Article
Chemistry, Physical
E. Silberstein, G. Makov
Summary: The structure of liquid methanol has been investigated using experimental and computational methods. The quasi-crystalline model is applied to analyze the short-range order of methanol, and molecular dynamics simulations are used to obtain the radial distribution functions. The results suggest that methanol at different temperatures and pressures can have different structures, with open chains and cyclic tetramers being the dominant structures at certain conditions.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Materials Science, Multidisciplinary
Lingling Zhou, Qi Wang, Jing Wang, Xuefei Chen, Ping Jiang, Hao Zhou, Fuping Yuan, Xiaolei Wu, Zhiying Cheng, En Ma
Summary: This study provides experimental evidence for the existence of chemical short-range order (CSRO) in CrCoNi alloy through electron diffraction and atomic-resolution chemical mapping. The spatial correlations between different atomic pairs are revealed through quantitative covariance analysis. The findings are significant for understanding CSRO in multi-principal-element solutions.
Article
Chemistry, Physical
Celeste L. Melamed, Moira K. Miller, Jacob Cordell, Linda Pucurimay, Alyssa Livingood, Rekha R. Schnepf, Jie Pan, Karen N. Heinselman, Fernando D. Vila, Allison Mis, Dennis Nordlund, Ben Levy-Wendt, Stephan Lany, Eric S. Toberer, Steven T. Christensen, Adele C. Tamboli
Summary: This study demonstrates that short-range ordering can tune the optical absorption edge in the long-range disordered alloy system (ZnSnN2)1-x(ZnO)2x at x=0.25. Using combinatorial cosputtering, a set of thin-film samples spanning this alloy space is synthesized. X-ray diffraction confirms the synthesis of a mixed-anion and -cation alloy. X-ray absorption analysis and spectroscopic ellipsometry reveal that local ordering increases the absorption edge energy at constant composition. This work opens up possibilities for property tuning with short-range ordering in (ZnSnN2)1-x(ZnO)2x and similar materials.
CHEMISTRY OF MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
D. Liu, Q. Wang, J. Wang, X. F. Chen, P. Jiang, F. P. Yuan, Z. Y. Cheng, E. Ma, X. L. Wu
Summary: This study investigates CSRO in high-entropy alloys, providing definitive proof through systematic electron microscopy experiments. The CSRO regions occupy 20% of the area fraction and have dimensions on a sub-nanometer scale. Spatial correlation analysis reveals a general tendency towards nearest-neighbor chemical ordering, with a preference for unlike species and an avoidance for like-species.
MATERIALS TODAY NANO
(2021)
Article
Chemistry, Physical
Shang Liu, Alejandra Cuervo Covian, Xiaoxin Wang, Cory T. Cline, Austin Akey, Weiling Dong, Shui-Qing Yu, Jifeng Liu
Summary: This article introduces a new method based on physics-informed Poisson statistical analysis for 3D nanoscale mapping of short-range order (SRO) in GeSn using atom probe tomography (APT) and demonstrates its ability to map semi-quantitative strain. The method provides unique insights into the SRO behavior and can be extended to other alloy systems.
Article
Physics, Applied
Michael Xu, Shaolou Wei, C. Cem Tasan, James M. LeBeau
Summary: The presence of short-range chemical order in metals can significantly affect their mechanical behavior. However, determining the distribution of chemical order in complex alloy systems is challenging. In this study, we use aberration corrected scanning transmission electron microscopy (STEM) and spatial statistics methods to identify and quantify chemical order in the BCC-TiVNbHf(Al) system. Through null hypothesis tests, we differentiate the experimental data from random chemical distribution and find that the experimental results deviate significantly from both random solid solution and fully ordered structures. We also observe and quantify the enhancement of short-range order with the addition of Al. These findings provide valuable insights into the local chemical order in TiVNbHf(Al) alloys and demonstrate the usefulness of spatial statistics in characterizing nanoscale short-range order in complex systems.
APPLIED PHYSICS LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Wei Chen, Lin Li, Qiang Zhu, Houlong Zhuang
Summary: Complex concentrated alloys (CCAs) have attracted significant attention for their wide range of applications and novel properties. Chemical short-range ordering (CSRO) in CCAs plays a crucial role in understanding their properties and phase stability. This article reviews recent experimental efforts in identifying and characterizing CSRO in CCAs, and discusses theoretical and computational techniques, such as density functional theory (DFT) and molecular dynamics (MD), used to investigate CSRO effects.
