Article
Chemistry, Physical
Florian Kraushofer, Lena Haager, Moritz Eder, Ali Rafsanjani-Abbasi, Zdenek Jakub, Giada Franceschi, Michele Riva, Matthias Meier, Michael Schmid, Ulrike Diebold, Gareth S. Parkinson
Summary: This study investigates the stability of single Rh atoms on alpha-Fe2O3 in the presence of water using STM, ncAFM, and XPS, revealing the crucial role of OH ligands in stabilizing single atoms, which should be taken into consideration when modeling single-atom catalysis systems.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Physical
Florian Kraushofer, Lena Haager, Moritz Eder, Ali Rafsanjani-Abbasi, Zdenek Jakub, Giada Franceschi, Michele Riva, Matthias Meier, Michael Schmid, Ulrike Diebold, Gareth S. Parkinson
Summary: The study demonstrates that high densities of single Rh adatoms can be stabilized on the alpha-Fe2O3 surface in the presence of water, in contrast to rapid sintering observed under UHV conditions. The importance of OH ligands in the stability of single atoms is highlighted, suggesting that their presence should be considered when modeling single-atom catalysis systems.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Quan Li, Hong Wang, Guan Wang, Fanjie Xia, Weihao Zeng, Haoyang Peng, Ganggang Ma, Anan Guo, Ruifeng Dong, Jinsong Wu
Summary: It is found that trace amount lanthanide element Yb doping can mitigate the structural degradation during cycling of Li-rich layered oxides (LLOs) by forming a surficial Yb-rich layer with high density of oxygen vacancy on the cathodes, and doping into the lattice of LLO to enhance the binding energy with oxygen and stabilize the lattice in grain interior, resulting in significantly improved cycling stability.
Article
Engineering, Chemical
Linn Katinka Emhjellen, Wen Xing, Zuoan Li, Reidar Haugsrud
Summary: Composite ceramic membranes based on BTM and LSM exhibit high oxygen flux values, with the oxygen permeability becoming more bulk-limited as the temperature increases. The oxygen exchange coefficients of BTM-LSM are significantly higher than its constituent phases, and introducing electronic conductivity into BTM increases the surface exchange coefficients. However, the oxygen flux of BTP remains lower compared to percolating BTM-LSM composites.
JOURNAL OF MEMBRANE SCIENCE
(2022)
Article
Chemistry, Physical
Zdenek Rafaj, Jozef Krutel, Vaclav Nehasil
Summary: Rhodium (Rh) is predominantly used in the automotive industry for three-way catalysis (TWC), with improved efficiency achieved by adding CeO2-active support for oxygen storage capacity. In this study, the CO oxidation mechanism of Rh nanoparticles on CeO2(111) and CeO2(110) was investigated, revealing higher performance on Rh/CeO2(110) due to weaker CO-Rh bond and increased oxygen exchange activity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Lifan Wang, Guicheng Liu, Rui Wang, Xindong Wang, Liguang Wang, Zhenpeng Yao, Chun Zhan, Jun Lu
Summary: By introducing dual-ion conductors, the reactivity of surface lattice oxygen ions in high-active anionic oxides can be effectively controlled, suppressing oxygen release, irreversible phase transition, and intergranular mechanical cracking. The dual-ion conductor also facilitates lithium-ion diffusion kinetics and electronic conductivity, achieving a balance between capacity and stability for high-energy cathodes.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Hiroki Nakayama, Makoto Nagata, Toshihisa Tomie, Tomoaki Ishitsuka, Nobuyuki Matsubayashi, Yukihiro Shimizu
Summary: In this study, the valence band spectra of Rh catalysts on various supports were measured and correlated with the catalytic activities in the CO-NO reaction. The effects of SMSI on the activities of Rh catalysts were analyzed using density functional theory calculations. The study reveals the critical mechanisms whereby SMSIs contribute to oxygen-mediated reactions on catalyst surfaces.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Bernhard von Boehn, Jon-Olaf Krisponeit, Jens Falta, Ronald Imbihl
Summary: Using low-energy electron microscopy (LEEM) and micro-LEED as in situ techniques, the structural transitions in traveling interface pulses (TIPs) in bistable methanol oxidation on a bare Rh(110) and on a Rh(110) surface covered with a 0.1 monolayer of V oxide were studied. The addition of 0.1 monolayer of V oxide increased structural disorder but did not cause qualitative changes in the structural transitions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Wenjie Dai, Yang Chen, Xu Liu, Henggao Xiang, Chi Xu, Gong Zheng, Guang Chen
