Investigating the temperature-dependent selectivity of CO2 reduction on Ru-cluster catalysts supported by MXene
The catalytic conversion of carbon dioxide (CO2) into valuable products represents a promising strategy for mitigating the greenhouse effect. However, developing catalysts that exhibit both high activity and selectivity remains a considerable challenge. Composite catalysts based on metal clusters su...
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| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Elsevier
2025-05-01
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| Series: | Journal of CO2 Utilization |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2212982025000721 |
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| Summary: | The catalytic conversion of carbon dioxide (CO2) into valuable products represents a promising strategy for mitigating the greenhouse effect. However, developing catalysts that exhibit both high activity and selectivity remains a considerable challenge. Composite catalysts based on metal clusters supported on MXene have emerged as a promising candidate for CO2 reduction. A thorough understanding of the catalytic mechanisms of CO2 reduction utilizing MXene-based catalysts is crucial for advancing and optimizing these catalysts. In this study, the detailed reaction mechanism of CO2 reduction on composite Run@Mo2TiC2O2 catalysts was investigated theoretically, employing the four-atom Ru4 cluster as the model system. Electronic structure analysis revealed that the orbital interactions between the Ru4 cluster and CO2 play a pivotal role in determining the adsorption configuration of the CO2 molecule. Specifically, CO2 exhibits distinct adsorption modes on planar and tetrahedral Ru4 clusters, leading to divergent CO2 reduction pathways. Density functional theory (DFT) calculations suggest that the tetrahedral Ru4 cluster demonstrates higher selectivity for the reduction of CO2 to carbon monoxide (CO) compared to the planar configuration. However, the results indicate that although the planar Ru4 cluster is predominant on the Mo2TiC2O2 surface at room temperature, there is a coexistence of planar and tetrahedral Ru4 clusters at the higher temperature used in photothermal catalysis. It suggests that the configuration of Ru4@Mo2TiC2O2 can be modulated by manipulating the reaction temperature, thereby adjusting the selectivity. This finding provides comprehensive insights into the CO2 reduction mechanism facilitated by MXene-supported metal cluster catalysts. This work also highlights that the impact of temperature on the catalytic activity and selectivity of catalysts comprising metal clusters should be subjected to more rigorous investigation. |
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| ISSN: | 2212-9839 |