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1520329 
Journal Article 
Kinetics of N-Nitrosopiperazine Formation from Nitrite and Piperazine in CO2 Capture 
Goldman, MJ; Fine, NA; Rochelle, GT 
2013 
Environmental Science & Technology
ISSN: 0013-936X
EISSN: 1520-5851 
47 
3528-3534 
English 
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. 
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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