Fundamentals of photocatalytic water splitting at spinel oxide interfaces

Subproject P11

Obtaining mechanistic insights into photocatalytic processes in their natural aqueous environment is challenging since it is difficult to probe just the interfacial molecules in the presence of the bulk. Moreover, typical reaction timescales are very short, making high time resolution necessary.

The long-term objective of P11 is to unravel the reaction mechanism of photocatalytic processes in real-time directly at the water-catalyst interface, where the reaction is taking place. In the first project period, we focus on photocatalytic water splitting at iron spinel oxide interfaces. The project will benefit from high-quality and well-characterized spinel samples prepared by P04 Parkinson. We will use vibrational spectroscopy to probe only the interfacial molecules. In this way, we study the strength of hydrogen bonds and the orientation of the water molecules, i.e., how water binds to various spinel oxides. Subsequently, photodissociation will be initiated by a laser pulse mimicking sunlight. We will follow the reaction on sub-picosecond timescales by probing the water molecules and potential reaction intermediates and products. The collaboration with theoretical projects helps with data interpretation and fundamental insights into the reaction (P12 Dellago). The water structure and reaction dynamics will be linked to reported efficiencies of the photocatalysts to connect molecular-level details to high catalytic efficiency (P10 Föttinger).

Ellen Backus
PI

Expertise

Our expertise is ultrafast and nonlinear optical spectroscopy, predominantly in the infrared spectral region. We have two femtosecond amplifiers and several optical parametric amplifiers to convert the amplifier’s 800 nm output into other frequencies.

To study the solid-liquid interface, our focus in the TACO project, we will have two time-resolved sum-frequency generation setups, of which one is phase-resolved as well.

Team

Ellen Backus
PI

Moritz Zelenka
PhD Student

Publications

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43 entries « 1 of 5 »

2021

Ni-modified Fe3O4(001) surface as a simple model system for understanding the oxygen evolution reaction

Mirabella, Francesca; Müllner, Matthias; Touzalin, Thomas; Riva, Michele; Jakub, Zdenek; Kraushofer, Florian; Schmid, Michael; Koper, Marc T M; Parkinson, Gareth S; Diebold, Ulrike

Ni-modified Fe3O4(001) surface as a simple model system for understanding the oxygen evolution reaction Journal Article

In: Electrochimica Acta, 389 , pp. 138638, 2021.

Abstract | Links | BibTeX | Tags: P02, P04, pre-TACO

Emerging applications of MXene materials in CO2 photocatalysis

Shen, Jiahui; Wu, Zhiyi; Li, Chaoran; Zhang, Chengcheng; Genest, Alexander; Rupprechter, Günther; He, Le

Emerging applications of MXene materials in CO2 photocatalysis Journal Article

In: FlatChem, 28 , pp. 100252, 2021.

Abstract | Links | BibTeX | Tags: P08, pre-TACO

Resolving multifrequential oscillations and nanoscale interfacet communication in single-particle catalysis

Suchorski, Yuri; Zeininger, Johannes; Buhr, Sebastian; Raab, Maximilian; Stöger-Pollach, Michael; Bernardi, Johannes; Grönbeck, Henrik; Rupprechter, Günther

Resolving multifrequential oscillations and nanoscale interfacet communication in single-particle catalysis Journal Article

In: Science, 372 (6548), pp. 1314–1318, 2021.

Links | BibTeX | Tags: P08, pre-TACO

Improved description of atomic environments using low-cost polynomial functions with compact support

Bircher, Martin P; Singraber, Andreas; Dellago, Christoph

Improved description of atomic environments using low-cost polynomial functions with compact support Journal Article

In: Machine Learning: Science and Technology, 2 (3), pp. 035026, 2021.

Abstract | Links | BibTeX | Tags: P12, pre-TACO

α-β phase transition of zirconium predicted by on-the-fly machine-learned force field

Liu, Peitao; Verdi, Carla; Karsai, Ferenc; Kresse, Georg

α-β phase transition of zirconium predicted by on-the-fly machine-learned force field Journal Article

In: Physical Review Materials, 5 (5), pp. 053804, 2021.

Abstract | Links | BibTeX | Tags: P03, pre-TACO

Evolutionary computing and machine learning for discovering of low-energy defect configurations

Arrigoni, Marco; Madsen, Georg K H

Evolutionary computing and machine learning for discovering of low-energy defect configurations Journal Article

In: npj Computational Materials, 7 (1), 2021.

Abstract | Links | BibTeX | Tags: P09, pre-TACO

Co3O4-CeO2 Nanocomposites for Low-Temperature CO Oxidation

Yang, Jingxia; Yigit, Nevzat; Möller, Jury; Rupprechter, Günther

Co3O4-CeO2 Nanocomposites for Low-Temperature CO Oxidation Journal Article

In: Chemistry A European Journal, 2021.

Abstract | Links | BibTeX | Tags: P08, pre-TACO

Direct CO2 capture and conversion to fuels on magnesium nanoparticles under ambient conditions simply using water

Rawool, Sushma A; Belgamwar, Rajesh; Jana, Rajkumar; Maity, Ayan; Bhumla, Ankit; Yigit, Nevzat; Datta, Ayan; Rupprechter, Günther; Polshettiwar, Vivek

Direct CO2 capture and conversion to fuels on magnesium nanoparticles under ambient conditions simply using water Journal Article

In: Chemical Science, 12 (16), pp. 5774–5786, 2021.

Abstract | Links | BibTeX | Tags: P08, pre-TACO

Polarons in materials

Franchini, Cesare; Reticcioli, Michele; Setvin, Martin; Diebold, Ulrike

Polarons in materials Journal Article

In: Nature Reviews Materials, 2021.

Abstract | Links | BibTeX | Tags: P02, P07, pre-TACO

Operando Surface Spectroscopy and Microscopy during Catalytic Reactions: From Clusters via Nanoparticles to Meso-Scale Aggregates

Rupprechter, Günther

Operando Surface Spectroscopy and Microscopy during Catalytic Reactions: From Clusters via Nanoparticles to Meso-Scale Aggregates Journal Article

In: Small, 2021.

Abstract | Links | BibTeX | Tags: P08, pre-TACO

43 entries « 1 of 5 »