Article
Materials Science, Multidisciplinary
Flynn Walsh, Anas Abu-Odeh, Mark Asta
Summary: This passage addresses the seemingly contradictory state of research on short-range order in many-component alloys by critically reviewing the characterization of face-centered-cubic 3d systems. Despite the lack of direct observations, the ordering of widely studied alloys is argued to be primarily interesting for its potential ubiquity. To clarify this situation, the article proposes future research directions based on historical results, including a review of the fundamental principles of ordering and clustering.
Article
Chemistry, Multidisciplinary
Jumpei G. Nakamura, Yukinobu Kawakita, Hirotaka Okabe, Bing Li, Koichiro Shimomura, Takashi Suemasu
Summary: Muon spin rotation (mu SR) experiments were conducted to investigate the temperature dependence of the short-range order or correlations of chromium spins in the paramagnetic phase of AgCrSe2. The results showed that short-range spin correlations developed below approximately 184 K, confirming controversial findings from previous quasi-elastic neutron scattering studies. The muon spin relaxation also exhibited a qualitative change and displayed significant missing asymmetry below around 89 K, indicating the presence of short-range spin order.
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
(2023)
Article
Materials Science, Multidisciplinary
E. Antillon, C. Woodward, S. Rao, B. Akdim
Summary: Atomistic methods were used to anneal two BCC chemically complex alloys to evaluate the effect of chemical short-range order on alloy strength. It was found that annealing led to a softening of the BCC quaternary alloy but had minimal effect on solid solution strengthening in the ternary alloy. Results were modeled using an extension of the Suzuki model of substitutional solid solution strengthening, with good agreement between the model results and direct atomistic simulation data.
Article
Materials Science, Ceramics
P. Jovari, V Nazabal, C. Boussard, S. Cui, I Kaban, S. Michalik, M. A. Webb, D. Le Coq, R. Chernikov, N. Chen, J. Darpentigny
Summary: This study examined glasses with approximate compositions of GeTe4-Ag using multiple experimental techniques. By employing simulation techniques, the chemical correlations were determined. The results showed that Ge atoms were mainly fourfold coordinated, while Te atoms were predominantly twofold coordinated. Additionally, the addition of Ag did not alter the topology of the GeTe4 host network, and neighboring GeTe4 tetrahedra continued to predominantly exhibit corner sharing configuration.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2023)
Article
Physics, Fluids & Plasmas
Chae Woo Ryu, Takeshi Egami
Summary: This article discusses the influence of short-range order (SRO) and medium-range order (MRO) on the physical properties of liquids and glasses, showing that MRO plays a critical role in the viscosity of supercooled liquids.
Article
Multidisciplinary Sciences
Anton Gradisek, Tomaz Apih, Maria J. Beira, Carlos Cruz, Susete N. Fernandes, Helena M. Godinho, Pedro J. Sebastiao
Summary: This study used NMR relaxometry to observe dynamic clusters with short-range orientational order in liquids. These clusters exhibit local order driven by interactions between molecules. In liquid crystal, the size of these clusters was observed to increase during the phase transition.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Physical
Stefan Michalik, Pal Jovari, Karel Saksl, Martin Durisin, Dusan Balga, Jacques Darpentigny, Michael Drakopoulos
Summary: Detailed information on the atomic arrangement of glassy Cu54Hf46, Cu61Hf39 and Cu69Hf31 alloys has been obtained through reverse Monte Carlo simulation using high-energy X-ray diffraction and neutron diffraction data. Cu-centered clusters exhibit stronger ordering compared to Hf-centered clusters, and Cu54Hf46 and Cu61Hf39 have better glass forming ability than Cu69Hf31.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Physical
I Pethes, P. Jovari, S. Michalik, T. Wagner, V Prokop, I Kaban, D. Szaraz, A. Hannon, M. Krbal
Summary: Short range order and topology of GexS100-x glasses with a composition range of 20 <= x <= 42 at% were investigated using neutron diffraction, X-ray diffraction, and Ge K-edge extended X-ray absorption fine structure (EXAFS) measurements. The experimental data sets were analyzed using the reverse Monte Carlo simulation method. It was observed that both Ge and S atoms in the glasses satisfied the Mott-rule, with Ge and S atoms having 4 and 2 neighbors, respectively. The chemically ordered network model described the structure of these glasses, with Ge-S bonds being preferred and S-S bonds only present in S-rich glasses. Ge-Ge bonds were found to be necessary in Ge-rich glasses, and the connections between Ge atoms, such as edge-sharing GeS4/2 tetrahedra, were analyzed. The frequency of primitive rings was also calculated.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Engineering, Chemical
Sotiria Mostrou, Mark A. Newton, Andreas Tarcevski, Andreas Nagl, Karin Foettinger, Jeroen A. van Bokhoven
Summary: The oxidation of bio-ethanol to acetic acid using gold nanoparticles supported on silica with titanium showed improved selectivity and increased acetic acid yield compared to pure titania-supported gold. The addition of titanium stabilized the gold nanoparticles and minimized sintering effects, leading to a more efficient catalytic system. Furthermore, the use of mixed supports opens up possibilities for further enhancing ethanol oxidation reactions in industry.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Materials Science, Ceramics
C. Drechsel, H. Peterlik, C. Gierl-Mayer, M. Stoeger-Pollach, T. Konegger
Summary: This study focused on the formation of transient microporosity during the polymer-to-ceramic conversion in polymer-derived ceramics using a poly(vinyl)silazane precursor modified with divinylbenzene as a linker molecule during crosslinking. The introduction of the linker molecule led to distinct changes in elemental composition, structural features, and micropore size in the resulting materials after pyrolysis treatments. Hindered transamination reactions resulted in higher nitrogen content in the linker-containing samples, leading to different composition of micropore-forming entities and smaller pores in the studied system.
