Green Chemistry; Solar Light; Hydrogen; Sustainability; CO2 conversion; Photocatalysis
Mosberger Mathias, Probst Benjamin, Spingler Bernhard, Alberto Roger (2019), Influence of Hetero-Biaryl Ligands on the Photo-Electrochemical Properties of [Re I NCS(N ∩ N)(CO) 3 ]-Type Photosensitizers Influence of Hetero-Biaryl Ligands on the Photo-Electrochemical Properties of [Re I NCS(N ∩ N)(CO) 3 ]-Type Photosensitizers, in European Journal of Inorganic Chemistry
, 2019(30), 3518-3525.
Mokolokolo Pennie P., Frei Angelo, Tsosane Mampotso S., Kama Dumisani V., Schutte-Smith Marietjie, Brink Alice, Visser Hendrik G., Meola Giuseppe, Alberto Roger, Roodt Andreas (2018), Nuclearity manipulation in Schiff-base fac -tricarbonyl complexes of Mn(I) and Re(I), in Inorganica Chimica Acta
, 471, 249-256.
Raleaooa Pule V., Roodt Andreas, Mhlongo Gugu G., Motaung David E., Ntwaeaborwa Odireleng M. (2018), Analysis of the structure, particle morphology and photoluminescent properties of ZnS:Mn 2+ nanoparticulate phosphors, in Optik - International Journal for Light and Electron Optics
, 153, 31-42.
Zbačnik Marija, Pičuljan Katarina, Parlov-Vuković Jelena, Novak Predrag, Roodt Andreas (2017), Four Thermochromic o-Hydroxy Schiff Bases of α-Aminodiphenylmethane: Solution and Solid State Study, in Crystals
, 7(12), 25-25.
Schnidrig Stephan, Bachmann Cyril, Müller Peter, Weder Nicola, Spingler Bernhard, Joliat-Wick Evelyne, Mosberger Mathias, Windisch Johannes, Alberto Roger, Probst Benjamin (2017), Structure-Activity and Stability Relationships for Cobalt Polypyridyl-Based Hydrogen-Evolving Catalysts in Water, in ChemSusChem
, 10(22), 4570-4580.
Il'in Mikhail V., Bolotin Dmitrii S., Novikov Alexander S., Suslonov Vitalii V., Chezhina Natalia V., Bubnov Michael P., Cherkasov Vladimir K., Venter Gertruida J.S., Roodt Andreas (2017), Square-planar aminonitronate transition metal complexes (M = Cu II , Ni II , Pd II , and Pt II ), in Inorganica Chimica Acta
, 467, 372-378.
Conradie Marrigje Marianne, van Rooyen Petrus H., Pretorius Carla, Roodt Andreas, Conradie Jeanet (2017), Rhodium-rhodium interactions in [Rh(β-diketonato)(CO)2] complexes, in Journal of Molecular Structure
, 1144, 280-289.
Raleaooa Pule V., Roodt Andreas, Mhlongo Gugu G., Motaung David E., Kroon Robin E., Ntwaeaborwa Odireleng M. (2017), Luminescent, magnetic and optical properties of ZnO-ZnS nanocomposites, in Physica B: Condensed Matter
, 507, 13-20.
Manicum Amanda-Lee, Alexander Orbett, Schutte-Smith Marietjie, Visser Hendrik G., Roodt Andreas (2017), Crystal structure of fac-(acetylacetonato-κ2O,O′)tricarbonyl(benzyldiphenylphosphine-κP)rhenium(I), C27H24O5PRe, in Zeitschrift für Kristallographie - New Crystal Structures
, 232(6), 957-959.
Hill Tania N., Koen Renier, Roodt Andreas (2017), Crystal structure of trans-bis((E)-7-oxo-4-(phenyldiazenyl)cyclohepta-1,3,5-trien-1-olato)-κ2O,O′)-bis(pyridine-κN)cobalt(II), C36H28CoN6O4, in Zeitschrift für Kristallographie - New Crystal Structures
, 232(3), 447-449.
Bolotin Dmitrii S., Il’in Mikhail V., Kolesnikov Ilya E., Suslonov Vitaliy V., Novozhilov Yuri, Ronzhina Oksana, Krasavin Mikhail, Boyarskiy Vadim P., Koen Renier, Roodt Andreas (2017), Fluorescent (pyrazolyl acetoxime)Zn II complexes: Synthetic, structural, and photophysical studies, in Inorganica Chimica Acta
, 455, 9-14.
Belay Alebel N., Venter Johan A., Roodt Andreas (2017), The crystal structure of triphenylphosphineoxide – 2,5-dichloro-3,6-dihydroxycyclohexa-2,5-diene-1,4-dione (2/1), C42H32Cl2O6P2, in Zeitschrift für Kristallographie - New Crystal Structures
, 232(2), 163-164.
In this project, we propose to investigate two uphill reactions, which are of great relevance for sustainable production, ultimately of industrial compounds; the reduction of protons from water to H2 and the activation/reduction of atmospheric CO2 to CO. Both reactions are uphill and shall be driven by solar light, either in an electrocatalytic way with energy harvested in solar cells or directly in a photocatalytic assembly. Whereas both reactions are researched worldwide with great effort, we propose inhere a different approach by combining the different modalities via the rather uncommon scaffold, [Re(arene)2]+. Reports on intramolecular, di-functional assemblies exist, but are rare. The conjugation into an intramolecular assembly should help to overcome rate - and performance limiting reaction steps. The [Re(arene)2]+ is proposed for two reasons. First, it is of utmost (photo)chemical stability in water up to high temperatures and not sensitive at all towards air. Second, our concept of preparing catalyst-catalyst, catalyst-proton donor or catalyst-electron donor combinations leaves the two subunits different degrees of structural freedom, rotation and tilting, which allows their structurally unrestricted, functional interaction. The catalysts for CO2 activation/conversion are selected from groups of known activity but altered according to our specific needs, the proton reduction catalysts from basic architectures with Co, Ni and Fe in newly developed ligands. The procedure follows a stepwise approach; mechanistic and kinetic investigations in homogeneous solution of the isolated catalysts - bound to the scaffold and then combined with the second functionality. Key numbers to be elucidated are turn over numbers, turn over frequencies and long-term stability. The performance of the conjugates must be superior as compared to isolated, intermolecular mixtures. Our two groups are synergistically experienced in the fields; the SA group has extended background in the catalytic preparation of industrially relevant compounds including hydrocarbons and CO whereas the CH group is involved via a “university research priority project” on artificial photosynthesis in proton reduction. Syntheses of respective catalysts will be done at the two involved universities whereas the electro- and photocatalytic studies will be performed jointly at the appropriate institutions. The proposed studies are fundamental and do not aim at a device. Basic insights from these studies will however enable transfer of knowledge to a later and practical application.