High-performance single-atom M/TiO2 catalysts in the reverse water-gas shift reaction: A comprehensive experimental and theoretical investigation
Single-atom catalysts (SACs) offer high efficiency and selectivity in chemical reactions but face challenges in converting CO2 to CO via the reverse water gas shift (RWGS) reactions. This study addresses these challenges by anchoring three noble metals (Ir, Pd, and Ru) onto titania (TiO2) and analyz...
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Elsevier
2024-12-01
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| Series: | Journal of CO2 Utilization |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2212982024003238 |
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| author | Moshood O. Bolarinwa Aasif A. Dabbawala Shamraiz Hussain Talib Georgian Melinte Thomas Delclos Abdulmuizz Adamson Abbas Khaleel Kyriaki Polychronopoulou Dalaver H. Anjum |
| author_facet | Moshood O. Bolarinwa Aasif A. Dabbawala Shamraiz Hussain Talib Georgian Melinte Thomas Delclos Abdulmuizz Adamson Abbas Khaleel Kyriaki Polychronopoulou Dalaver H. Anjum |
| author_sort | Moshood O. Bolarinwa |
| collection | DOAJ |
| description | Single-atom catalysts (SACs) offer high efficiency and selectivity in chemical reactions but face challenges in converting CO2 to CO via the reverse water gas shift (RWGS) reactions. This study addresses these challenges by anchoring three noble metals (Ir, Pd, and Ru) onto titania (TiO2) and analyzing their performance. Comprehensive characterization techniques, including electron microscopy, confirmed the uniform dispersion of metal atoms on TiO2. Among the catalysts, Ir/TiO2 exhibited the best results, achieving an 84 % CO2 conversion rate and ∼98 % CO selectivity, surpassing Pd/TiO2 and Ru/TiO2, which gained 56 % and 52 % conversion, respectively. In-situ gas transmission electron microscopy revealed the catalytic behavior of Ir/TiO2, showing Ir atom mobility and the formation of ∼1 nm nanoclusters. Density functional theory (DFT) and in-situ diffuse reflectance infrared spectroscopy (DRIFTs) further explained that the atomically dispersed Ir sites in Ir/TiO2 follow a hydrogen-assisted mechanism, with the COOH* intermediate desorbing and dissociating into CO. These findings suggest SACs' potential to facilitate greener chemical processes and reduce greenhouse gas emissions. |
| format | Article |
| id | doaj-art-0084fc935be1448d8fe43355ee2fb588 |
| institution | OA Journals |
| issn | 2212-9839 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Journal of CO2 Utilization |
| spelling | doaj-art-0084fc935be1448d8fe43355ee2fb5882025-08-20T01:58:08ZengElsevierJournal of CO2 Utilization2212-98392024-12-019010298810.1016/j.jcou.2024.102988High-performance single-atom M/TiO2 catalysts in the reverse water-gas shift reaction: A comprehensive experimental and theoretical investigationMoshood O. Bolarinwa0Aasif A. Dabbawala1Shamraiz Hussain Talib2Georgian Melinte3Thomas Delclos4Abdulmuizz Adamson5Abbas Khaleel6Kyriaki Polychronopoulou7Dalaver H. Anjum8Department of Physics, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates; Center for Catalysis and Separation (CeCaS), Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab EmiratesCenter for Catalysis and Separation (CeCaS), Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates; Department of Mechanical Engineering, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab EmiratesCenter for Catalysis and Separation (CeCaS), Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates; Department of Chemistry, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab EmiratesKing Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi ArabiaMaterials and Surface Core Labs, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab EmiratesDepartment of Chemistry, United Arab Emirates University, Al-Ain, United Arab EmiratesDepartment of Chemistry, United Arab Emirates University, Al-Ain, United Arab EmiratesCenter for Catalysis and Separation (CeCaS), Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates; Department of Mechanical Engineering, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates; Corresponding authors at: Center for Catalysis and Separation (CeCaS), Khalifa University of Science and Technology Abu Dhabi 127788, United Arab EmiratesDepartment of Physics, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates; Center for Catalysis and Separation (CeCaS), Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates; Corresponding authors at: Center for Catalysis and Separation (CeCaS), Khalifa University of Science and Technology Abu Dhabi 127788, United Arab EmiratesSingle-atom catalysts (SACs) offer high efficiency and selectivity in chemical reactions but face challenges in converting CO2 to CO via the reverse water gas shift (RWGS) reactions. This study addresses these challenges by anchoring three noble metals (Ir, Pd, and Ru) onto titania (TiO2) and analyzing their performance. Comprehensive characterization techniques, including electron microscopy, confirmed the uniform dispersion of metal atoms on TiO2. Among the catalysts, Ir/TiO2 exhibited the best results, achieving an 84 % CO2 conversion rate and ∼98 % CO selectivity, surpassing Pd/TiO2 and Ru/TiO2, which gained 56 % and 52 % conversion, respectively. In-situ gas transmission electron microscopy revealed the catalytic behavior of Ir/TiO2, showing Ir atom mobility and the formation of ∼1 nm nanoclusters. Density functional theory (DFT) and in-situ diffuse reflectance infrared spectroscopy (DRIFTs) further explained that the atomically dispersed Ir sites in Ir/TiO2 follow a hydrogen-assisted mechanism, with the COOH* intermediate desorbing and dissociating into CO. These findings suggest SACs' potential to facilitate greener chemical processes and reduce greenhouse gas emissions.http://www.sciencedirect.com/science/article/pii/S2212982024003238Single atom catalyst (SACs)Reverse water gas shift (RWGS) reactionCO2 conversionNanoclusters (NCs)In-situ TEM |
| spellingShingle | Moshood O. Bolarinwa Aasif A. Dabbawala Shamraiz Hussain Talib Georgian Melinte Thomas Delclos Abdulmuizz Adamson Abbas Khaleel Kyriaki Polychronopoulou Dalaver H. Anjum High-performance single-atom M/TiO2 catalysts in the reverse water-gas shift reaction: A comprehensive experimental and theoretical investigation Journal of CO2 Utilization Single atom catalyst (SACs) Reverse water gas shift (RWGS) reaction CO2 conversion Nanoclusters (NCs) In-situ TEM |
| title | High-performance single-atom M/TiO2 catalysts in the reverse water-gas shift reaction: A comprehensive experimental and theoretical investigation |
| title_full | High-performance single-atom M/TiO2 catalysts in the reverse water-gas shift reaction: A comprehensive experimental and theoretical investigation |
| title_fullStr | High-performance single-atom M/TiO2 catalysts in the reverse water-gas shift reaction: A comprehensive experimental and theoretical investigation |
| title_full_unstemmed | High-performance single-atom M/TiO2 catalysts in the reverse water-gas shift reaction: A comprehensive experimental and theoretical investigation |
| title_short | High-performance single-atom M/TiO2 catalysts in the reverse water-gas shift reaction: A comprehensive experimental and theoretical investigation |
| title_sort | high performance single atom m tio2 catalysts in the reverse water gas shift reaction a comprehensive experimental and theoretical investigation |
| topic | Single atom catalyst (SACs) Reverse water gas shift (RWGS) reaction CO2 conversion Nanoclusters (NCs) In-situ TEM |
| url | http://www.sciencedirect.com/science/article/pii/S2212982024003238 |
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