Thermal Management Approach to Stabilization of Disordered Active Sites for Sabatier Reaction
Abstract The transition metal nanocatalysts containing disordered active sites can potentially achieve efficient Sabatier reactions with high selectivity. However, it remains a challenge to maintain the stability of these active sites in such an exothermic reaction. Here, a thermal management approa...
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| Format: | Article |
| Language: | English |
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Wiley
2025-01-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202409048 |
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| author | Delong Duan Di Wu Hongwei Shou Chuansheng Hu Canyu Hu Min Zhou Ran Long Yingpu Bi Yujie Xiong |
| author_facet | Delong Duan Di Wu Hongwei Shou Chuansheng Hu Canyu Hu Min Zhou Ran Long Yingpu Bi Yujie Xiong |
| author_sort | Delong Duan |
| collection | DOAJ |
| description | Abstract The transition metal nanocatalysts containing disordered active sites can potentially achieve efficient Sabatier reactions with high selectivity. However, it remains a challenge to maintain the stability of these active sites in such an exothermic reaction. Here, a thermal management approach is reported to address this challenge. Specifically, an efficient and stable catalytic system is developed by integrating urchin‐like Ru nanoparticles with disordered active sites (d‐RuNUs) and multi‐walled carbon nanotubes (MWCNTs) as heat transfer framework, which achieves a CH4 yield of 3.3 mol g−1 h−1 with nearly 100% selectivity in 12 h. The characterizations reveal that the thermal‐induced crystallization seriously weakens the adsorption of CO2, leading to significant degradation of catalytic performance. The heat transfer simulation confirms that the MWCNTs with high thermal conductivity play a key role in rapidly redistributing the reaction heat, thereby preventing the crystallization of disordered structures. This work elucidates the deactivation mechanism of disordered active sites in exothermic reactions and opens the avenue for local thermal management of non‐thermal equilibrium reactions. |
| format | Article |
| id | doaj-art-971c27efbd8f4fa3a4657fa8200393f4 |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-971c27efbd8f4fa3a4657fa8200393f42025-01-29T09:50:19ZengWileyAdvanced Science2198-38442025-01-01124n/an/a10.1002/advs.202409048Thermal Management Approach to Stabilization of Disordered Active Sites for Sabatier ReactionDelong Duan0Di Wu1Hongwei Shou2Chuansheng Hu3Canyu Hu4Min Zhou5Ran Long6Yingpu Bi7Yujie Xiong8Hefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials Science National Synchrotron Radiation Laboratory School of Nuclear Science and Technology University of Science and Technology of China Hefei Anhui 230026 ChinaHefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials Science National Synchrotron Radiation Laboratory School of Nuclear Science and Technology University of Science and Technology of China Hefei Anhui 230026 ChinaHefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials Science National Synchrotron Radiation Laboratory School of Nuclear Science and Technology University of Science and Technology of China Hefei Anhui 230026 ChinaHefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials Science National Synchrotron Radiation Laboratory School of Nuclear Science and Technology University of Science and Technology of China Hefei Anhui 230026 ChinaHefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials Science National Synchrotron Radiation Laboratory School of Nuclear Science and Technology University of Science and Technology of China Hefei Anhui 230026 ChinaHefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials Science National Synchrotron Radiation Laboratory School of Nuclear Science and Technology University of Science and Technology of China Hefei Anhui 230026 ChinaHefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials Science National Synchrotron Radiation Laboratory School of Nuclear Science and Technology University of Science and Technology of China Hefei Anhui 230026 ChinaState Key Laboratory for Oxo Synthesis and Selective Oxidation National Engineering Research Center for Fine Petrochemical Intermediates Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou Gansu 730000 ChinaHefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials Science National Synchrotron Radiation Laboratory School of Nuclear Science and Technology University of Science and Technology of China Hefei Anhui 230026 ChinaAbstract The transition metal nanocatalysts containing disordered active sites can potentially achieve efficient Sabatier reactions with high selectivity. However, it remains a challenge to maintain the stability of these active sites in such an exothermic reaction. Here, a thermal management approach is reported to address this challenge. Specifically, an efficient and stable catalytic system is developed by integrating urchin‐like Ru nanoparticles with disordered active sites (d‐RuNUs) and multi‐walled carbon nanotubes (MWCNTs) as heat transfer framework, which achieves a CH4 yield of 3.3 mol g−1 h−1 with nearly 100% selectivity in 12 h. The characterizations reveal that the thermal‐induced crystallization seriously weakens the adsorption of CO2, leading to significant degradation of catalytic performance. The heat transfer simulation confirms that the MWCNTs with high thermal conductivity play a key role in rapidly redistributing the reaction heat, thereby preventing the crystallization of disordered structures. This work elucidates the deactivation mechanism of disordered active sites in exothermic reactions and opens the avenue for local thermal management of non‐thermal equilibrium reactions.https://doi.org/10.1002/advs.202409048disordered active sitesheterogeneous catalysisSabatier reactionThermal managementthermochemistry |
| spellingShingle | Delong Duan Di Wu Hongwei Shou Chuansheng Hu Canyu Hu Min Zhou Ran Long Yingpu Bi Yujie Xiong Thermal Management Approach to Stabilization of Disordered Active Sites for Sabatier Reaction Advanced Science disordered active sites heterogeneous catalysis Sabatier reaction Thermal management thermochemistry |
| title | Thermal Management Approach to Stabilization of Disordered Active Sites for Sabatier Reaction |
| title_full | Thermal Management Approach to Stabilization of Disordered Active Sites for Sabatier Reaction |
| title_fullStr | Thermal Management Approach to Stabilization of Disordered Active Sites for Sabatier Reaction |
| title_full_unstemmed | Thermal Management Approach to Stabilization of Disordered Active Sites for Sabatier Reaction |
| title_short | Thermal Management Approach to Stabilization of Disordered Active Sites for Sabatier Reaction |
| title_sort | thermal management approach to stabilization of disordered active sites for sabatier reaction |
| topic | disordered active sites heterogeneous catalysis Sabatier reaction Thermal management thermochemistry |
| url | https://doi.org/10.1002/advs.202409048 |
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