Near-Barrierless CO Oxidation Using Phosphotungstic Acid-Supported Single-Atom Catalysts
Efficient CO oxidation at ambient or low temperatures is essential for environmental purification and selective CO oxidation in H2, yet achieving this remains a challenge with current methodologies. In this research, we extensively evaluated the catalytic performance of phosphotungstic acid (PTA)-su...
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| Published in | Inorganic chemistry Vol. 63; no. 29; pp. 13253 - 13264 |
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| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
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United States
American Chemical Society
22.07.2024
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| Abstract | Efficient CO oxidation at ambient or low temperatures is essential for environmental purification and selective CO oxidation in H2, yet achieving this remains a challenge with current methodologies. In this research, we extensively evaluated the catalytic performance of phosphotungstic acid (PTA)-supported 11 M1/PTA single-atom catalysts (SACs) using density functional theory calculations across both gas phase and 12 common solvents. The Rh1/PTA, Pd1/PTA, and Pt1/PTA systems exhibit moderate CO adsorption energies, facilitating the feasibility of oxygen vacancy formation. Remarkably, the Pd1/PTA and Pt1/PTA catalysts exhibited negligible energy barriers and demonstrated exceptionally high catalytic rates, with values reaching up to (1 × 1010)11, markedly exceeding the threshold for room temperature reactions, set at 6.55 × 108. This phenomenon is attributed to a transition from the high-energy barrier processes of oxygen dissociation in O2 and N–O bond dissociation in N2O to the more efficient dissociation of H2O2. Orbital analysis and charge variations at metal sites throughout the reaction process provide deeper insights into the role of the three metal catalytic sites in CO activation. Our findings not only reveal key aspects of SACs in facilitating CO oxidation at low temperatures but also provide valuable insights for future catalytic reaction mechanism studies and environmental applications. |
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| AbstractList | Efficient CO oxidation at ambient or low temperatures is essential for environmental purification and selective CO oxidation in H2, yet achieving this remains a challenge with current methodologies. In this research, we extensively evaluated the catalytic performance of phosphotungstic acid (PTA)-supported 11 M1/PTA single-atom catalysts (SACs) using density functional theory calculations across both gas phase and 12 common solvents. The Rh1/PTA, Pd1/PTA, and Pt1/PTA systems exhibit moderate CO adsorption energies, facilitating the feasibility of oxygen vacancy formation. Remarkably, the Pd1/PTA and Pt1/PTA catalysts exhibited negligible energy barriers and demonstrated exceptionally high catalytic rates, with values reaching up to (1 × 1010)11, markedly exceeding the threshold for room temperature reactions, set at 6.55 × 108. This phenomenon is attributed to a transition from the high-energy barrier processes of oxygen dissociation in O2 and N–O bond dissociation in N2O to the more efficient dissociation of H2O2. Orbital analysis and charge variations at metal sites throughout the reaction process provide deeper insights into the role of the three metal catalytic sites in CO activation. Our findings not only reveal key aspects of SACs in facilitating CO oxidation at low temperatures but also provide valuable insights for future catalytic reaction mechanism studies and environmental applications. Efficient CO oxidation at ambient or low temperatures is essential for environmental purification and selective CO oxidation in H2, yet achieving this remains a challenge with current methodologies. In this research, we extensively evaluated the catalytic performance of phosphotungstic acid (PTA)-supported 11 M1/PTA single-atom catalysts (SACs) using density functional theory calculations across both gas phase and 12 common solvents. The Rh1/PTA, Pd1/PTA, and Pt1/PTA systems exhibit moderate CO adsorption energies, facilitating the feasibility of oxygen vacancy formation. Remarkably, the Pd1/PTA and Pt1/PTA catalysts exhibited negligible energy barriers and demonstrated exceptionally high catalytic rates, with values reaching up to (1 × 1010)11, markedly exceeding the threshold for room temperature reactions, set at 6.55 × 108. This phenomenon is attributed to a transition from the high-energy barrier processes of oxygen dissociation in O2 and N-O bond dissociation in N2O to the more efficient dissociation of H2O2. Orbital analysis and charge variations at metal sites throughout the reaction process provide deeper insights into the role of the three metal catalytic sites in CO activation. Our findings not only reveal key aspects of SACs in facilitating CO oxidation at low temperatures but also provide valuable insights for future catalytic reaction mechanism studies and environmental applications.Efficient CO oxidation at ambient or low temperatures is essential for environmental purification and selective CO oxidation in H2, yet achieving this remains a challenge with current methodologies. In this research, we extensively evaluated the catalytic performance of phosphotungstic acid (PTA)-supported 11 M1/PTA single-atom catalysts (SACs) using density functional theory calculations