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HERO ID
1520329
Reference Type
Journal Article
Title
Kinetics of N-Nitrosopiperazine Formation from Nitrite and Piperazine in CO2 Capture
Author(s)
Goldman, MJ; Fine, NA; Rochelle, GT
Year
2013
Is Peer Reviewed?
1
Journal
Environmental Science & Technology
ISSN:
0013-936X
EISSN:
1520-5851
Volume
47
Issue
7
Page Numbers
3528-3534
Language
English
PMID
23438967
DOI
10.1021/es304640f
Web of Science Id
WOS:000317173100066
Abstract
Piperazine (PZ) is an efficient amine for carbon capture systems, but it can form N-nitrosopiperazine (MNPZ), a carcinogen, from nitrogen oxides (NOx) in flue gas from coal or natural gas combustion. The reaction of nitrite with PZ was studied in 0.1 to 5 mol/dm(3) PZ with 0.001 to 0.8 mol CO2/mol PZ at 50 to 135 °C. The reaction forming MNPZ is first order in nitrite, piperazine carbamate species, and hydronium ion. The activation energy is 84 ± 2 kJ/mol with a rate constant of 8.5 × 10(3) ± 1.4 × 10(3) dm(6) mol(-2) s(-1) at 100 °C. The proposed mechanism involves protonation of the carbamate species, nucleophilic attack of the carbamic acid, and formation of bicarbonate and MNPZ. These kinetics and mechanism will be useful in identifying inhibitors and other strategies to reduce nitrosamine accumulation in CO2 capture by scrubbing with PZ or other amines.
Keywords
Capture system; Carbamate species; Carbamic acid; First order; Hydronium ions; Kinetics and mechanism; Natural gas combustion; Nucleophilic attack; Activation energy; Coal combustion; Flue gases; Nitrogen oxides; Organic acids; Rate constants; Carbon dioxide; 1 nitrosopiperazine; amine; bicarbonate; carbamic acid; carbon dioxide; hydronium ion; nitrite; nitrosamine; nucleophile; piperazine; piperazine derivative; unclassified drug; accumulation; activation energy; bicarbonate; carbamate (ester); carbon dioxide; carcinogen; combustion; inhibitor; natural gas; nitrite; nitrogen oxides; reaction kinetics; article; chemical reaction kinetics; controlled study; Carbamates; Carbon Dioxide; Catalysis; Hydrogen-Ion Concentration; Kinetics; Models, Chemical; Nitrites; Nitrosamines; Nitrosation; Piperazines; Temperature
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