Summary: Through theoretical calculations, this study found that surface doping with titanium and silicon can effectively inhibit the surface diffusion of Cu and Sn atoms in three-dimensional integrated circuits (3D-ICs), reducing the growth of lateral Cu3Sn.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Inorganic & Nuclear
Yue Song, Tianjun Zhang, Risheng Bai, Yida Zhou, Lin Li, Yongcun Zou, Jihong Yu
Summary: This study reports a method to stabilize Rh metal species supported on zeolites at high temperatures by forming Rh-[O]x-Hf species, which improves the stability and activity of the catalyst and is significant for various catalytic processes.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Materials Science, Multidisciplinary
S. Sarkar, F. Cossu, P. Kumari, A. G. Moghaddam, A. Akbari, Y. O. Kvashnin, I Di Marco
Summary: This work presents an ab-initio computational study on the electronic and magnetic properties of transition metal adatoms on a monolayer of NbSe2. It is found that Cr, Mn, Fe, and Co preferentially sit above the Nb atom, leading to strong hybridization with the d states. The inter-atomic exchange coupling exhibits oscillatory behavior accompanied by exponential decay, consistent with the theory for a damped Ruderman-Kittel-Kasuya-Yosida interaction. The results suggest that the magnetic coupling of the investigated adatoms is connected to the fine details of their Fermi surface.
Article
Chemistry, Multidisciplinary
Jonas Bjork, Carlos Sanchez-Sanchez, Qiang Chen, Carlo A. Pignedoli, Johanna Rosen, Pascal Ruffieux, Xinliang Feng, Akimitsu Narita, Klaus Mullen, Roman Fasel
Summary: This study reveals the importance of metal adatoms and their effect on regioselectivity in surface-assisted cyclodehydrogenation on Au(111).
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Marcus A. Sharp, Christopher J. Lee, Mausumi Mahapatra, R. Scott Smith, Bruce D. Kay, Zdenek Dohnalek
Summary: In this study, the morphological changes of a model Rh catalyst supported on Fe3O4(001) were investigated using scanning tunneling microscopy and X-ray photoelectron spectroscopy. Various Rh sites were identified, and the properties of these sites were characterized using adsorbates such as CO and CO2. The high-temperature CO desorption and CO oxidation mechanisms were demonstrated for adatoms and nanoparticles.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Materials Science, Multidisciplinary
Alma L. Marcos-Viquez, Alvaro Miranda, Miguel Cruz-Irisson, Luis A. Perez
Summary: In this study, the interactions between oxygen molecule O-2 and pristine or gold-decorated SnC monolayers were investigated using density functional calculations. Results showed that O-2 is adsorbed in a bond-like configuration on the pristine SnC monolayer, and when a gold adatom is present, O-2 dissociates and adsorbs on different tin atoms.
Article
Chemistry, Physical
Bernhard von Boehn, Anton Weissbach, Jon-Olaf Krisponeit, Jan Ingo Flege, Jens Falta, Luca Gregoratti, Matteo Amati, Patrick Zeller, Ronald Imbihl
Summary: This study investigates the condensation of submonolayer coverages of V-oxide on Rh(111) into macroscopic stripes or islands during catalytic methanol oxidation. The phase separation within the VOx islands under reaction conditions is studied using various techniques, including PEEM, LEEM, mu LEED, and mu XPS. The dependence of the substructure on reaction conditions, V coverage, and island size is explored and the V coverages of different phases in the VOx islands are determined using mu XPS.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Chu Zhang, Baochang Wang, Anders Hellman, Mikhail Shipilin, Andreas Schaefer, Lindsay R. Merte, Sara Blomberg, Xueting Wang, Per-Anders Carlsson, Edvin Lundgren, Jonas Weissenrieder, Andrea Resta, Anders Mikkelsen, Jesper N. Andersen, Johan Gustafson
Summary: The study found that the oxidation of CO on a stepped Rh(553) surface occurs faster than on a flat Rh(111) surface at the same temperature, however, it is not due to reactions at the step sites but rather at the terrace sites close to the steps. This insight can provide ways to optimize the shape of nanoparticles to further improve the activity of certain reactions.
