Catalytic CO2 conversion to fuels and chemicals is important for mitigating the climate change and reducing the dependence on fossil resources. In order to achieve this goal on a large industrial level, effective catalysts need to be developed. Among them, gallium nitride (GaN) and related Mg-doped and In-alloyed systems have been proven as efficient materials for the reduction of highly stable CO2 molecules. This work presents a density functional theory (DFT) investigation, performing periodic boundary condition (PBC) calculations which allow to employ a more extended surface for a detailed analysis of the CO2 coverage, and the effect of Mg doping and In alloying on the CO2 adsorption and its conversion to CO. The results show the great potential of GaN(100) surfaces to simultaneously bind and strongly activate multiple CO2 molecules, which is a crucial aspect for an efficient CO2 conversion process. Moreover, the presence of Mg-dopant on the top layer is found to be more beneficial for the CO2 adsorption and activation with respect to both the pristine and In-alloyed system, and this effect is further improved by the inclusion of a second impurity on the top layer. In line with the previous experimental findings, these calculations support the potential of pristine GaN(100) to catalyze the CO2-to-CO reduction. The results presented here offer crucial information for the development of more efficient and selective catalysts for the CO2 reduction.
|Original language||English (US)|
|State||Published - Nov 22 2022|
Bibliographical noteKAUST Repository Item: Exported on 2022-12-23
Acknowledgements: I.R. thanks MIUR and European Union for AIM-International attraction and mobility call for researchers funded by PON RI 2014–2020. The Computational work was performed using the resources of the KAUST Super-computing Laboratory (KSL) at KAUST, and IT4Innovations National Supercomputer Center, supported by The Ministry of Education, Youth and Sports from the Large Infrastructures for Research, Experimental Development and Innovations Project “e-Infrastructure CZ – LM2018140”. CzechNanoLab project LM2018110 funded by MEYS CR is gratefully acknowledged for the financial support at CEITEC Nano Research Infrastructure.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.
ASJC Scopus subject areas
- Inorganic Chemistry
- Physical and Theoretical Chemistry
- Organic Chemistry