# US 2015/0147259 A1 · Methods and systems for forming ammonia and solid carbon products

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- Number: US 2015/0147259 A1
- Document ID: US20150147259A1
- Status: Published application
- Kind: A1
- Application number: 14/414,364
- Filed: 2013-03-15
- Published: 2015-05-28
- Earliest claimed: 2012-07-13
- Assignees: Seerstone LLC
- Applicants: Seerstone LLC
- Inventors: Dallas B. Noyes
- Web page: https://patentgrep.com/patent/US20150147259A1

## CPC

- C01B 5/00: Water
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- B82Y 40/00: Manufacture or treatment of nanostructures
- C01B 32/05: Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
- C01B 32/16: Preparation
- C01B 32/162: characterised by catalysts
- C01C 1/04: Preparation of ammonia by synthesis (preparation or purification of gas mixtures for ammonia synthesis C01B3/025)
- C01C 1/0405: {from N2 and H2 in presence of a catalyst}
- Y02P 20/52: using catalysts, e.g. selective catalysts
- Y10S 977/742: Carbon nanotubes, CNTs
- Y10S 977/843: Gas phase catalytic growth, i.e. chemical vapor deposition
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- C01C: AMMONIA; CYANOGEN; COMPOUNDS THEREOF ({metal hydrides, monoborane, diborane or addition complexes thereof C01B6/00}; salts of oxyacids of halogens C01B11/00; peroxides, salts of peroxyacids C01B15/00; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium or tellurium C01B19/00; azides C01B21/08; {compounds other than ammonia or cyanogen, containing nitrogen, non-metals and optionally metals C01B21/082}; metal imides or amides C01B21/092; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; compounds containing silicon C01B33/00; compounds containing boron C01B35/00)
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y10S: TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS

## Abstract

Methods of concurrently forming ammonia and solid carbon products include reacting a carbon oxide, nitrogen, and a reducing agent at preselected reaction conditions in the presence of a catalyst to form a solid carbon product entrained in a tail gas mixture comprising water and ammonia; separating entrained solid carbon product from the tail gas mixture; and recovering water and ammonia from the tail gas mixture. Systems for forming ammonia and solid carbon products from a gaseous source containing carbon oxides include mixing means for mixing the gaseous source with a reducing agent, reactor means for reacting at least a portion of the gaseous source with the reducing agent in the presence of a catalyst to produce the solid carbon products and a tail gas mixture comprising the ammonia, and solid separation means for separating the solid carbon products from the tail gas mixture.

## Claims

### Claim 1

A method of concurrently forming ammonia and a solid carbon product, comprising:
reacting at least one carbon oxide, nitrogen, and at least one reducing agent at preselected temperature and a preselected pressure in the presence of a catalyst to form solid carbon entrained in a tail gas mixture comprising water, ammonia, and unreacted gases;
separating the entrained solid carbon from the tail gas mixture;
recovering water from the tail gas mixture; and
recovering ammonia from the tail gas mixture.

### Claim at position 2

2-7. (canceled)

### Claim 8 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting a carbon oxide comprising primarily carbon dioxide with the nitrogen and the at least one reducing agent in the presence of the catalyst.

### Claim 9 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting a carbon oxide comprising primarily carbon monoxide with the nitrogen and the at least one reducing agent in the presence of the catalyst.

### Claim 10 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting a carbon oxide comprising carbon dioxide and carbon monoxide with the nitrogen and the at least one reducing agent in the presence of the catalyst.

### Claim 11

(canceled)

### Claim 12 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting the at least one carbon oxide, the nitrogen, and a reducing agent comprising hydrogen in the presence of the catalyst.

### Claim 13 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting the at least one carbon oxide, the nitrogen, and a reducing agent comprising a hydrocarbon in the presence of the catalyst.

### Claim 14 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting the at least one carbon oxide, the nitrogen, and a reducing agent comprising methane in the presence of the catalyst.

### Claim 15 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting a synthesis gas in the presence of the catalyst.

### Claim 16 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting the at least one carbon oxide, the nitrogen, and the at least one reducing agent in the presence of a catalyst comprising iron.

### Claim 17

(canceled)

### Claim 18 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting the at least one carbon oxide, the nitrogen, and the at least one reducing agent in the presence of a catalyst comprising a plurality of nanoparticles, wherein each nanoparticle is mounted on a carbon nanofiber.

### Claim 19 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises reacting the at least one carbon oxide, the nitrogen, and the at least one reducing agent in the presence of a catalyst at a temperature of between about 400° C. and about 1,000° C.

### Claim at position 15

20-22. (canceled)

### Claim 23 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide, nitrogen, and at least one reducing agent in the presence of a catalyst comprises forming a plurality of carbon nanotubes.

### Claim 24 (depends on 23)

The method of claim 23, wherein forming a plurality of carbon nanotubes comprises forming the plurality of carbon nanotubes to have a portion of nitrogen and a portion of amine groups functionalizing the surfaces of the plurality of carbon nanotubes.

### Claim 25 (depends on 1)

The method of claim 1, wherein recovering ammonia from the tail gas mixture comprises:
exposing the tail gas mixture to an aqueous liquid;
absorbing at least a portion of the ammonia in the aqueous liquid; and
separating the tail gas mixture from the aqueous liquid.

### Claim 26

(canceled)

### Claim 27 (depends on 1)

The method of claim 1, wherein reacting at least one carbon oxide and at least one reducing agent in the presence of a catalyst comprises forming water as steam, the method further comprising:
condensing at least a portion of the steam to form liquid water;
absorbing at least a portion of the ammonia in the liquid water; and
separating the absorbed ammonia from the liquid water.

### Claim 28 (depends on 1)

The method of claim 1, further comprising forming a reaction gas mixture comprising the at least one carbon oxide, the nitrogen, and the at least one reducing agent, wherein a molar ratio of the at least one carbon oxide to the nitrogen is in a range from about 10:1 to about 1:10.

### Claim 29 (depends on 1)

The method of claim 1, further comprising mixing at least a portion of the tail gas mixture with the at least one carbon oxide, nitrogen, and the at least one reducing agent after separating the solid carbon product and recovering the water and the ammonia.

### Claim 30

(canceled)

### Claim 31

A method for producing ammonia and solid carbon products, comprising:
heating a first gas stream to a predetermined reaction temperature to form a first heated gas stream, wherein the first gas stream comprises at least one carbon oxide and nitrogen;
heating a second gas stream to the predetermined reaction temperature to form a second heated gas stream, wherein the second gas stream comprises at least one reducing agent;
mixing the first heated gas stream with the second heated gas stream;
reacting the nitrogen, the at least one carbon oxide, and the at least one reducing agent in the presence of a catalyst to form a solid carbon product entrained in a tail gas mixture comprising steam, ammonia, and a residual gas mixture;
separating at least a portion of the entrained solid carbon product from the tail gas mixture; and
separating the tail gas mixture to form a water stream, an ammonia product stream, and a residual gas stream.

### Claim at position 25

32-36. (canceled)

### Claim 37

A system for forming ammonia and solid carbon products from a gaseous source containing at least one carbon oxide and nitrogen, the system comprising:
mixing means for mixing the gaseous source with at least one reducing agent;
reactor means for reacting at least a portion of the gaseous source with the at least one reducing agent in the presence of a catalyst to produce the solid carbon products and a tail gas mixture comprising water and ammonia; and
solid separation means for separating the solid carbon products from the tail gas mixture.

### Claim 38

(canceled)

### Claim 39 (depends on 37)

The system of claim 37, further comprising absorption means for removing ammonia from the tail gas mixture.

### Claim 40

(canceled)