across both gas phase and 12 common solvents. The Rh1/PTA, Pd1/PTA, and Pt1/PTA systems exhibit moderate CO adsorption energies, facilitating the feasibility of oxygen vacancy formation. Remarkably, the Pd1/PTA and Pt1/PTA catalysts exhibited negligible energy barriers and demonstrated exceptionally high catalytic rates, with values reaching up to (1 × 1010)11, markedly exceeding the threshold for room temperature reactions, set at 6.55 × 108. This phenomenon is attributed to a transition from the high-energy barrier processes of oxygen dissociation in O2 and N-O bond dissociation in N2O to the more efficient dissociation of H2O2. Orbital analysis and charge variations at metal sites throughout the reaction process provide deeper insights into the role of the three metal catalytic sites in CO activation. Our findings not only reveal key aspects of SACs in facilitating CO oxidation at low temperatures but also provide valuable insights for future catalytic reaction mechanism studies and environmental applications. Efficient CO oxidation at ambient or low temperatures is essential for environmental purification and selective CO oxidation in H , yet achieving this remains a challenge with current methodologies. In this research, we extensively evaluated the catalytic performance of phosphotungstic acid (PTA)-supported 11 M /PTA single-atom catalysts (SACs) using density functional theory calculations across both gas phase and 12 common solvents. The Rh /PTA, Pd /PTA, and Pt /PTA systems exhibit moderate CO adsorption energies, facilitating the feasibility of oxygen vacancy formation. Remarkably, the Pd /PTA and Pt /PTA catalysts exhibited negligible energy barriers and demonstrated exceptionally high catalytic rates, with values reaching up to (1 × 10 ) , markedly exceeding the threshold for room temperature reactions, set at 6.55 × 10 . This phenomenon is attributed to a transition from the high-energy barrier processes of oxygen dissociation in O and N-O bond dissociation in N O to the more efficient dissociation of H O . Orbital analysis and charge variations at metal sites throughout the reaction process provide deeper insights into the role of the three metal catalytic sites in CO activation. Our findings not only reveal key aspects of SACs in facilitating CO oxidation at low temperatures but also provide valuable insights for future catalytic reaction mechanism studies and environmental applications. |
| Author | Li, Shiyu Xu, Feng Yang, Song Chen, Dandan Zhang, Jian Wang, Kaijie Yang, Anqi Zhang, Li-Long |
| AuthorAffiliation | Key Laboratory of Material Chemistry for Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Huazhong Institute of New Type Optoelectronic Materials and Technology, College of Big Data and Information Engineering Center for R&D of Fine Chemicals of Guizhou University National Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, State-Local Joint Laboratory for Comprehensive Utilization of Biomass School of Chemistry and Chemical Engineering Guizhou University |
| AuthorAffiliation_xml | – name: Guizhou University – name: Institute of New Type Optoelectronic Materials and Technology, College of Big Data and Information Engineering – name: National Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, State-Local Joint Laboratory for Comprehensive Utilization of Biomass – name: School of Chemistry and Chemical Engineering – name: Center for R&D of Fine Chemicals of Guizhou University – name: Key Laboratory of Material Chemistry for Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Huazhong |
| Author_xml | – sequence: 1 givenname: Kaijie surname: Wang fullname: Wang, Kaijie organization: Guizhou University – sequence: 2 givenname: Shiyu surname: Li fullname: Li, Shiyu organization: Center for R&D of Fine Chemicals of Guizhou University – sequence: 3 givenname: Anqi surname: Yang fullname: Yang, Anqi organization: Institute of New Type Optoelectronic Materials and Technology, College of Big Data and Information Engineering – sequence: 4 givenname: Dandan surname: Chen fullname: Chen, Dandan organization: Center for R&D of Fine Chemicals of Guizhou University – sequence: 5 givenname: Feng surname: Xu fullname: Xu, Feng organization: Center for R&D of Fine Chemicals of Guizhou University – sequence: 6 givenname: Li-Long orcidid: 0000-0003-4724-913X surname: Zhang fullname: Zhang, Li-Long email: zhanglilong125@163.com organization: Center for R&D of Fine Chemicals of Guizhou University – sequence: 7 givenname: Jian orcidid: 0000-0001-7584-3799 surname: Zhang fullname: Zhang, Jian email: zhangjian7@hust.edu.cn organization: Key Laboratory of Material Chemistry for Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Huazhong – sequence: 8 givenname: Song orcidid: 0000-0003-1301-3030 surname: Yang fullname: Yang, Song email: jhzx.msm@gmail.com organization: Center for R&D of Fine Chemicals of Guizhou University |
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| Snippet | Efficient CO oxidation at ambient or low temperatures is essential for environmental purification and selective CO oxidation in H2, yet achieving this remains... Efficient CO oxidation at ambient or low temperatures is essential for environmental purification and selective CO oxidation in H , yet achieving this remains... |
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| Title | Near-Barrierless CO Oxidation Using Phosphotungstic Acid-Supported Single-Atom Catalysts |
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