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
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
Chemistry, Physical
Yongli Li, Wenli Xia, Jingyu Qin, Degang Zhao, Min Zuo
Summary: This study investigated the featured local structure units and microstructure evolution of Cu-Fe-P immiscible alloy through first principle molecular dynamics simulation, revealing the tendency of P atoms to connect with Fe. Special clusters containing P were determined at different temperatures, and XRD analysis identified the composition of the alloy and observed an evolving core-shell structure. The controlled synthesis of Fe-P spheres with and without pores could be achieved with phase extraction of the Cu-32Fe-8P alloy, providing a novel route for the wider potential application of functional phosphides.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Nanoscience & Nanotechnology
Xiaofeng Yang, Yongzhi Xi, Chenyun He, Hao Chen, Xiancheng Zhang, ShanTung Tu
Summary: In this study, the enhancing effect of chemical short-range order (SRO) structure on CoCrNi medium-entropy alloy (MEA) was investigated using molecular dynamics simulations of nanoindentation. Results showed a quantitative correlation between SRO parameters and mechanical properties, with strength and hardness of the alloy increasing with higher SRO parameters until reaching a stable value. Additionally, an increase in average hardness and dislocation nucleation force were observed in models with intermediate and stable SRO structures compared to a random solid solution (RSS) state model.
SCRIPTA MATERIALIA
(2022)
Article
Nanoscience & Nanotechnology
Hamdy Arkoub, Miaomiao Jin
Summary: Chemical short-range order (CSRO), a nanoscale atomic feature, has been shown to significantly affect defect properties and radiation behavior in Fe-Ni-Cr alloys. Molecular dynamics simulations reveal that random solutions, characterized by negative stacking fault energy, exhibit the strongest diffusion tendency, while high CSRO degrees reduce defect diffusivity due to trapping effects. In high-CSRO scenarios, interstitial clusters become Cr-rich and interstitial loops prefer Cr-rich CSRO domains. CSRO dynamically evolves during irradiation and reaches a steady-state value. These findings emphasize the importance of considering CSRO when investigating radiation-driven microstructural evolution.
SCRIPTA MATERIALIA
(2023)
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
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
Multidisciplinary Sciences
Flynn Walsh, Mark Asta, Robert O. Ritchie
Summary: The presence, nature, and impact of chemical short-range order in the multi-principal element alloy CrCoNi are currently under debate, with first-principles calculations revealing a magnetic origin to this phenomenon. Models based on magnetic interactions are found to explain experimental anomalies, suggesting that short-range order of this type may be more common than previously realized.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
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
Physics, Condensed Matter
LiJun Yuan, Ran Tao, PengCheng Wen, Jing Li, Shen Wang, Da Li
Summary: The strengthening effect and micro mechanism of CSRO on FCC FeNiCrCoAlx alloys were studied using Molecular Dynamics simulation method. The results show that CSRO can increase the alloy's yield strength, reduce dislocation slip, and has a more significant strengthening effect at room and low temperatures.
PHYSICA B-CONDENSED MATTER
(2023)
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
Multidisciplinary Sciences
Xuefei Chen, Qi Wang, Zhiying Cheng, Mingliu Zhu, Hao Zhou, Ping Jiang, Lingling Zhou, Qiqi Xue, Fuping Yuan, Jing Zhu, Xiaolei Wu, En Ma
Summary: The study provides direct experimental evidence of chemical short-range atomic-scale ordering (CSRO) in a VCoNi medium-entropy alloy through diffraction and electron microscopy analysis. The research demonstrates that using specific crystallographic directions can reveal CSRO in face-centred-cubic VCoNi concentrated solution, offering insights into atomic packing configuration and dislocation interactions enhanced by CSROs.
Article
Materials Science, Multidisciplinary
Irene J. Beyerlein, Penghui Cao, Tresa M. Pollock
Summary: Complex concentrated alloys (CCAs) are materials with three or more elements in similar proportions and lacking chemical long-range order. They have attracted attention in the past two decades and offer a new materials design paradigm for applications in aggressive environments. However, understanding their behavior is challenging due to the fluctuating chemical and structural variations at the atomic and nanoscales.
Article
Materials Science, Multidisciplinary
Y. Rao, W. A. Curtin
Summary: In this study, a statistical-mechanics analysis is used to estimate the short-range order (SRO) parameters in solid solution alloys. The analysis assumes pair interactions among atoms at different distances and treats the crystal as a set of independent clusters. The results allow for a fast assessment of likely SRO using estimated or computed inputs for atom-atom interaction energies.
Article
Materials Science, Multidisciplinary
Xin Liu, W. A. Curtin
Summary: A recent theory has been developed for strengthening multicomponent non-dilute alloys with short-range order (SRO). The theory predicts that SRO has a notable effect on solute-dislocation interactions, which can either decrease or increase alloy strength. Atomistic simulations in a binary NbW alloy validate the theory and demonstrate the unexpected possibility of reduced strength due to SRO. The findings also further validate the analytical theory as a tool for alloy design.
