Article
Chemistry, Physical
Xinli Wang, Canying Cai, Guangwen Zhou
Summary: This study elucidates the interfacial dynamics of hafnium with gamma-Al2O3 and theta-Al2O3 during the oxidation of Ni-Al alloys. The presence of interfacial Al vacancies plays a critical role in influencing the interfacial segregation of Hf atoms and HfO2 formation. The results provide insights into manipulating the interfacial transport process of reactive elements by controlling the phase and stoichiometry of the transient oxide phases.
APPLIED SURFACE SCIENCE
(2022)
Article
Materials Science, Multidisciplinary
C. Ferreira-Palma, M. C. Poletti, R. M. Pineda-Huitron, V. M. Lopez-Hirata, D. Rivas-Lopez, H. J. Dorantes-Rosales
Summary: This study investigates the effects of Cr content on the precipitation of beta ' in Fe-Ni-Al ferritic alloys. It is found that an increase in Cr shifts the dissolution of beta ' to higher temperatures and lowers the Curie point, while also increasing the coarsening rate of the beta ' phase with higher Cr concentrations. The addition of Cr in these alloys presents a tradeoff between increased corrosion resistance and extended beta ' stability range against the partial loss of coherency and a higher coarsening rate.
METALLURGICAL AND MATERIALS TRANSACTIONS A-PHYSICAL METALLURGY AND MATERIALS SCIENCE
(2021)
Article
Chemistry, Physical
Min Wu, Haojie Zhu, Jing Wang, Junliang Wang, Jianguo Zhu
Summary: Hydrogen embrittlement is a major obstacle for the application of hydrogen energy. This study found that doping nickel in iron structures can suppress hydrogen diffusion, which is significant for understanding hydrogen embrittlement.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Lu-Yao Hao, Xu-Zhong Wen, Xiao-Wei Lei, Wen-Jing Yao, Nan Wang
Summary: The diffusion behavior of nitrogen at the interface of Ni-based superalloys was investigated using first-principles calculations. It was found that the γ matrix provides more trapping sites for nitrogen atoms compared to the γ' precipitate, due to the preference of nitrogen atoms to occupy the 6-Ni octahedral interstitial site. The migration energy barrier for nitrogen crossing the (002)γ/γ' coherent plane is higher in the γ phase, indicating that nitrogen atoms can move into the γ' phase only under certain conditions. The low diffusion ability of nitrogen in the γ' phase and the potential barrier role of the (002)γ/γ' coherent plane contribute to the unfavorable nitriding behavior of the γ' phase in Ni-based superalloys.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Chemistry, Physical
Veronique Van Speybroeck, Massimo Bocus, Pieter Cnudde, Louis Vanduyfhuys
Summary: In this Perspective, the role of first-principles molecular dynamics (MD) simulations in unraveling the catalytic function within zeolites under operating conditions is critically reflected upon. Through a series of exemplary cases, it is demonstrated how first-principles MD simulations can provide insights into the molecular-scale complexity of catalysts, allowing for the discovery of competitive pathways and exploration of broad transition state regions. However, there are still major hurdles to overcome in fully integrating these simulations into computational catalytic workflows.
Article
Chemistry, Physical
Wiwittawin Sukmas, Prutthipong Tsuppayakorn-aek, Prayoonsak Pluengphon, Stewart J. Clark, Rajeev Ahuja, Thiti Bovornratanaraks, Wei Luo
Summary: Focusing on ternary metal hydrides has become a new area of research for high-temperature superconductors affected by pressure, owing to the various combinations of alloying metals, even metalloids, and hydrogen. Using first-principles evolutionary techniques, this study predicts new phases of Mg-B-H ternary hydrides and confirms their dynamic stability and potential as conductors through phonon and electronic calculations. The metallic MgBH9 phase exhibits a superconducting state with a maximum Tc of 64 K at 110 GPa, with its spectral function primarily active in the optical modes. On the other hand, non-metallic candidate MgB2H8 shows hydrogen-vacancy diffusion kinetics determined by total energy calculations, indicating that pressure reduces the activation energy through optimal inter-fragment distances of H-H(B).
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Yubo Sun, Zhiping Wang, Mingrun Du, Yimeng Du, Wang Zhang
Summary: The diffusion behavior of Si atoms in Ni-based superalloys was evaluated using first-principles calculations. The occupation of Si atoms as melting point depressants in Cr, Mo, and W doped γ-Ni and γ'-Ni3Fe supercells was discussed, and the diffusion behavior of Si atoms in adjacent octahedral interstices was analyzed. The results show that the addition of alloying elements Cr, Mo, and W decreases the formation enthalpy and improves stability, leading to a higher inclination of Si atoms to occupy octahedral interstices. Increasing the radius of the doped alloy element increases the diffusion energy barrier. Moreover, Si atoms in γ'-Ni3Fe exhibit two diffusion paths, with the diffusion energy barrier around shared Fe atoms being significantly lower than that around shared Ni atoms. The increase in interaction strength between the doped M atom/octahedron constituent atom and Si atom promotes Si atom diffusion and lowers the diffusion energy barrier. The diffusion behavior of Si atoms provides a theoretical basis for the phase structure evolution in wide-gap brazed joints.