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
(2021)
Article
Physics, Applied
Gernot Pacholik, Ludwig Enzlberger, Anna Benzer, Raffael Rameshan, Markus Latschka, Christoph Rameshan, Karin Foettinger
Summary: In this study, various Co, Ni, and K modified MoS2-based catalysts were synthesized and compared in their catalytic performance in CO2 hydrogenation, revealing that the addition of K reduced the selectivity to CH4 and affected the temperature at which the maximum methanol formation rate occurred. The materials were characterized using multiple techniques, and different species of Mo and O were observed under reaction conditions.
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2021)
Article
Materials Science, Ceramics
Renan Belli, Katrin Hurle, Jana Schuerrlein, Anselm Petschelt, Katharina Werbach, Herwig Peterlik, Torsten Rabe, Bjoern Mieller, Ulrich Lohbauer
Summary: This study revised the relationship between fracture toughness and Yttria content in modern zirconia ceramics by evaluating 10 modern Y2O3-stabilized zirconia materials. The study found an inverse power-law behavior between K-Ic and Y2O3 content, as well as a linear relationship between K-Ic and the fraction of the transformable t-phase within a certain range of volume percentage.
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
(2021)
Article
Chemistry, Applied
Thomas Konegger, Christina Drechsel, Herwig Peterlik
Summary: In this study, in-situ small angle X-ray scattering (SAXS) was used to monitor the structural evolution of polymer-derived ceramic materials during the pyrolytic conversion process, focusing on the emergence, transformation, and collapse of transient microporosity. Results showed that the in-situ experiments were in good agreement with conventionally obtained ex-situ data, indicating the significant potential of this method for gaining fundamental insights into the conversion of polymer-derived ceramics.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Dentistry, Oral Surgery & Medicine
Julia Lubauer, Renan Belli, Herwig Peterlik, Katrin Hurle, Ulrich Lohbauer
Summary: Lithium-based glass-ceramics are widely used in dental restorative materials. This study characterized the microstructure, crystalline fraction, glass chemistry, and mechanical properties of eleven commercial dental lithium-based glass ceramics. The results showed significant differences in chemical composition, microstructure, crystallinity, and mechanical properties among these materials. The findings provide valuable information for dentists to make informed choices.
Article
Chemistry, Multidisciplinary
M. Eugenia Perez-Ojeda, Edison Castro, Claudia Kroeckel, Matteo Andrea Lucherelli, Ursula Ludacka, Jani Kotakoski, Katharina Werbach, Herwig Peterlik, Manuel Melle-Franco, Julio C. Chacon-Torres, Frank Hauke, Luis Echegoyen, Andreas Hirsch, Gonzalo Abellan
Summary: In this study, covalently functionalized carbon nano-onions (CNOs) were synthesized using a reductive approach with unprecedented alkali-metal CNO intercalation compounds. The controlled intercalation process with potassium was investigated for the first time, revealing a Fano resonance in highly doped CNOs. The experimental results were further confirmed by electron energy loss spectroscopy, X-ray diffraction, and rationalized with DFT calculations. This work provides important insights into reductive CNO functionalization principles and potential applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Engineering, Biomedical
Julia Lubauer, Katrin Hurle, Maria Rita Cicconi, Anselm Petschelt, Herwig Peterlik, Ulrich Lohbauer, Renan Belli
Summary: The research found that the Obsidian glass-ceramic went through two growth stages during the crystallization process, and the changes in crystal phase fraction were accompanied by a transition in crystal phase types, indicating a change in mechanical properties; during the crystallization process, the toughness of the material showed a reverse trend with the decrease in crystal fraction and size, mainly due to the relaxation of residual stresses caused by the spheroidization of crystals.
