Ammonia synthesis process

• US 8,623,313 B2
• Filed: 12/22/2009
• Issued: 01/07/2014
• Est. Priority Date: 01/09/2009
• Status: Expired due to Fees

• Current Assignee: Hitachi Zosen Corporation, Toyota Jidosha Kabushiki Kaisha (Toyota Motor Corporation)
• Original Assignee: Hitachi Zosen Corporation, Toyota Jidosha Kabushiki Kaisha (Toyota Motor Corporation)
• Inventors: Nakamura, Norihiko, Nakanishi, Haruyuki, Arikawa, Hidekazu, Hikazudani, Susumu, Inazumi, Chikashi
• Primary Examiner(s): Nguyen, Ngoc-Yen
• Assistant Examiner(s): BOVA, JUSTIN M
• Application Number:
  US13/143,619
• Publication Number:
  US 20110286907A1
• Time in Patent Office: 1,477 Days
• Field of Search: 423/352, 423/359
• US Class Current: 423/352
• CPC Class Codes: B01J 35/39 Photocatalytic properties
• CPC Class Codes: C01B 13/0207 Water
• CPC Class Codes: C01B 13/0251 by making use of membranes
• CPC Class Codes: C01B 13/0281 in getters
• CPC Class Codes: C01B 2203/042 Purification by adsorption on solids
• CPC Class Codes: C01B 2203/068 Ammonia synthesis
• CPC Class Codes: C01B 2210/0053 Hydrogen
• CPC Class Codes: C01B 3/025 Preparation or purification of gas mixtures for ammonia synthesis
• CPC Class Codes: C01B 3/042 Decomposition of water
• CPC Class Codes: C01B 3/061 by reaction of metal oxides with water
• CPC Class Codes: C01B 3/063 Cyclic methods
• CPC Class Codes: C01B 3/501 by diffusion
• CPC Class Codes: C01B 3/56 by contacting with solids; Regeneration of used solids C01B3/508 takes precedence
• CPC Class Codes: C01B 5/00 Water
• CPC Class Codes: C01C 1/0405 from N2 and H2 in presence of a catalyst
• CPC Class Codes: Y02E 60/36 Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
• CPC Class Codes: Y02P 20/133 Renewable energy sources, e.g. sunlight
• CPC Class Codes: Y02P 20/52 using catalysts, e.g. selective catalysts

Abstract

The invention provides a process for efficient synthesis of ammonia. The process includes a water-splitting step in which water is decomposed to obtain a first source gas comprising hydrogen and oxygen, a first oxygen removal step in which the oxygen contained in the first source gas is at least partially separated and removed by an oxygen separating membrane or hydrogen separating membrane to obtain a second source gas having a lower oxygen concentration than the first source gas, a second oxygen removal step in which the oxygen in the second source gas is reacted with hydrogen to produce water for removal, or is adsorbed onto an adsorption medium for removal, to obtain a third source gas having a lower oxygen concentration than the second source gas, and an ammonia synthesis step in which the hydrogen in the third source gas is reacted with nitrogen to synthesize ammonia.

Claims

1. An ammonia synthesis method comprising:

(a) a water-splitting step in which water is decomposed to obtain a first source gas comprising hydrogen and oxygen,

(b) a first oxygen removal step in which the oxygen contained in the first source gas is at least partially separated and removed by an oxygen separating membrane or hydrogen separating membrane to obtain a second source gas having a lower oxygen concentration than the first source gas,

(c) a second oxygen removal step in which the oxygen in the second source gas is reacted with hydrogen to produce water for removal, or is adsorbed onto an adsorption medium for removal, to obtain a third source gas having a lower oxygen concentration than the second source gas, and

(d) an ammonia synthesis step in which the hydrogen in the third source gas is reacted with nitrogen to synthesize ammonia,

wherein;

in the water-splitting step (a), the water is decomposed by thermochemical decomposition utilizing oxidation-reduction reaction between a metal and a metal oxide, or thermochemical decomposition utilizing oxidation-reduction reaction between metal oxides having different oxidation states from each other, to obtain the first source gas,

the water-splitting step (a) is carried out in a water-splitting/regenerating apparatus having a plurality of water-splitting sections that hold a metal and/or metal oxide to be used for thermal decomposition,

while the water-splitting step (a) is being conducted in at least one of the plurality of water-splitting sections, at least one used water-splitting section among the plurality of water-splitting sections is regenerated by;

(i) an electrolytic method in which a metal oxide produced by a hydrogen-producing reaction is reacted with seawater to yield a metal chloride and the metal chloride is subjected to molten salt electrolysis, or

(ii) a reduction firing method in which a supply of carbon or carbon monoxide is fed to a metal oxide produced by a hydrogen-producing reaction and reduction is accomplished directly by heat, and

the regenerated water-splitting section is reutilized in the water-splitting step (a).

2. The method according to claim 1, wherein in the water-splitting step (a), the water is decomposed by thermochemical decomposition utilizing oxidation-reduction reaction between iron oxides in different oxidation states, to obtain the first source gas.

3. The method according to claim 1, wherein in the water-splitting step (a) and/or the ammonia synthesis step (d), at least part of a required thermal energy is obtained from solar energy.

4. The method according to claim 3, wherein the water-splitting step (a) and/or the ammonia synthesis step (d) are carried out in a light collecting section of a solar collecting device to obtain at least part of the required thermal energy from solar energy.

5. The method according to claim 2, wherein in the water-splitting step (a) and/or the ammonia synthesis step (d), at least part of the required thermal energy is obtained from solar energy.

6. The method according to claim 5, wherein the water-splitting step (a) and/or the ammonia synthesis step (d) are carried out in the light collecting section of a solar collecting device to obtain at least part of the required thermal energy from solar energy.