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1.
Environ Sci Technol ; 58(10): 4606-4616, 2024 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-38427797

RESUMO

Transforming hazardous species into active sites by ingenious material design was a promising and positive strategy to improve catalytic reactions in industrial applications. To synergistically address the issue of sluggish CO2 desorption kinetics and SO2-poisoning solvent of amine scrubbing, we propose a novel method for preparing a high-performance core-shell C@Mn3O4 catalyst for heterogeneous sulfur migration and in situ reconstruction to active -SO3H groups, and thus inducing an enhanced proton-coupled electron transfer (PCET) effect for CO2 desorption. As anticipated, the rate of CO2 desorption increases significantly, by 255%, when SO2 is introduced. On a bench scale, dynamic CO2 capture experiments reveal that the catalytic regeneration heat duty of SO2-poisoned solvent experiences a 32% reduction compared to the blank case, while the durability of the catalyst is confirmed. Thus, the enhanced PCET of C@Mn3O4, facilitated by sulfur migration and simultaneous transformation, effectively improves the SO2 resistance and regeneration efficiency of amine solvents, providing a novel route for pursuing cost-effective CO2 capture with an amine solvent.


Assuntos
Dióxido de Carbono , Prótons , Elétrons , Solventes , Aminas , Enxofre
2.
Environ Sci Technol ; 58(37): 16376-16385, 2024 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-39225344

RESUMO

Carbon dioxide (CO2) chemisorption using biphasic solvents has been regarded as a promising approach, but challenges remain in achieving efficient dynamic phase-splitting during practical implementation. To address this, the centrifugal force was innovatively adopted to enhance the coalescence and separation of immiscible fine droplets within the biphasic solvent. The comprehensive evaluation demonstrates that centrifugal phase-splitting shows outstanding separation efficiency (>95%) and excellent applicability for various solvents. Correlation analysis reveals a strong relationship between the rich phase's viscosity, lean phase's residual CO2, and the phase separation efficiency. The time-profile behavior of immiscible droplets, observed through microscope images of phase-splitting, enables the estimation of the growth and coalescence rates of the discrete phase. Industrial-scale process simulation for technical and economic analysis confirms that the total capture cost ($ 42.5/t CO2) can be reduced by ∼22% with the use of biphasic solvents and a centrifugal separator compared to conventional methods. This study introduces a fresh perspective on polarity-induced cluster generation and coagulation-induced separation, offering an effective solution to address the challenges associated with dynamic phase-splitting in biphasic solvents during practical applications.


Assuntos
Dióxido de Carbono , Solventes , Dióxido de Carbono/química , Solventes/química , Centrifugação , Gases/química
3.
Waste Manag ; 175: 62-72, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38171077

RESUMO

CO2 mineral sequestration using alkaline solid waste (ASW) is a promising strategy for synergistically reducing CO2 emissions and reusing industrial waste. However, improvement the carbonation degree still remains challenges due to the sluggish leaching rate of Ca/Mg ion at low pH. To the issues, this study proposed an amine-mediated CO2 absorption and mineralization process with six common ASWs, as well an ecological utilization route of CO2-ASW productions. Experimental results indicated that calcium carbide slag (CS) had greater CO2 mineralization capacity (86.2 g-CO2/kg-CS) than other ASWs, while stirring rate and particle size played a more important role during CO2 capture. Amine-mediated CO2 capture was verified to be more excellent with steel slag (SS) as mineral medium. When the MEA concentration was increased to 2 mol/L, the extraction efficiency of Ca2+ was increased by 35 %, leaded to the CO2 removal efficiency significantly promoted from 49 % to 92 %. The characterization of structural morphology referred spherical aragonite or needle-bar calcite was dominant for the porous mineralization products (30.6 m2/g). High germination index of pea seed (112.1 % at a dose of 10 g/L) inferred the negligible toxicological effects of tiny MEA residue over SS mineralization products, after centrifugally washing treatment. Pea seeds cultivated with mineralized products after centrifugal washing can achieve a growth rate of about 4 mm/d. Overall, this work provides a feasible route to apply the porous CO2-ASWs production into water conservation in arid and sandy land.


Assuntos
Dióxido de Carbono , Resíduos Sólidos , Dióxido de Carbono/química , Carbonato de Cálcio/química , Resíduos Industriais/análise , Minerais/química , Aço/química , Aminas
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