Theoretical Investigation of Carbon Dioxide Adsorption on Li+-Decorated Nanoflakes.

Igor K Petrushenko,Nikolay A Ivanov,Konstantin B Petrushenko

doi:10.3390/molecules26247688

Igor K Petrushenko, Nikolay A Ivanov + Show 1 more

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https://doi.org/10.3390/molecules26247688

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Abstract

Recently, the capture of carbon dioxide, the primary greenhouse gas, has attracted particular interest from researchers worldwide. In the present work, several theoretical methods have been used to study adsorption of CO2 molecules on Li+-decorated coronene (Li+@coronene). It has been established that Li+ can be strongly anchored on coronene, and then a physical adsorption of CO2 will occur in the vicinity of this cation. Moreover, such a decoration has substantially improved interaction energy (Eint) between CO2 molecules and the adsorbent. One to twelve CO2 molecules per one Li+ have been considered, and their Eint values are in the range from −5.55 to −16.87 kcal/mol. Symmetry-adapted perturbation theory (SAPT0) calculations have shown that, depending on the quantity of adsorbed CO2 molecules, different energy components act as the main reason for attraction. AIMD simulations allow estimating gravimetric densities (GD, wt.%) at various temperatures, and the maximal GDs have been calculated to be 9.3, 6.0, and 4.9% at T = 77, 300, and 400 K, respectively. Besides this, AIMD calculations validate stability of Li+@coronene complexes during simulation time at the maximum CO2 loading. Bader’s atoms-in-molecules (QTAIM) and independent gradient model (IGM) techniques have been implemented to unveil the features of interactions between CO2 and Li+@coronene. These methods have proved that there exists a non-covalent bonding between the cation center and CO2. We suppose that findings, derived in this theoretical work, may also benefit the design of novel nanosystems for gas storage and delivery.

Highlights

Carbon dioxide (CO2) is a greenhouse gas that has severe environmental and health effects
density functional theory (DFT) and SAPT0 calculations of the 1–12 CO2 molecules adsorbed at Li+@coronene exhibit larger Eint values compared with those for pristine graphene, some of them do not satisfy the optimal energy range for CO2 storage
The ab initio molecular dynamics (AIMD) results show that the cation center of the Li+@coronene complex can favorably accommodate numerous CO2 molecules that leads to the maximal gravimetric density (GD) of 5.0 (9.3) wt.% for one-side adsorption

Summary

Introduction

Carbon dioxide (CO2) is a greenhouse gas that has severe environmental and health effects. Numerous steps have been proposed to overcome this problem, such as the use of renewable energy, a decrease of deforestation, and the decarbonization of buildings and infrastructure. These pathways need sophisticated equipment and large assets; the idea of direct capture and further conversion of CO2 becomes very appealing. The well-established technology is the chemical absorption in liquid amines This methodology, though, holds numerous drawbacks, such as low CO2 capacity, equipment corrosion, amine degradation by SO2, NO2, and O2 existed in the flue gases, low energy efficiency owing to the high temperatures utilized during absorbent regeneration, and, large size of the equipment [1]

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