Guo, Jiuli ; Liang, Yan ; Song, Rui ; Loh, Joel Y. Y. ; Kherani, Nazir P. ; Wang, Wu ; Kübel, Christian ; Dai, Ying ; Wang, Lu ; Ozin, Geoffrey A. (2021)
Construction of new active sites: Cu substitution enabled surface frustrated Lewis pairs over calcium hydroxyapatite for CO2 hydrogenation.
In: Advanced Science, 8 (17)
doi: 10.1002/advs.202101382
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
Calcium hydroxyphosphate, Ca-10(PO4)(6)(OH)(2), is commonly known as hydroxyapatite (HAP). The acidic calcium and basic phosphate/hydroxide sites in HAP can be modified via isomorphous substitution of calcium and/or hydroxide ions to enable a cornucopia of catalyzed reactions. Herein, isomorphic substitution of Ca2+ ions by Cu2+ ions especially at very low levels of exchange created new analogs of molecular surface frustrated Lewis pairs (SFLPs) in CuxCa10-x(PO4)(6)(OH)(2), thereby boosting its performance metrics in heterogeneous CO2 photocatalytic hydrogenation. In situ Fourier transform infrared spectroscopy characterization and density functional theory calculations provided fundamental insights into the catalytically active SFLPs defined as proximal Lewis acidic Cu2+ and Lewis basic OH-. The photocatalytic pathway proceeds through a formate reaction intermediate, which is generated by the reaction of CO2 with heterolytically dissociated H-2 on the SFLPs. Given the wealth of information thus uncovered, it is highly likely that this work will spur the further development of similar classes of materials, leading to the advancement and, ultimately, large-scale application of photocatalytic CO2 reduction technologies.
Typ des Eintrags: | Artikel |
---|---|
Erschienen: | 2021 |
Autor(en): | Guo, Jiuli ; Liang, Yan ; Song, Rui ; Loh, Joel Y. Y. ; Kherani, Nazir P. ; Wang, Wu ; Kübel, Christian ; Dai, Ying ; Wang, Lu ; Ozin, Geoffrey A. |
Art des Eintrags: | Bibliographie |
Titel: | Construction of new active sites: Cu substitution enabled surface frustrated Lewis pairs over calcium hydroxyapatite for CO2 hydrogenation |
Sprache: | Englisch |
Publikationsjahr: | September 2021 |
Verlag: | Wiley-VCH |
Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Advanced Science |
Jahrgang/Volume einer Zeitschrift: | 8 |
(Heft-)Nummer: | 17 |
DOI: | 10.1002/advs.202101382 |
Kurzbeschreibung (Abstract): | Calcium hydroxyphosphate, Ca-10(PO4)(6)(OH)(2), is commonly known as hydroxyapatite (HAP). The acidic calcium and basic phosphate/hydroxide sites in HAP can be modified via isomorphous substitution of calcium and/or hydroxide ions to enable a cornucopia of catalyzed reactions. Herein, isomorphic substitution of Ca2+ ions by Cu2+ ions especially at very low levels of exchange created new analogs of molecular surface frustrated Lewis pairs (SFLPs) in CuxCa10-x(PO4)(6)(OH)(2), thereby boosting its performance metrics in heterogeneous CO2 photocatalytic hydrogenation. In situ Fourier transform infrared spectroscopy characterization and density functional theory calculations provided fundamental insights into the catalytically active SFLPs defined as proximal Lewis acidic Cu2+ and Lewis basic OH-. The photocatalytic pathway proceeds through a formate reaction intermediate, which is generated by the reaction of CO2 with heterolytically dissociated H-2 on the SFLPs. Given the wealth of information thus uncovered, it is highly likely that this work will spur the further development of similar classes of materials, leading to the advancement and, ultimately, large-scale application of photocatalytic CO2 reduction technologies. |
Freie Schlagworte: | coppergas-phase reactions, hydroxyapatite, surface chemistry, surface frustrated Lewis pair |
ID-Nummer: | Artikel-ID: 2101382 |
Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > In-Situ Elektronenmikroskopie |
Hinterlegungsdatum: | 12 Jun 2024 08:15 |
Letzte Änderung: | 12 Jun 2024 08:15 |
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