Liu Xunshan, Matej Adam, Kratky Tim, Mendieta‐Moreno Jesús I., Günther Sebastian, Mutombo Pingo, Decurtins Silvio, Aschauer Ulrich, Repp Jascha, Jelinek Pavel, Liu Shi‐Xia, Patera Laerte L. (2022), Exploiting Cooperative Catalysis for the On‐Surface Synthesis of Linear Heteroaromatic Polymers via Selective C–H Activation, in Angewandte Chemie International Edition
, 61(5), e202112798.
Vonrüti Nathalie, Rao Reshma, Giordano Livia, Shao-Horn Yang, Aschauer Ulrich (2022), Implications of Nonelectrochemical Reaction Steps on the Oxygen Evolution Reaction: Oxygen Dimer Formation on Perovskite Oxide and Oxynitride Surfaces, in ACS Catalysis
, 12(2), 1433-1442.
Ricca Chiara, Grad Lisa, Hengsberger Matthias, Osterwalder Jürg, Aschauer Ulrich (2021), Importance of surface oxygen vacancies for ultrafast hot carrier relaxation and transport in Cu2O, in Physical Review Research
, 3(4), 043219-043219.
Zhou Ping, Aschauer Ulrich, Decurtins Silvio, Feurer Thomas, Häner Robert, Liu Shi-Xia (2021), Effect of tert-butyl groups on electronic communication between redox units in tetrathiafulvalene-tetraazapyrene triads, in Chemical communications
, 57(96), 12972-12975.
Liu Yongpeng, Bouri Maria, Yao Liang, Xia Meng, Mensi Mounir, Grätzel Michael, Sivula Kevin, Aschauer Ulrich, Guijarro Néstor (2021), Identifying Reactive Sites and Surface Traps in Chalcopyrite Photocathodes, in Angewandte Chemie (International ed. in English)
, 60(44), 23651-23655.
Lan Zhenyun, Småbråten Didrik René, Xiao Chengcheng, Vegge Tejs, Aschauer Ulrich, Castelli Ivano E. (2021), Enhancing Oxygen Evolution Reaction Activity by Using Switchable Polarization in Ferroelectric InSnO 2 N, in ACS Catalysis
, 11(20), 12692-12700.
Franklin J., Xu B., Davino D., Mahabir A., Balatsky A. V., Aschauer U., Sochnikov I. (2021), Giant Grüneisen parameter in a superconducting quantum paraelectric, in Physical Review B
, 103(21), 214511-214511.
Flores Eibar, Mozhzhukhina Nataliia, Aschauer Ulrich, Berg Erik J. (2021), Operando Monitoring the Insulator–Metal Transition of LiCoO2, in ACS Applied Materials & Interfaces
, 13(19), 22540-22548.
Burns Eric, Aschauer Ulrich, Döbeli Max, Schneider Christof W., Pergolesi Daniele, Lippert Thomas (2020), LaTiO2N crystallographic orientation control significantly increases visible-light induced charge extraction, in Journal of Materials Chemistry A
, 8(43), 22867-22873.
Zhou Ping, Aschauer Ulrich, Decurtins Silvio, Feurer Thomas, Häner Robert, Liu Shi-Xia (2020), Chemical control of photoinduced charge-transfer direction in a tetrathiafulvalene-fused dipyrrolylquinoxaline difluoroborate dyad, in Chemical Communications
, 56(87), 13421-13424.
The development of alternative renewable energy sources is a highly relevant goal in view of our ever-increasing energy needs and the negative environmental and climate effects of current fossil or nuclear energy sources. Photocatalysis using semiconducting light absorbers is a promising route to convert solar energy into chemical energy stored in the bonds of the formed molecular products. A good photocatalyst has to efficiently absorb solar light, promote separation of the resulting electron and hole charge carriers and provide high catalytic efficiency for the targeted chemical reaction at its surfaces. While many reactions can be photocatalyzed, photocatalytic water splitting and in particular the oxygen evolution (OER) half-reaction is considered to be a good test case to characterize the activity of different semiconductors. Among earth-abundant semiconductor materials that have suitable band gaps, perovskite oxynitrides have emerged as a highly promising class of visible-light absorbers.The preceding project has, for the first time, established the atomic-scale surface structure of these oxynitride materials using density functional theory calculations and highlighted that they have promising catalytic properties. Moreover, we have shown that they can be rendered ferroelectric under compressive epitaxial strain, which will dramatically improve electron-hole separation and, with the switching of the ferroelectric polarization, may enable unprecedented control of reaction pathways. While these results highlight the potential of oxynitrides for photocatalytic applications, they also lead to additional open questions. As such, we have found that the effect of the ferroelectric polarization on the reactivity may be affected by oxidizing adsorbates under photocatalytic application conditions but the relation between polarization, adsorbate coverage and fundamental material parameters is not yet clear. Also, in our calculations, we observed a photo-corrosion instability resulting in N2 or NO evolution under photocatalytic application conditions, which indicates that oxynitrides need to be protected, for example by cocatalysts or protective catalytic coatings. To address these open questions, the goals of this extension project are to: 1) more deeply investigate the effect of ferroelectricity on the catalytic activity of the surface, focusing on application conditions with oxidizing adsorbates; 2) study which materials are suitable as protective and catalytic coatings for oxynitrides and how their thickness affects the stability of the oxynitride and the catalytic activity of the coating.