One-pot integrated CO2 and NH3 capture and utilization using ionic liquids towards ammonium carbamate
An innovative and effective integrated CO2 and NH3 capture and conversion system is developed using ionic liquids (ILs) as bifunctional sorbent/catalyst media to produce ammonium carbamate (CM), added-value product with high potential as fertilizer, urea precursor, hydrogen carrier, among others. IL...
| Autores: | , , , |
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| Tipo de documento: | artigo |
| Data de publicação: | 2025 |
| País: | España |
| Recursos: | Universidad Autónoma de Madrid |
| Repositório: | Biblos-e Archivo. Repositorio Institucional de la UAM |
| Idioma: | inglês |
| OAI Identifier: | oai:repositorio.uam.es:10486/728580 |
| Acesso em linha: | https://hdl.handle.net/10486/728580 https://dx.doi.org/10.1016/j.cej.2025.166708 |
| Access Level: | Acceso aberto |
| Palavra-chave: | CO2 capture and conversion NH3 valorization Ionic liquids Ammonium carbamate Química |
| Resumo: | An innovative and effective integrated CO2 and NH3 capture and conversion system is developed using ionic liquids (ILs) as bifunctional sorbent/catalyst media to produce ammonium carbamate (CM), added-value product with high potential as fertilizer, urea precursor, hydrogen carrier, among others. ILs have demonstrated valuable behavior as reactive carbon capture (RCC) agents, allowing integrated CO2 absorption and conversion. In addition, task-specific ILs demonstrated competitive process performance in NH3 capture from gas streams. In this work, DFT/COSMO-RS computational methodology was applied to select IL compounds, among a broad range of cation/anion combinations, with the required: i) high NH3 and CO2 gas solubility, to promote capture from gas stream; and ii) low ammonium carbamate solubility, facilitating solid product separation. The hydroxylfunctionalized IL [EtOHmim][NTf2] emerges as the most appropriate option based on molecular simulations. One-pot absorption/catalytic essays demonstrated the formation of CM production IL media at room temperature. A novel characterization methodology based on thermogravimetric analysis (TGA) was developed to fulfill the need of product quantitative analysis, providing reliable composition of CM and side products. The influence of different operating variables on NH3 conversion, CM yield and purity were analyzed, including reaction time, IL mass loading, NH3 feeding time and water presence. Furthermore, consecutive reaction cycles were carried out obtaining nearly complete conversion for every reaction, demonstrating the feasibility of continuous operation without the requirement for sorbent/catalyst regeneration, due to product precipitation. Noteworthy, highpurity CM was obtained by working in the absence of water. Summarizing, a new one-pot IL-based process to produce CM at mild operating conditions through CO2 and NH3 capture, and conversion was developed, with promising potential in agro-industrial and energy applications |
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