Role of Functional Groups in ILs Decorated Au(111) Surface for CO2 Capture and Activation: A First Principle Approach

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Published Sep 16, 2021
Kamalakannan Shanmugasundaram Prakash Muthuramalingam Maiyelvaganan K. Rudharachari

Abstract

A heterogeneous catalytic environment (electrode/electrolyte) plays a major role to decide the catalytic activation and conversion of the CO2 molecule at the interface.[1,2] In this work, we have performed first-principle calculations to study the adsorption mechanism of CO2 at the electrode-electrolyte interface. To examine this, we have selected functionalized ionic liquid (IL) decorated Au(111) surface. For this, we have chosen functionalized 1-ethyl-3-methylimidazolium cation (i.e. [EMIm-Z]+[X]-; Where, Z = NH2 and CF3) with two different anions (i.e. [X]- = [DCA]- and [SCN]-). To study the effect of functional groups in the alkyl chain, we have selected both electron-donating (i.e., –NH2) and electron-withdrawing (i.e. –CF3) groups with two different anions. Our results reveal that the electron donating groups ILs@Au(111) surface effectively activates and converts CO2 to  radical anion. But the electron-withdrawing (i.e. –CF3) substituent lowers the binding strength of CO2 and it slightly affects the electronic structure of the CO2 molecule. Besides, the adsorption and activation mechanism of CO2 at the interface is directly influenced by the involvement of the -NH2 functional groups in the ([EMIm]+) cation. It is identified that the different types of intermolecular interactions between the CO2 and interface. Such as, (i) O=C=O····H(-NH2) (ii) O=C=O····H (-CH3)) (iii) O=C=O····F(-CF3). In addition, we have computed vibrational level changes in the CO2 molecule during the interaction at the interface. The shift in vibrational frequency confirms that activation of CO2 occurred due to the introduction of functional group in ILs. Our work provides a clear picture of the role of a functional group on the solid-liquid interface for the activation of CO2. Hence, our study provides a guideline to the design and development of the functional materials for the selective carbon capture, activation, and conversion of CO2 into other value-added products.[3]

How to Cite

Shanmugasundaram, K., Muthuramalingam, P., & K. Rudharachari , M. (2021). Role of Functional Groups in ILs Decorated Au(111) Surface for CO2 Capture and Activation: A First Principle Approach . SPAST Abstracts, 1(01). Retrieved from https://spast.org/techrep/article/view/663
Abstract 60 |

Article Details

Keywords

Au(111) Surface, CO2 Activation, Functionalized ILs, electron-donating/withdrawing groups, electrode-electrolyte interface,.

References
[1] A. Liu, M. Gao, X. Ren, F. Meng, Y. Yang, L. Gao, Q. Yang, T. Ma, J. Mater. Chem. A. 8, 3541–3562 (2020). https://doi:10.1039/c9ta11966c.
[2] A. Parameswari, Y. Soujanya, G.N. Sastry, J. Phys. Chem. C. 123, 3491–3504 (2019). https://doi.org/10.1021/acs.jpcc.8b09311
[3] S. Kamalakannan, K. Rudharachari Maiyelvaganan, K. Palanisamy, A. Thomas, R. Ben Said, M. Prakash, M. Hochlaf, Chemosphere. 286 (2022) 131612. https://doi:10.1016/j.chemosphere.2021.131612.
Section
NS2: Chemistry