# US 2022/0034858 A1 · A method of selectively catalytically oxidizing dinitrogen oxide, a method of detecting radiocarbon, an apparatus, and use of a NiO catalyst

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- Number: US 2022/0034858 A1
- Document ID: US20220034858A1
- Status: Published application
- Kind: A1
- Application number: 17/280,210
- Filed: 2019-09-24
- Published: 2022-02-03
- Earliest claimed: 2018-09-26
- Assignees: Teknologian tutkimuskeskus VTT Oy
- Applicants: Teknologian tutkimuskeskus VTT Oy
- Inventors: Guillaume Genoud; Matti Reinikainen; Mari-Leena Koskinen-Soivi; Johannes Lehmuskoski
- Web page: https://patentgrep.com/patent/US20220034858A1

## CPC

- G01N 33/0055: {Radionuclides}
- B01D 53/8628: {Processes characterised by a specific catalyst}
- B01D 53/864: {Removing carbon monoxide or hydrocarbons}
- B01J 21/04: Alumina
- B01J 23/44: Palladium
- B01J 23/755: Nickel
- B01J 23/78: with alkali- or alkaline earth metals
- B01J 23/892: {Nickel and noble metals}
- B01J 35/19: {Catalysts containing parts with different compositions}
- B01J 37/031: {Precipitation}
- G01N 21/39: using tunable lasers
- G01N 33/004: {CO or CO2}
- G01N 33/225: {Gaseous fuels, e.g. natural gas}
- B01D 2255/1023: Palladium
- B01D 2255/2027: Sodium
- B01D 2255/20753: Nickel
- B01D 2257/402: Dinitrogen oxide
- B01D 2257/7025: Methane
- B01D 2258/06: Polluted air
- G01N 33/22: Fuels; Explosives
- G01N 2021/399: {Diode laser}
- G01N 2201/0612: Laser diodes
- Y02C 20/10: of nitrous oxide (N2O)
- Y02C 20/20: of methane
- G01N: INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES (measuring or testing apparatus or processes other than immunoassay, involving enzymes or microorganisms C12M, C12Q)
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- Y02C: CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]

## Abstract

A method of selectively catalytically oxidizing dinitrogen oxide present in a gaseous sample, comprising: heating a NiO catalyst to a temperature of at least 250° C.; and bringing the gaseous sample into contact with the heated NiO catalyst to oxidize dinitrogen oxide of the gaseous sample in the presence of the heated NiO catalyst.

## Claims

### Claim 1

A method of selectively catalytically oxidizing dinitrogen oxide present in a gaseous sample, comprising:
heating a NiO catalyst to a temperature of at least 250° C.; and
bringing the gaseous sample into contact with the heated NiO catalyst to oxidize the dinitrogen oxide of the gaseous sample in the presence of the heated NiO catalyst.

### Claim 2 (depends on 1)

The method according to claim 1, wherein the concentration of methane in the sample is less than 1% and the oxidation of the dinitrogen oxide is carried out while avoiding oxidation of any methane present in the sample.

### Claim 3 (depends on 1)

The method according to claim 1, wherein the catalyst is a heterogeneous alkaline NiO catalyst.

### Claim 4 (depends on 1)

The method according to claim 1, wherein the catalyst is a heterogeneous NiO/NaOH catalyst.

### Claim 5 (depends on 1)

The method according to claim 1, wherein the catalyst is heated to a temperature of at least 300° C.

### Claim 6 (depends on 1)

The method according to claim 1, wherein the gaseous sample additionally contains 14CO2 and 14CH4.

### Claim 7 (depends on 1)

The method according to claim 1, wherein the gaseous sample is a gaseous emission sample from a nuclear power plant or originates from a biofuel.

### Claim 8 (depends on 1)

The method according to claim 1, wherein the gaseous sample is a gaseous atmospheric sample.

### Claim 9

A method of detecting radiocarbon in the form of 14CO2 in a gaseous sample comprising at least 14CO2 and dinitrogen oxide, the method comprising:
selectively catalytically oxidizing the dinitrogen oxide present in the gaseous sample; and subsequently
determining the amount of 14CO2 in the gaseous sample by infrared absorption spectroscopy.

### Claim 10 (depends on 9)

The method according to claim 9, wherein, before the determination step:
the gaseous sample is led to a cryogenic trap which has been cooled to a temperature below 195 K, whereby the 14CO2 present in the sample solidifies and becomes trapped; and
the trapped 14CO2 is released by heating the cryogenic trap to a temperature above 195 K.

### Claim 11 (depends on 9)

The method according to claim 9, wherein the determining step comprises measuring an infrared absorption spectrum of a sample released from the cryogenic trap by using a cavity ring-down laser spectroscopy.

### Claim 12 (depends on 9)

The method according to claim 9, wherein the gaseous sample further comprises 14CH4, and the method further comprises, before the determination step:
catalytically oxidizing the 14CH4 to 14CO2 with a second catalyst, wherein the 14CO2 to be determined in the determination step also comprises the 14CO2 catalytically oxidized from the 14CH4.

### Claim 13 (depends on 12)

The method according to claim 12, wherein the second catalyst is a Pd catalyst, and the step of catalytically oxidizing the 14CH4 to 14CO2 comprises:
heating the Pd catalyst to a temperature of at least 300° C.; and
bringing the gaseous sample into contact with the heated Pd catalyst;
wherein the heated Pd catalyst catalyses oxidation of the 14CH4 present in the gaseous sample to 14CO2.

### Claim 14

An apparatus comprising:
first means for selectively catalytically oxidizing dinitrogen oxide present in a gaseous sample with a NiO catalyst; and
second means for determining the amount of 14CO2 present in the gaseous sample by infrared absorption spectroscopy.

### Claim 15 (depends on 14)

The apparatus according to claim 14, wherein the first means for selectively catalytically oxidizing dinitrogen oxide present in a gaseous sample comprises a first catalyst bed comprising the NiO catalyst.

### Claim 16 (depends on 14)

The apparatus according to claim 14, wherein the apparatus comprises:
first means for selectively catalytically oxidizing dinitrogen oxide present in a gaseous sample and further means for catalytically oxidizing 14CH4 present in the gaseous sample, in any order; and downstream of said first means and further means, and
second means for determining the combined amount of 14CO2 present in the gaseous sample and 14CO2 converted from the 14CH4 present in the gaseous sample by infrared absorption spectroscopy.

### Claim 17 (depends on 16)

The apparatus according to claim 16, wherein the further means for catalytically oxidizing 14CH4 present in the gaseous sample comprises a second catalyst bed comprising a second catalyst.

### Claim 18 (depends on 14)

The apparatus according to claim 14, wherein the second means comprises a cavity ring-down laser spectrometer comprising a quantum cascade laser as an infrared light source.

### Claim at position 19

19-22. (canceled)

### Claim 23 (depends on 1)

The method according to claim 1, wherein the catalyst is heated to a temperature of from 350 to 500° C.

### Claim 24 (depends on 17)

The apparatus according to claim 17, wherein the second catalyst comprises a Pd catalyst.
