Experimental kinetics and thermodynamics investigation: Chemically activated carbon-enriched monolithic reduced graphene oxide for efficient CO2 capture

Ranjeet Kumar Jha; Haripada Bhunia; Soumen Basu

doi:10.1016/j.heliyon.2024.e27439

Experimental kinetics and thermodynamics investigation: Chemically activated carbon-enriched monolithic reduced graphene oxide for efficient CO₂ capture

Heliyon. 2024 Mar 2;10(5):e27439. doi: 10.1016/j.heliyon.2024.e27439. eCollection 2024 Mar 15.

Authors

Ranjeet Kumar Jha¹, Haripada Bhunia², Soumen Basu¹

Affiliations

¹ Department of Chemistry and Biochemistry, Thapar Institute of Engineering and Technology, Patiala-147004, Punjab, India.
² Department of Chemical Engineering, Thapar Institute of Engineering and Technology, Patiala-147004, Punjab, India.

Abstract

In this research, we have developed solid MGOs by self-assembled reduction process of GO at 90 °C with different weight ratios of oxalic acid (1:1, 1:0.500, and 1:0.250). The as-synthesized monoliths were carbonized (at 600 °C) and chemically activated with varying proportions of NaOH (1:1, 1:2, and 1:3). This materials offer the CO₂ adsorption effect under dynamic conditions, fast mass transfer, easy handling, and outstanding stability throughout the adsorption-desorption cycle. FE-SEM, and HR-TEM analyses confirmed the porous nature and shape of the adsorbents, while XPS examination revealed the presence of distinct functional groups on the surface of the monolith. By increasing the mass ratios (MGO:NaOH) from 1:1 to 1:2, the surface areas increased by approximately 2.6 times, ranging from 520.8 to 753.9 m² g⁻¹ (surface area of the untreated MGO was 289.2 m² g⁻¹). Consequently, this resulted in a notable enhancement of 2.10 mmol g⁻¹ in dynamic CO₂ capture capacity. The assessment encompassed the evaluation of production yield, selectivity, regenerability, kinetics, equilibrium isotherm, and isosteric temperatures of adsorption (Q_st). The decrease in CO₂ capture effectiveness with rising adsorption temperature indicated an exothermic and physisorption process. The regenerability of 99.1 % at 100 °C and excellent cyclic stability with efficient CO₂ adsorption make this monolithic adsorbent appropriate for post-combustion CO₂ capture. The significant Q_st lend support to the heterogeneity of the adsorbent's surface, and the pseudo-second-order kinetic model along with the Freundlich isotherm model emerged as the most fitting. Therefore, the current investigation shows that the carbon-enriched adsorbents enhance the CO₂ adsorption capacity. It may be used as a low-cost pretreatment method on an industrial scale before carbon capture.

Keywords: CO2 capture; Chemically activated; Graphene-oxide; Kinetic study; Monolith; Thermodynamic study.