Efficient CO₂ adsorption and mechanism on nitrogen-doped porous carbons

Abstract

In this work, nitrogen-doped porous carbons (NACs) were fabricated as an adsorbent by urea modification and KOH activation. The CO₂ adsorption mechanism for the NACs was then explored. The NACs are found to present a large specific surface area (1920.72– 3078.99 m²·g⁻¹) and high micropore percentage (61.60%–76.23%). Under a pressure of 1 bar, sample NAC-650-650 shows the highest CO₂ adsorption capacity up to 5.96 and 3.92 mmol·g⁻¹ at 0 and 25 °C, respectively. In addition, the CO₂/N₂ selectivity of NAC-650-650 is 79.93, much higher than the value of 49.77 obtained for the nonnitrogen-doped carbon AC-650-650. The CO₂ adsorption capacity of the NAC-650-650 sample maintains over 97% after ten cycles. Analysis of the results show that the CO₂ capacity of the NACs has a linear correlation (R² = 0.9633) with the cumulative pore volume for a pore size less than 1.02 nm. The presence of nitrogen and oxygen enhances the CO₂/N₂ selectivity, and pyrrole-N and hydroxy groups contribute more to the CO₂ adsorption. In situ Fourier transform infrared spectra analysis indicates that CO₂ is adsorbed onto the NACs as a gas. Furthermore, the physical adsorption mechanism is confirmed by adsorption kinetic models and the isosteric heat, and it is found to be controlled by CO₂ diffusion. The CO₂ adsorption kinetics for NACs at room temperature and in pure CO₂ is in accordance with the pseudo-first-order model and Avramís fractional-order kinetic model.

Key words： porous carbon; CO₂ adsorption; nitrogen-doped; adsorption mechanism; kinetics

Acknowledgments

This work is funded by the National Key Research and Development Program of China (Grant No. 2018YFB0605401); the National Natural Science Foundation of China (Grant No. 21868025); the National First-rate Discipline Construction Project of Ningxia (No. NXYLXK2017A04); the Key Research and Development Program of Ningxia Province, China (No. 2018BCE01002); and Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (Grant No. 2020-KF-39).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-020-1967-0 and is accessible for authorized users.

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