence of gaseous oxidants
Fanxing Li, Raleigh, NC (US); Arya Shafiefarhood, Raleigh, NC (US); and Amit Mishra, Raleigh, NC (US)
Assigned to North Carolina State University, Raleigh, NC (US)
Appl. No. 16/618,890
Filed by North Carolina State University, Raleigh, NC (US)
PCT Filed Jun. 5, 2018, PCT No. PCT/US2018/035973
§ 371(c)(1), (2) Date Dec. 3, 2019,
PCT Pub. No. WO2018/226635, PCT Pub. Date Dec. 13, 2018.
Claims priority of provisional application 62/515,169, filed on Jun. 5, 2017.
Prior Publication US 2021/0113996 A1, Apr. 22, 2021
Int. Cl. B01J 23/06 (2006.01); B01J 23/00 (2006.01); B01J 23/10 (2006.01); B01J 23/34 (2006.01); B01J 23/46 (2006.01); B01J 23/96 (2006.01); B01J 38/06 (2006.01); C01B 3/40 (2006.01); C01B 3/48 (2006.01)
CPC B01J 23/464 (2013.01) [B01J 23/002 (2013.01); B01J 23/10 (2013.01); B01J 23/34 (2013.01); B01J 23/96 (2013.01); B01J 38/06 (2013.01); C01B 3/40 (2013.01); C01B 3/48 (2013.01); C01B 2203/0261 (2013.01); C01B 2203/0283 (2013.01); C01B 2203/1064 (2013.01); C01B 2203/1082 (2013.01); C01B 2203/1241 (2013.01)] 26 Claims
OG exemplary drawing
 
1. A method of converting methane to syngas, the method comprising contacting the methane with a redox catalyst to produce the syngas,
wherein the redox catalyst comprises metal cations and is (1) a cerium containing oxide or (2) a perovskite oxide comprising La, Ba, Sr, Ca, or any combination thereof;
wherein the redox catalyst is in a fixed bed reactor having a first end and a second end;
wherein the redox catalyst nearest the first end is initially at a first high average oxidation state and the redox catalyst nearest the second end is initially at a second low average oxidation state lower than the first high average oxidation state, and
wherein the method comprises:
(1) introducing the methane into the fixed bed reactor near the first end for a first period of time; wherein the methane contacts the redox catalyst in the first high average oxidation state near the first end of the fixed bed reactor; and
wherein after the first period of time the redox catalyst nearest the first end is in a third low average oxidation state;
(2) introducing a first amount of an oxidant into the fixed bed reactor near the second end for a second period of time; and
wherein after the second period of time the redox catalyst near the second end is in a fourth high average oxidation state higher than the third low average oxidation state;
(3) introducing the methane into the fixed bed reactor near the second end for a third period of time; wherein the methane contacts the redox catalyst in the fourth high average oxidation state near the second end of the fixed bed reactor; and
wherein after the third period of time the redox catalyst nearest the second end is in a fifth low average oxidation state; and
(4) introducing a second amount of the oxidant into the fixed bed reactor near the first end for a fourth period of time; and
wherein after the fourth period of time the redox catalyst near the first end is in a sixth high average oxidation state higher than the fifth low average oxidation state.