Article
Chemistry, Physical
Alfred Larsson, Giulio D'Acunto, Mariya Vorobyova, Giuseppe Abbondanza, Ulrich Lienert, Zoltan Hegedus, Alexei Preobrajenski, Lindsay R. Merte, Josefin Eidhagen, Anna Delblanc, Jinshan Pan, Edvin Lundgren
Summary: The surface chemistry and thickness distribution of three Ni superalloys were investigated using synchrotron X-ray Photoelectron Spectroscopy and X-ray Reflectivity. The results showed variations in the composition and thickness of the oxide, hydroxide, and sub-surface layer, which were correlated with the thermodynamic properties of the metal elements in the alloys.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Chemistry, Physical
Stefano Albertin, Lindsay R. Merte, Edvin Lundgren, Rachel Martin, Jason F. Weaver, Ann-Christin Dippel, Olof Gutowski, Uta Hejral
Summary: The oxidation and reduction reactions on the Ir(100) surface were studied using high-energy surface X-ray diffraction. Different oxide structures were observed under varied O-2 partial pressure, and the reduction process led to the formation of metallic Ir islands.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Dorotea Gajdek, Par A. T. Olsson, Sara Blomberg, Johan Gustafson, Per-Anders Carlsson, Dorthe Haase, Edvin Lundgren, Lindsay R. Merte
Summary: Grazing incidence X-ray absorption fine structure spectroscopy was used to study the CoO films on Pt(111). The results showed that the chemical state of Co changed under different oxidizing and reducing conditions, indicating the formation of cobalt hydroxide, oxyhydroxide, and bulklike Co3O4.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Harald J. Wallander, Freddy E. Oropeza, Benjamin Hagman, Jan Knudsen, Edvin Lundgren, Lindsay R. Merte
Summary: The surface composition of a Pt3Sn(111) surface during CO oxidation has been investigated using ambient pressure X-ray photoemission spectroscopy. Oxidation of tin coincides with catalytic conversion, and the morphology and oxidation state of the formed oxide depend on the gas composition. An oxygen-rich mixture leads to the formation of 2D wetting layers, while a CO-rich mixture leads to the formation of 3D oxide islands. Spontaneous oscillations in conversion are observed in the oxygen-rich gas mixture, attributed to the combined effects of tin oxides and CO blocking.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Multidisciplinary Sciences
Michele Reticcioli, Zhichang Wang, Michael Schmid, Dominik Wrana, Lynn A. Boatner, Ulrike Diebold, Martin Setvin, Cesare Franchini
Summary: By combining scanning probe microscopy with density functional theory calculations, this study reveals that excess charge on the polar TaO2 termination of KTaO3(001) forms complex electronic states, including charge density waves, electron polarons, and bipolarons. These surface electronic reconstructions impact surface properties.
NATURE COMMUNICATIONS
(2022)
Article
Multidisciplinary Sciences
Zhichang Wang, Michele Reticcioli, Zdenek Jakub, Igor Sokolovic, Matthias Meier, Lynn A. Boatner, Michael Schmid, Gareth S. Parkinson, Ulrike Diebold, Cesare Franchini, Martin Setvin
Summary: Polarizable materials, such as the incipient ferroelectric perovskite KTaO3, exhibit the ability to tune chemical reactivity. The adsorption states of molecules are influenced by the coupling between surface polarity and ferroelectric polarization.
