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Solar Light-driven Homogeneous Catalysis for Greener Industrial Processes with H2 as Energy Source and CO2 as C1 Building Block

English title Solar Light-driven Homogeneous Catalysis for Greener Industrial Processes with H2 as Energy Source and CO2 as C1 Building Block
Applicant Alberto Roger
Number 170856
Funding scheme Bilateral programmes
Research institution Institut für Chemie Universität Zürich
Institution of higher education University of Zurich - ZH
Main discipline Inorganic Chemistry
Start/End 01.02.2017 - 31.01.2021
Approved amount 346'189.00
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Keywords (6)

Green Chemistry; Solar Light; Hydrogen; Sustainability; CO2 conversion; Photocatalysis

Lay Summary (German)

Lead
Photokatalytische homogene Katalyse für umweltverträgliche industrielle Prozesse mit H2 als Energieträger und CO2 als C1 QuelleDas Treibhausgas CO2 ist in grosser Menge in der Atmosphäre enthalten oder wird konzentriert aus Kohlekraftwerken emittiert. Die Konversion von CO2 in C1 Bausteine oder Treibstoffe ist heute zwar möglich, hat aber eine negative CO2 Bilanz, da H2 aus Kohle oder Erdgas hergestellt wird. Dies zu ändern ist eine grosse Herausforderung der Wissenschaft und Inhalt dieses Forschungsprojektes.
Lay summary

Inhalt und Ziel   

Um CO2 in Bausteinen zu „fixieren“ muss es aktiviert und reduziert oder direkt mit H2 (2 H+ und 2 e-) umgesetzt werden. Um diese mechanistisch schwierigen Reaktionen zu ermöglichen, entwickeln wir Katalysatoren mit Kobalt, Niob, Rhodium oder Rhenium. Ihr Design ist so, dass sie CO2 binden können. Parallel dazu synthetisieren wir Katalysatoren, welche H2O mit Elektronen zu H2 reduzieren. Die Energie für beide thermodynamisch schwierigen Prozesse „ernten“ wir aus Sonnenlicht über geeignete Photosensibilisatoren. Die Partner in SA werden in diesem stark interdisziplinären Projekt kinetische und mechanistische Untersuchungen beitragen und Katalysatoren mit Rh und Nb optimieren. Die Gruppe in ZH wird die Re und Co Katalysatoren nach einem grundsätzlich neuen Funktionalitätsansatz herstellen und mit dem Netzwerk LightChEC (www.lightcheck.uzh.ch) untersuchen.

Wissenschaftlicher und gesellschaftlicher Kontext

Photokatalyse mit Substraten wie CO2 oder H2O ist die Grundlage für eine nachhaltige und CO2 neutrale Energieversorgung. Weltweit wird sehr viel in dieses Gebiet gesteckt, das nicht nur wissenschaftlich sondern auch gesellschaftlich von grösster Bedeutung ist.

Direct link to Lay Summary Last update: 18.01.2017

Responsible applicant and co-applicants

Employees

Project partner

Natural persons


Name Institute

Publications

Publication
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
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.
Nuclearity manipulation in Schiff-base fac -tricarbonyl complexes of Mn(I) and Re(I)
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.
Analysis of the structure, particle morphology and photoluminescent properties of ZnS:Mn 2+ nanoparticulate phosphors
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.
Four Thermochromic o-Hydroxy Schiff Bases of α-Aminodiphenylmethane: Solution and Solid State Study
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.
Structure-Activity and Stability Relationships for Cobalt Polypyridyl-Based Hydrogen-Evolving Catalysts in Water
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.
Square-planar aminonitronate transition metal complexes (M = Cu II , Ni II , Pd II , and Pt II )
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.
Rhodium-rhodium interactions in [Rh(β-diketonato)(CO)2] complexes
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.
Luminescent, magnetic and optical properties of ZnO-ZnS nanocomposites
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.
Crystal structure of fac-(acetylacetonato-κ2O,O′)tricarbonyl(benzyldiphenylphosphine-κP)rhenium(I), C27H24O5PRe
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.
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
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.
Fluorescent (pyrazolyl acetoxime)Zn II complexes: Synthetic, structural, and photophysical studies
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.
The crystal structure of triphenylphosphineoxide – 2,5-dichloro-3,6-dihydroxycyclohexa-2,5-diene-1,4-dione (2/1), C42H32Cl2O6P2
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.

Collaboration

Group / person Country
Types of collaboration
Prof. Peter Hamm, University of Zürich Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Research Infrastructure
Dr. Gerdus Kemp, PET Labs Pretoria South Africa (Africa)
- Research Infrastructure
- Industry/business/other use-inspired collaboration
Prof. André Roodt, University of the Free State South Africa South Africa (Africa)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
- Exchange of personnel

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
GDCh Lecture Individual talk Homo- and heterogeneous light-induced proton reduction with cyclic and acyclic poly-pyridyl complexes 22.05.2019 Berlin, Germany Alberto Roger;
GdCh talk Individual talk Light-induced Proton Reduction with Cyclic and Acyclic Polypyridyl-based Cobalt Complexes 18.12.2018 Free University of Berlin, Germany Alberto Roger;
ReMec1: 1st Symposium on Reaction Mechanisms Talk given at a conference Carbon dioxide fixation in succulent plants, synthesis and characterization of metal carboxylates, Plastic recycling, water purification and heavy metal recovery. 13.11.2018 Bloemfontein, South Africa Hernández Valdés Daniel; Alberto Roger; Roodt Andreas;
Lecture Series Individual talk Artificial Water Splitting with Cobalt 07.08.2018 Montevideo, Uruguay Alberto Roger;
43rd International Conference on Coordination Chemistry Sendai, Japan, 30.7.-4.8.2017. Talk given at a conference Re(I) bis-arenes complexes as scaffold for photocatalytic water splitting 30.07.2018 Sendai, Japan Alberto Roger; Hernández Valdés Daniel;
Fall Meeting 2017 of the Swiss Chemical Society Poster Towards the direct synthesis of nitrogen functionalized bis arene complexes of Re and 99(m)Tc 21.08.2017 Bern, Switzerland Hernández Valdés Daniel;
25th Solvenian-Croatian Crystallographic Meeting Talk given at a conference Metals ‘communicating’ in ‘dinuclear’ Rh(I) complexes? Understanding(?) metallophilic interactions… 14.06.2017 Ljubljana, Slovenia Roodt Andreas;
Seminar, University of Paris Saclay and CEA Individual talk Acyclic and Cyclic Polypyridyl-based Cobald Complexes in Photocatalysis 09.05.2017 Paris, France Alberto Roger;
Anorganisches-Chemisches Kolloquium, Universität Basel Individual talk Acyclic and Cyclic Polypyridyl-based Cobald Complexes in Photocatalysis 31.03.2017 Basel, Switzerland Alberto Roger;


Knowledge transfer events



Self-organised

Title Date Place
Energie der Zukunft 25.01.2018 University of Zurich, Switzerland

Awards

Title Year
Alexander von Humboldt Research Award 2017

Associated projects

Number Title Start Funding scheme
160801 Photocatalytic Processes at Solvated Interfaces 01.02.2016 Sinergia

Abstract

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.
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