Synergistic interplay of dual active sites on spinel ZnAl2O4 for syngas conversion
The urgent need for efficiency improvement in the oxide-zeolite bifunctional syngas-to-hydrocarbon catalysis necessitates in-depth mechanistic insights into this reaction, especially for the initial syngas conversion over the oxide component, which remains poor. Herein, we comprehensively investigat...
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| Published in: | Chem 2023-03, Vol.9 (3), p.721-738 |
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| Main Authors: | , , , , , , , , |
| Format: | Article |
| Language: | eng |
| Subjects: | |
| Online Access: | Get full text |
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| Summary: | The urgent need for efficiency improvement in the oxide-zeolite bifunctional syngas-to-hydrocarbon catalysis necessitates in-depth mechanistic insights into this reaction, especially for the initial syngas conversion over the oxide component, which remains poor. Herein, we comprehensively investigated syngas conversion over a representative ZnAl2O4 spinel oxide with state-of-the-art solid-state NMR technologies. Notably, specific surface dual active sites for syngas activation with –AlIV–OH···ZnIII– structure were unambiguously identified. More importantly, the dynamic evolution of the reaction intermediates and active sites during the reaction process was elaborated at atomic level by a series of double resonance and multi-dimensional correlation NMR experiments. In combination with in situ spectroscopic characterizations, we revealed the full cycle of the formate-methoxy-based pathway for the syngas-to-methanol conversion via synergistic interplay of the dual active sites. The in-depth atomic-level understanding of the catalytic mechanism will be beneficial to further rational design of high-performance catalysts for syngas conversion.
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•Specific surface dual active sites on ZnAl2O4 for syngas conversion are identified•Dynamic interaction between the active sites and intermediates is elaborated•Synergistic interplay of heteroatoms for syngas conversion is revealed
The catalytic syngas conversion is the key route to bridge the gap between various carbon resources and the essential chemicals. Recently, the oxide-zeolite (OXZEO) bifunctional catalysis has emerged as a new platform for this conversion, showing a great potential for further industrialization. However, to become a strong competitor to the conventional Fischer-Tropsch synthesis (FTS), a breakthrough in syngas conversion of OXZEO catalysis is highly demanded, which relies on the in-depth understanding of the structure-activity relationship of the catalysts/reaction, especially on oxide component. Here, we unambiguously identified the specific surface dual active sites on the bimetallic oxide catalyst, and their dynamic evolution with the reactants/intermediates in the syngas activation and conversion, using advanced solid-state NMR techniques. The detailed synergistic effect of heteroatoms for syngas conversion was revealed for the first time at atomic level, which will significantly benefit further rational design of high-efficiency catalysts.
Hou and co-workers carried out mec |
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| ISSN: | 2451-9294 2451-9294 |