Article
Chemistry, Multidisciplinary
Hao Chen, Matthias A. . Blatnik, Christian L. Ritterhoff, Igor Sokolovic, Francesca Mirabella, Giada Franceschi, Michele Riva, Michael Schmid, Jan Cechal, Bernd Meyer, Ulrike Diebold, Margareta Wagner
Summary: Clean oxide surfaces are usually hydrophilic, but the In2O3(111) surface shows chemical heterogeneity with different adsorption behaviors and structural arrangements of water molecules in different regions.
Article
Materials Science, Multidisciplinary
Claudiu Bulbucan, Pau Ternero, Calle Preger, Aram Kostanyan, Maria E. Messing, Rasmus Westerstrom
Summary: We investigated the influence of particle size on the formation of antiferromagnetic FexO subdomains and the occurrence of exchange bias in novel ferrimagnetic Cr-substituted Fe3O4 nanoparticles generated using an aerosol technique. Cooling the samples in a magnetizing field at the Néel temperature of the FexO subdomains caused significant shifts in the hysteresis loops. The shift magnitude decreased with decreasing particle diameter for the larger systems, while only minor exchange fields were observed for the smallest system. This reduction in exchange bias was attributed to the lower volume fraction and size of the metastable FexO phase, which readily transformed into the thermodynamically stable (Fe,Cr)3O4 phase with decreasing particle diameter.
JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS
(2023)
Article
Multidisciplinary Sciences
Giada Franceschi, Pavel Kocan, Andrea Conti, Sebastian Brandstetter, Jan Balajka, Igor Sokolovic, Markus Valtiner, Florian Mittendorfer, Michael Schmid, Martin Setvin, Ulrike Diebold
Summary: This study presents atomic force microscopy images to investigate the distribution of K+ ions on the cleaved mica surface under ultra-high vacuum conditions. The data reveal the presence of short-range ordering and provide insights into the distribution of subsurface Al3+ ions.
NATURE COMMUNICATIONS
(2023)
Article
Electrochemistry
Lena Puntscher, Kevin Daninger, Michael Schmid, Ulrike Diebold, Gareth S. Parkinson
Summary: Understanding the stability of metal atoms on metal oxide supports is crucial for predicting the stability of single-atom catalysts. In this study, scanning tunnelling microscopy (STM) and x-ray photoelectron spectroscopy (XPS) were used to investigate the stability of platinum, rhodium, nickel, and iridium on the anatase TiO2(101) surface. The study found that introducing defect sites into metal oxide supports can aid the dispersion of single atoms on metal-oxide surfaces, and the presence of water should be taken into account in the modelling of single-atom catalysts.
ELECTROCHIMICA ACTA
(2023)
Article
Chemistry, Physical
Florian Kraushofer, Matthias Meier, Zdenek Jakub, Johanna Huetner, Jan Balajka, Jan Hulva, Michael Schmid, Cesare Franchini, Ulrike Diebold, Gareth S. Parkinson
Summary: This study investigates the (111) facet of magnetite (Fe3O4) and reveals three new surface structures that are more favorable under reducing conditions. The new structures change the coordination of iron atoms to a tetrahedral configuration. Atomically-resolved microscopy confirms the presence of tetrahedral iron atoms capped by 3-fold coordinated oxygen atoms. This discovery explains the inert nature of the reduced patches.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Computer Science, Artificial Intelligence
Marco Corrias, Lorenzo Papa, Igor Sokolovic, Viktor Birschitzky, Alexander Gorfer, Martin Setvin, Michael Schmid, Ulrike Diebold, Michele Reticcioli, Cesare Franchini
Summary: Analyzing atomically resolved images is a time-consuming process that requires expertise and manual intervention. To automate and improve the efficiency of image analysis, machine learning techniques have been applied in scanning probe and electron microscopies. This work introduces a free and open source tool called AiSurf that uses scale-invariant feature transform and clustering algorithms to inspect atomically resolved images. The tool extracts crucial information from the images without pre-assumptions or extensive user intervention, making it a valuable asset for interpreting scanning probe microscopy images.
MACHINE LEARNING-SCIENCE AND TECHNOLOGY
(2023)
Correction
Chemistry, Analytical
Michael Schmid, David Rath, Ulrike Diebold
ACS MEASUREMENT SCIENCE AU
(2023)
