Design of CO2 hydrogenation catalysts based on phosphane/borane frustrated Lewis pairs and xanthene-derived scaffolds
New naphtho[2,1,8,7-klmn]xanthene and benzo[kl]xanthene-based intramolecular phosphane–borane frustrated Lewis pairs (FLPs) were investigated in catalyzed H2 activation and CO2 hydrogenation processes. According to DFT predictions at the B3LYP-D3 level, the presence of rigid scaffolds and increased...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
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Elsevier
2022-02-01
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| Series: | Catalysis Communications |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S1566736721001084 |
| _version_ | 1819097781117124608 |
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| author | Maicon Delarmelina José Walkimar de M. Carneiro C. Richard A. Catlow Michael Bühl |
| author_facet | Maicon Delarmelina José Walkimar de M. Carneiro C. Richard A. Catlow Michael Bühl |
| author_sort | Maicon Delarmelina |
| collection | DOAJ |
| description | New naphtho[2,1,8,7-klmn]xanthene and benzo[kl]xanthene-based intramolecular phosphane–borane frustrated Lewis pairs (FLPs) were investigated in catalyzed H2 activation and CO2 hydrogenation processes. According to DFT predictions at the B3LYP-D3 level, the presence of rigid scaffolds and increased P···B distances in the investigated FLPs lead to a remarkable drop in the energy barrier for CO2 hydrogenation (by up to 19.2 kcal mol−1, compared to the parent dimethylxanthene-based FLP). Furthermore, the energy differences between the transition states for H2 activation and CO2 hydrogenation are significantly reduced, making both processes feasible under relatively mild experimental conditions. |
| first_indexed | 2024-12-22T00:20:32Z |
| format | Article |
| id | doaj.art-08d5108ead854d0496f9fa1b682e1ae2 |
| institution | Directory Open Access Journal |
| issn | 1873-3905 |
| language | English |
| last_indexed | 2024-12-22T00:20:32Z |
| publishDate | 2022-02-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Catalysis Communications |
| spelling | doaj.art-08d5108ead854d0496f9fa1b682e1ae22022-12-21T18:45:10ZengElsevierCatalysis Communications1873-39052022-02-01162106385Design of CO2 hydrogenation catalysts based on phosphane/borane frustrated Lewis pairs and xanthene-derived scaffoldsMaicon Delarmelina0José Walkimar de M. Carneiro1C. Richard A. Catlow2Michael Bühl3School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK; UK Catalysis Hub, Research Complex at Harwell, STFC Rutherford Appleton Laboratory, Didcot, Oxfordshire OX11 0FA, UK; Corresponding author at: School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK.Instituto de Química, Universidade Federal Fluminense, Niterói, Rio de Janeiro 24020-141, BrazilSchool of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK; UK Catalysis Hub, Research Complex at Harwell, STFC Rutherford Appleton Laboratory, Didcot, Oxfordshire OX11 0FA, UK; Department of Chemistry, University College London, 20 Gordon St, London WC1 HOAJ, UKSchool of Chemistry, University of St Andrews, North Haugh, St Andrews, KY16 9ST Fife, United KingdomNew naphtho[2,1,8,7-klmn]xanthene and benzo[kl]xanthene-based intramolecular phosphane–borane frustrated Lewis pairs (FLPs) were investigated in catalyzed H2 activation and CO2 hydrogenation processes. According to DFT predictions at the B3LYP-D3 level, the presence of rigid scaffolds and increased P···B distances in the investigated FLPs lead to a remarkable drop in the energy barrier for CO2 hydrogenation (by up to 19.2 kcal mol−1, compared to the parent dimethylxanthene-based FLP). Furthermore, the energy differences between the transition states for H2 activation and CO2 hydrogenation are significantly reduced, making both processes feasible under relatively mild experimental conditions.http://www.sciencedirect.com/science/article/pii/S1566736721001084Frustrated Lewis pairXantheneCO2 hydrogenationFormic acidDFT |
| spellingShingle | Maicon Delarmelina José Walkimar de M. Carneiro C. Richard A. Catlow Michael Bühl Design of CO2 hydrogenation catalysts based on phosphane/borane frustrated Lewis pairs and xanthene-derived scaffolds Catalysis Communications Frustrated Lewis pair Xanthene CO2 hydrogenation Formic acid DFT |
| title | Design of CO2 hydrogenation catalysts based on phosphane/borane frustrated Lewis pairs and xanthene-derived scaffolds |
| title_full | Design of CO2 hydrogenation catalysts based on phosphane/borane frustrated Lewis pairs and xanthene-derived scaffolds |
| title_fullStr | Design of CO2 hydrogenation catalysts based on phosphane/borane frustrated Lewis pairs and xanthene-derived scaffolds |
| title_full_unstemmed | Design of CO2 hydrogenation catalysts based on phosphane/borane frustrated Lewis pairs and xanthene-derived scaffolds |
| title_short | Design of CO2 hydrogenation catalysts based on phosphane/borane frustrated Lewis pairs and xanthene-derived scaffolds |
| title_sort | design of co2 hydrogenation catalysts based on phosphane borane frustrated lewis pairs and xanthene derived scaffolds |
| topic | Frustrated Lewis pair Xanthene CO2 hydrogenation Formic acid DFT |
| url | http://www.sciencedirect.com/science/article/pii/S1566736721001084 |
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