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Photocatalytic Reduction of CO$_2$ by Highly Efficient Homogeneous Fe$^{II}$ Catalyst based on 2,6‐Bis(1’,2’,3’‐triazolyl‐methyl)pyridine - Comparison with Analogues

Gracia, Lisa Lou ORCID iD icon 1; Barani, Elham 2; Braun, Jonas ORCID iD icon 3; Carter, Anthony B. 4; Fuhr, Olaf ORCID iD icon 2,5; Powell, Annie K. 2,3; Fink, Karin ORCID iD icon 2; Bizzarri, Claudia 1
1 Institut für Organische Chemie (IOC), Karlsruher Institut für Technologie (KIT)
2 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)
3 Institut für Anorganische Chemie (AOC), Karlsruher Institut für Technologie (KIT)
4 Karlsruher Institut für Technologie (KIT)
5 Karlsruhe Nano Micro Facility (KNMF), Karlsruher Institut für Technologie (KIT)

Abstract:

Fully earth-abundant and highly efficient systems for producing syngas CO/H$_2$ through photocatalytic reduction from CO$_2$ are essential to approach a sustainable way of closing the carbon cycle. Herein, the synthesis and characterization of a new iron complex, Fe$^{II}$L(NCS)$_2$py, coordinated to an N,N,N-pincer ligand 2,6-bis(4’-phenyl-1’,2’,3’-triazol-1’-yl-methyl)pyridine (L), two isothiocyanate groups (NCS) and one pyridine is reported. Its catalytic activity in the photo-driven reduction of carbon dioxide has been investigated and compared with its Co$^{II}$ analogue (CoL(NCS)$_2$py) and their homoleptic complexes ML$_2$. In this work, the catalysts are used in combination with the heteroleptic complex [Cu$^I$(dmp)(DPEphos)], where dmp is 2,9-dimethyl-1,10-phenanthroline and DPEPhos is bis[(2-diphenylphosphino)phenyl] ether, to reach entirely earth-abundant systems. The new iron heteroleptic complex Fe$^{II}$L(NCS)$_2$py showed considerable activity with a TON$_{CO}$ of 576 obtained after 4 h (TOF=144 h$^{−1}$) through visible light (λ=420 nm) and a quantum yield of 7.1 %.


Verlagsausgabe §
DOI: 10.5445/IR/1000153044
Veröffentlicht am 25.11.2022
Originalveröffentlichung
DOI: 10.1002/cctc.202201163
Scopus
Zitationen: 5
Dimensions
Zitationen: 5
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Anorganische Chemie (AOC)
Institut für Nanotechnologie (INT)
Institut für Organische Chemie (IOC)
Publikationstyp Zeitschriftenaufsatz
Publikationsmonat/-jahr 12.2022
Sprache Englisch
Identifikator ISSN: 1867-3880, 1867-3899
KITopen-ID: 1000153044
HGF-Programm 43.32.01 (POF IV, LK 01) Molecular Materials Basis for Optics & Photonics
Erschienen in ChemCatChem
Verlag Wiley-VCH Verlag
Band 14
Heft 23
Seiten Art.-Nr.: e202201163
Vorab online veröffentlicht am 07.10.2022
Schlagwörter carbon dioxide reduction, earth-abundant materials, iron complexes, noble-metal free artificial photosynthesis, syngas
Nachgewiesen in Scopus
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