JOURNAL OF THE MECHANICAL BEHAVIOR OF BIOMEDICAL MATERIALS
(2021)
Article
Chemistry, Physical
Alberto Tampieri, Karin Foettinger, Noelia Barrabes, Francesc Medina
Summary: Bio-derived furfural and 5-hydroxymethylfurfural can be reacted with acetone to produce biofuel and polymer precursors. Catalytic systems were explored to efficiently obtain and purify each product. In situ/operando ATR-IR and in situ NMR techniques were used to monitor the reaction and study its reactivity and stereoselectivity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Applied
Alexander Bartik, Josef Fuchs, Gernot Pacholik, Karin Foettinger, Hermann Hofbauer, Stefan Mueller, Florian Benedikt
Summary: This study investigates the catalytic methanation of syngas from dual fluidized bed steam gasification of biomass in an innovative bubbling fluidized bed methanation reactor with an optimized catalyst. The results suggest that sorption enhanced reforming in combination with an optimized fluidized bed methanation can lead to technical and economic improvements in sustainable synthetic natural gas production.
FUEL PROCESSING TECHNOLOGY
(2022)
Article
Chemistry, Applied
M. Latschka, B. Wellscheid, R. Rameshan, T. Schoeberl, J. Essmeister, G. Pacholik, F. Valentini, L. Balta, A. Limbeck, C. Rameshan, H. Kaehlig, K. Foettinger
Summary: Zeolite Y is widely used in catalysis for its high surface area and strong acidity. The impact of flowing water on zeolite Y was investigated, and it was found that water treatment caused significant structural changes and the formation of amorphous phase and small mesopores.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
E. Szoldatits, J. Essmeister, L. Schachtner, T. Konegger, K. Foettinger
Summary: In this study, Ni supported on polymer-derived ceramics was investigated as a new class of catalyst materials. The polymer-derived ceramics meet the requirements of outstanding thermal and mechanical stability for catalysts and offer the opportunity for complex porous structures.
FRONTIERS IN CHEMISTRY
(2023)
Article
Biotechnology & Applied Microbiology
Roghayeh Shirvani, Alexander Bartik, Gustavo A. S. Alves, Daniel Garcia de Otazo Hernandez, Stefan Mueller, Karin Foettinger, Matthias G. Steiger
Summary: Carbon and nitrogen are important elements that need to be efficiently regenerated in a circular economy. Gasification technology can utilize challenging waste streams and produce syngas that can be further processed into various useful products. This study focuses on recovering nitrogen from gasification byproduct gas cleaning to form protein-rich yeast biomass.
FRONTIERS IN BIOENGINEERING AND BIOTECHNOLOGY
(2023)
Article
Chemistry, Physical
Hipassia M. Moura, Herwig Peterlik, Miriam M. Unterlass
Summary: This study presents a one-pot hydrothermal synthesis of inorganic-organic hybrid materials, achieving the concomitant synthesis, nanoscopic interpenetration, and covalent linking of components, leading to synergistic materials properties and improved thermal stability in PBI@SiO2 class II hybrids. The hybrids are utilized as heterogeneous and reusable photoredox catalysts for the reduction of aryl halides, demonstrating good optoelectronic properties. Small-angle X-ray scattering and powder X-ray diffraction revealed the existence of ordered intermediates in the synthesis process, shedding light on the structure formation mechanisms in sol-gel processes.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Electrochemistry
Katharina Werbach, Christian Neiss, Alexander Muellner, Gonzalo Abellan, Daria Setman, Vicent Lloret, Stefan Wild, Frank Hauke, Thomas Pichler, Andreas Hirsch, Herwig Peterlik
Summary: The solid-state synthesis of pure sodium-black phosphorus intercalation compounds (Na-BPICs) has been optimized in bulk for two stoichiometric ratios. By introducing a new synthetic route based on thermal ball milling, the formation of undesired Na3P was significantly reduced. A new structural model for Na-based BPICs was developed through the combination of XRD, Raman spectroscopy, and DFT calculations, paving the way for large-scale synthesis and application in fields such as optoelectronics and energy storage.
BATTERIES & SUPERCAPS
(2021)