Article
Chemistry, Physical
Remco Dalebout, Laura Barberis, Giorgio Totarella, Savannah J. Turner, Camille La Fontaine, Frank M. F. de Groot, Xavier Carrier, Ad M. J. van der Eerden, Florian Meirer, Petra E. de Jongh
Summary: Despite the ongoing debate on the nature of Cu-ZnOx synergy and the active Zn-based promoter species in methanol synthesis, this study uses weakly interacting graphitic carbon supports to investigate the active speciation of Zn promoter phase in contact with Cu nanoparticles under working conditions. The results reveal that most of the added Zn is in a zerovalent oxidation state during methanol synthesis conditions, and the Zn diffuses into the Cu nanoparticles. This study provides insights into the speciation of relevant Zn promoter species and highlights the importance of using weakly interacting graphitic supports for studying the nature of promoter species.
Correction
Chemistry, Physical
Diana Chaykina, Ismene Usman, Giorgio Colombi, Herman Schreuders, Beata Tyburska-Pueschel, Ziying Wu, Stephan W. H. Eijt, Lars J. Bannenberg, Gilles A. de Wijs, Bernard Dam
Summary: The energy axes of the RBS and ERD data were initially underestimated, but the correction does not affect the data conclusions and peak assignments.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Nanoscience & Nanotechnology
Lars J. Bannenberg, Herman Schreuders, Nathan van Beugen, Christy Kinane, Stephen Hall, Bernard Dam
Summary: In the future hydrogen economy, accurate, cost-efficient, and safe hydrogen sensors based on metal hydrides will be important. Alloying can tune the properties of hydrogen-sensing materials, as demonstrated by thin films of tantalum doped with ruthenium. The alloying effects include modifying the enthalpy of hydrogenation, shifting the pressure window for hydrogen absorption, and reducing the amount of hydrogen absorbed by the material, allowing for tunable sensitivity and a wide sensing range.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
M. Fuhrer, T. van Haasterecht, E. J. J. de Boed, P. E. de Jongh, J. H. Bitter
Summary: In this study, carbon nanofiber-supported mixed Mo/W-carbide catalysts with varying compositions were prepared using different synthesis methods. The results showed that regardless of the synthesis method, all bimetallic catalysts were mixed at the nanoscale, although the Mo/W ratio in individual nanoparticles varied. The crystal structures and nanoparticle sizes differed depending on the synthesis method, and the TPR-synthesized carbides exhibited higher activity for the hydrodeoxygenation of fatty acids.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Laura de Kort, Peter Ngene, Marcello Baricco, Petra de Jongh, Valerio Gulino
Summary: It was found that the addition of silica nanoparticles to iodide-substituted LiBH4 significantly improves the ion conductivity and cycle life of all-solid state batteries. The synthesized h-Li(BH4)0.8(I)0.2-SiO2 demonstrates a Li+ conductivity of 9.3 x 10-5 S cm-1 at room temperature and an improved stability against Li-metal. The all-solid state battery Li|h-Li(BH4)0.8(I)0.2-SiO2|TiS2 showed good long-term cyclability, demonstrating the enhanced cycling stability of the electrolyte due to the addition of oxide nanoparticles.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Pan Li, Sven H. C. Askes, Esther del Pino Rosendo, Freek Ariese, Charusheela Ramanan, Elizabeth von Hauff, Andrea Baldi
Summary: In this work, temperature measurements at the nanoscale were achieved by exploiting the combination of surface-enhanced Raman spectroscopy and the temperature dependence of Raman peaks in beta-CuPc. The temperature of plasmonic gold nanoparticles under laser irradiation was determined by measuring the temperature-dependent Raman shifts of beta-CuPc films coated on an array of Au nanodisks and using calibration curves. The extracted temperatures were confirmed to be consistent with numerical modeling results.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Biochemistry & Molecular Biology
Radovan Cerny, Matteo Brighi, Hui Wu, Wei Zhou, Mirjana Dimitrievska, Fabrizio Murgia, Valerio Gulino, Petra E. de Jongh, Benjamin A. Trump, Terrence J. Udovic
Summary: This study investigates the thermal polymorphism in CsCB11H12 and discovers the existence of two polymorphs: the ordered R3 polymorph at around 313K and the disordered I43d polymorph at around 353K. Additionally, it identifies a disordered Fm3 polymorph appearing from the disordered I43d polymorph at 513K and transforming into a high-temperature P6(3)mc polymorph. Neutron scattering results show isotropic rotational diffusion of CB11H12- anions in the disordered phase at 560K.
Article
Chemistry, Physical
Andrea Baldi, Sven H. C. Askes
Summary: This study breaks the limitations of traditional steady-state modes by using ultrashort light pulses and photothermal nanoparticle arrays to modulate the temperature of catalytic sites, achieving high energy efficiency and high catalytic activity in dynamic catalytic reactions. Numerical simulations demonstrate that pulsed photothermal catalysis can operate at room temperature, resist catalyst poisons, and access adsorbed reagent distributions that are normally inaccessible. The study provides key experimental parameters for controlling reaction rates in pulsed heterogeneous catalysis and offers specific recommendations to explore its potential in real experiments, paving the way for a more energy-efficient and process intensive operation of catalytic reactors.
