Theoretical Insights into Synergistic Effects at Cu/TiC Interfaces for Promoting CO2 Activation
| Autor: | Yongfan Zhang, Hegen Zhou, Bin Wang, Wei Lin, Shuping Huang, Wen-Kai Chen, Yi Li, Yanli Li, Zhongpu Fang |
|---|---|
| Rok vydání: | 2021 |
| Předmět: | |
| Zdroj: | ACS Omega, Vol 6, Iss 41, Pp 27259-27270 (2021) ACS Omega |
| ISSN: | 2470-1343 |
| Popis: | The adsorption behaviors of CO2 at the Cu n /TiC(001) interfaces (n = 1-8) have been investigated using the density functional theory method. Our results reveal that the introduction of copper clusters on a TiC surface can significantly improve the thermodynamic stability of CO2 chemisorption. However, the most stable adsorption site is sensitive to the size and morphology of Cu n particles. The interfacial configuration is the most stable structure for copper clusters with small (n ≤ 2) and large (n ≥ 8) sizes, in which both Cu particles and TiC support are involved in CO2 activation. In such a case, the synergistic behavior is associated with the ligand effect introduced by directly forming adsorption bonds with CO2. For those Cu n clusters with a medium size (n = 3-7), the configuration where CO2 adsorbs solely on the exposed hollow site constructed by Cu atoms at the interface shows the best stability, and the charger transfer becomes the primary origin of the synergistic effect in promoting CO2 activation. Since the most obvious deformation of CO2 is observed for the TiC(001)-surface-supported Cu4 and Cu7 particles, copper clusters with specific sizes of n = 4 and 7 exhibit the best ability for CO2 activation. Furthermore, the kinetic barriers for CO2 dissociation on Cu4- and Cu7-supported TiC surfaces are determined. The findings obtained in this work provide useful insights into optimizing the Cu/TiC interface with high catalytic activation of CO2 by precisely controlling the size and dispersion of copper particles. |
| Databáze: | OpenAIRE |
| Externí odkaz: |
|