Targeted electrochemical reduction of carcinogenic N-nitrosamines from emission control systems within CO2 capture plants

Toma, Shino; Omosebi, Ayokunle; Gao, Xin; Abad, Keemia; Bhatnagar, Saloni; Qian, Dali; Liu, Kunlei; Thompson, Jesse G.

doi:10.1016/j.chemosphere.2023.138915

Targeted electrochemical reduction of carcinogenic N-nitrosamines from emission control systems within CO₂ capture plants

Journal Article · Wed May 10 00:00:00 EDT 2023 · Chemosphere

DOI:https://doi.org/10.1016/j.chemosphere.2023.138915· OSTI ID:2409391

Toma, Shino ^[1]; Omosebi, Ayokunle ^[2]; Gao, Xin ^[2]; Abad, Keemia ^[2]; Bhatnagar, Saloni ^[2]; Qian, Dali ^[2]; Liu, Kunlei ^[2]; ^[2]

University of Kentucky, Lexington, KY (United States); University of Kentucky
University of Kentucky, Lexington, KY (United States)

N-Nitrosamines are one of the environmentally significant byproducts from aqueous amine-based post-combustion carbon capture systems (CCS) due to their potential risk to human health. Safely mitigating nitrosamines before they are emitted from these CO₂ capture systems is therefore a key concern before widescale deployment of CCS can be used to address worldwide decarbonization goals. Electrochemical decomposition is one viable route to neutralize these harmful compounds. The circulating emission control waterwash system, commonly installed at the end of the flue gas treatment trains to minimize amine solvent emissions, plays an important role to capture N-nitrosamines and control their emission into the environment. The waterwash solution is the last point where these compounds can be properly neutralized before becoming an environmental hazard. In this study, the decomposition mechanisms of N-nitrosamines in a simulated CCS waterwash with residual alkanolamines was investigated using several laboratory-scale electrolyzers utilizing carbon xerogel (CX) electrodes. Hcell experiments revealed that N-nitrosamines were decomposed through a reduction reaction and are converted into their corresponding secondary amines thereby neutralizing their environmental impact. Batch-cell experiments statistically examined the kinetic models of N-nitrosamine removal by a combined adsorption and decomposition processes. The cathodic reduction of the N-nitrosamines statistically obeyed the first-order reaction model. Finally, a prototype flow-through reactor using an authentic waterwash was used to successfully target and decompose N-nitrosamines to below the detectable level without degrading the amine solvent compounds allowing them to be return to the CCS and lower the system operating costs. Furthermore, the developed electrolyzer was able to efficiently remove greater than 98% of N-nitrosamines from the waterwash solution without producing any additional environmentally harmful compounds and offers an effective and safe route to mitigate these compounds from CO₂ capture systems.

View Accepted Manuscript (DOE)

Research Organization:: University of Kentucky, Lexington, KY (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FE0031661

OSTI ID:: 2409391

Alternate ID(s):: OSTI ID: 1974470

Journal Information:: Chemosphere, Journal Name: Chemosphere Vol. 333; ISSN 0045-6535

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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