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1.
Chemosphere ; 333: 138915, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37172623

RESUMO

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. H-cell 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. 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.


Assuntos
Dióxido de Carbono , Nitrosaminas , Humanos , Dióxido de Carbono/química , Aminas/química , Nitrosaminas/química , Carbono , Solventes/química
2.
Nat Commun ; 14(1): 19, 2023 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-36624103

RESUMO

Increasing the performance of Pt-based electrocatalysts for the oxygen reduction reaction (ORR) is essential for the widespread commercialization of polymer electrolyte fuel cells. Here we show the synthesis of double-layer Pt nanosheets with a thickness of 0.5 nm via the topotactic reduction of 0.9 nm-thick single-layer PtOx nanosheets, which are exfoliated from a layered platinic acid (HyPtOx). The ORR activity of the Pt nanosheets is two times greater than that of conventionally used state-of-the-art 3 nm-sized Pt nanoparticles, which is attributed to their large electrochemically active surface area (124 m2 g-1). These Pt nanosheets show excellent potential in reducing the amount of Pt used by enhancing its ORR activity. Our results unveil strategies for designing advanced catalysts that are considerably superior to traditional nanoparticle systems, allowing Pt catalysts to operate at their full potential in areas such as fuel cells, rechargeable metal-air batteries, and fine chemical production.

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