Article
Nanoscience & Nanotechnology
Diana Chaykina, Giorgio Colombi, Herman Schreuders, Bernard Dam
Summary: Rare-earth metal oxyhydride thin films exhibit photochromism, causing reversible darkening when exposed to high-energy light. In this study, samarium oxyhydrides were included in the range of known photochromic RE-oxyhydrides. The properties of the Sm-oxyhydride film, such as optical bandgap, lattice constant, photochromic contrast, and bleaching speed, were controlled by the deposition pressure during reactive magnetron sputtering of SmH1.9+delta and post-oxidation. The slower bleaching speeds in Sm oxyhydrides compared to other lanthanides are attributed to the stability of the Sm2+ state and the difficulty in oxidizing it back to the original RE3+ state.
Article
Materials Science, Multidisciplinary
Giorgio Colombi, Bart Boshuizen, Diana Chaykina, Leyi Hsu, Herman Schreuders, Tom J. Savenije, Bernard Dam
Summary: Rare-earth oxyhydride thin films exhibit reversible photochromism and photoconductivity at ambient conditions, but the underlying mechanism and relationship are not clear. In this study, in situ time-resolved measurements of optical and transport properties were performed on Gd-based oxyhydride thin films to investigate this question. It was found that the initial mechanism of charge transport is p-type large polaron conduction; however, upon photo-darkening, a 10(4)-fold increase in conductivity occurs, and n-type carriers dominate. Furthermore, both photochromism and photoconductivity were shown to originate from a single process, as the photoconductivity is exponentially proportional to the increase in optical absorption. This exponential relationship suggests that the formation of optically absorbing species responsible for photochromism is accompanied by a concerted increase in negative charge carriers in the Gd oxyhydride films.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Luc C. J. Smulders, Johan H. van de Minkelis, Johannes D. Meeldijk, Min Tang, Anna Liutkova, Kang Cheng, S. Tegan Roberts, Glenn J. Sunley, Emiel J. M. Hensen, Petra E. de Jongh, Krijn P. de Jong
Summary: In this study, the heat treatment of the catalyst precursor was found to influence the location of Pd precursor within SAPO-11 and ZSM-22 zeotype materials, which in turn affects the performance of the catalyst. The catalytic performance of the Pd-on-zeotype catalysts prepared using the direct reduction approach is intermediate between that of the Pd-in-zeotype catalysts prepared using the calcination-reduction approach and that of the Pd-on-alumina catalysts.
CHEMISTRY-SWITZERLAND
(2023)
Article
Chemistry, Multidisciplinary
Nienke L. Visser, Savannah J. Turner, Joseph A. Stewart, Bart D. Vandegehuchte, Jessi E. S. van der Hoeven, Petra E. de Jongh
Summary: In this study, the movement and growth of supported nickel nanoparticles in CO2 hydrogenation reaction were visualized using in-situ gas-phase transmission electron microscopy. Two modes of particle movement with different velocities were observed, and two distinct particle growth mechanisms, diffusion and coalescence, and Ostwald ripening, were visualized. An interplay between the two mechanisms was demonstrated, where coalescence was followed by fast Ostwald ripening. This study highlights the importance of studying nanoparticle growth in supported ensembles for the understanding of stability in metal catalysts.
Article
Chemistry, Physical
Shrestha Banerjee, Diana Chaykina, Rens Stigter, Giorgio Colombi, Stephan W. H. Eijt, Bernard Dam, Gilles A. A. de Wijs, Arno P. M. Kentgens
Summary: Rare earth oxyhydrides REOxH(3-2x), with RE = Y, Sc, or Gdand a cationic FCC lattice, show reversible photochromic behavior. The efficiency of the photochromism is determined by the structural details and anion composition. In this study, NMR spectroscopy and DFT calculations are used to investigate the local environments, oxidation states, and dynamics of yttrium, hydrogen, and oxygen in YOxH(3-2x). The results suggest that the samples consist of domains with different hydride contents rather than a homogeneous anion mixing.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Tom A. J. Welling, Suzan E. Schoemaker, Krijn P. de Jong, Petra E. de Jongh
Summary: Gas-cell transmission electron microscopy has enabled direct, nanoscale imaging of catalysts during reaction. We compared the growth rates of carbon nanofibers measured gravimetrically in a reactor and observed through electron microscopy, and found good agreement. This allowed for detailed insight into the contribution of individual catalyst nanoparticles in these heterogeneous catalysts to overall carbon growth. The methodology of nanoscale in situ observations paves the way for understanding macroscopic rates of catalyzed reactions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Letter
Multidisciplinary Sciences
Thomas Burdyny, Bernard Dam