Article
Chemistry, Physical
Jiayao Qin, Zhigao Liu, Wei Zhao, Dianhui Wang, Yanli Zhang, Yan Zhong, Xiaohui Zhang, Zhongmin Wang, Chaohao Hu, Jiangwen Liu
Summary: Hydrogen embrittlement causes material degradation in metal-hydrogen systems. Alloying with Ni can improve the stability and resistance to H embrittlement of VHx phases in pure V. The addition of Ni helps reduce the H trapping ability of vacancies and suppresses H retention in V.
Article
Nanoscience & Nanotechnology
Jiexiang Li, Min Yang, Xiaoming Zhang, Jiawei Wen, Chunxia Wang, Guoyong Huang, Weiyu Song
Summary: This study theoretically investigated the discharge process of LiMn2O4 and LiNi0.5Mn1.5O4 and found that it is accompanied by an increase in unit cell volume and lattice distortion. Additionally, 25% Ni-substitution increased the average calculated voltage of LiMn2O4 from 3.83 V to 4.61 V and reduced the Li-ion diffusion barrier, improving the intrinsic rate performance of LiMn2O4.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Multidisciplinary Sciences
Jussi Lehtonen
Summary: This article reviews the experiments and concepts presented by Angus Bateman in 1948 regarding sexual selection and the Bateman gradient. The study develops mathematical models showing that asymmetry in gamete numbers alone can generate steeper Bateman gradients in males. The research provides evidence for Bateman's claim about the role of gamete numbers in sexual selection.
NATURE COMMUNICATIONS
(2022)
Article
Nanoscience & Nanotechnology
Zhiwen Min, Chunlei Yang, Guo-Hua Zhong, Ziheng Lu
Summary: Lithium-rich ternary phosphides have high ionic conductivity but their electrochemical and interfacial stability in complex battery setups are poorly characterized. This study examines their phase stability and electrochemical stability using first-principles calculations and thermodynamic analysis. While they have narrow intrinsic electrochemical stability windows, they show high efficiency in lithium conduction and impressive lithium storage capacity, making them potential anode materials for high-rate and energy-dense batteries.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Materials Science, Multidisciplinary
Yanli Lu, Yi Wang, Yifan Wang, Meng Gao, Yao Chen, Zheng Chen
Summary: The study found that the hydrogen solution energy of V-Ni-M alloys is higher than pure vanadium, but the ability to capture hydrogen atoms is lower. In addition, V-Ni-M alloys exhibit higher resistance to embrittlement and smaller diffusion coefficients, making them suitable for hydrogen separation. In terms of mechanical properties, V-Ni-Ti has the best deformation resistance, while V-Ni-Si performs best in terms of thermal properties.
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
(2021)
Article
Materials Science, Multidisciplinary
M. Seyring, F. Wanierke, T. Kaaden, S. Lippmann, M. Rettenmayr
Summary: The study demonstrates the significant influence of natural oxide layers on the formation of Ni3Al phase at (Ni)/NiAl interfaces. These oxide layers act as diffusion barriers, retarding or locally suppressing growth of Ni3Al into the (Ni) phase. Removing the oxide layers leads to higher interdiffusion coefficients in diffusion couples.
MATERIALS CHARACTERIZATION
(2021)
Article
Chemistry, Multidisciplinary
Xiaoliang Wang, Haonan Zhao, Leiming Chang, Zhenqiu Yu, Zhiwu Xiao, Shuwei Tang, Chuanhui Huang, Jingxin Fan, Shaobin Yang
Summary: The size and arrangement structure of anions have an impact on the interlayer spacing and structural stability of LDHs. The larger the interlayer anion diameter, the larger the interlayer spacing.
Article
Engineering, Mechanical
Xiaolin Song, Xuanran Fu, Meng Wang
Summary: Resource conservation and environmental protection have made lightweight materials like magnesium alloys essential for rail transit. This study investigates the structure and properties of the beta ' phase in Mg-RE (RE = Y, Gd, Tb, or Dy) alloys using first-principles calculations. The results show that these alloys are thermodynamically and mechanically stable, and the addition of RE improves their elastic moduli, especially Young's modulus. Moreover, Mg-RE alloys exhibit better hardness and elastic anisotropy compared to α-Mg, due to the strong metallic bonds between RE and Mg atoms.
INTERNATIONAL JOURNAL OF MECHANICAL SCIENCES
(2023)
Article
Chemistry, Physical
J. Mark P. Martirez, Emily A. Carter
Summary: Ammonia is considered a practical means for hydrogen transportation due to its higher volumetric energy density. By using density functional theory, the researchers studied the decomposition of NH3 on a catalyst and predicted surface phase diagrams that provide insights for designing efficient catalysts for NH3 decomposition. It was found that a catalyst with weakened N binding is needed to enable high-turnover NH3 decomposition.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Multidisciplinary Sciences
Yigao Yuan, Linan Zhou, Hossein Robatjazi, Junwei Lucas Bao, Jingyi Zhou, Aaron Bayles, Lin Yuan, Minghe Lou, Minhan Lou, Suman Khatiwada, Emily A. Carter, Peter Nordlander, Naomi J. Halas
Summary: Plasmonic photocatalysis can transform a thermally unreactive transition metal into a catalytically active site, achieving efficient photocatalytic decomposition of ammonia.
Article
Multidisciplinary Sciences
Robert B. Wexler, Emily A. Carter
Summary: This study used DFT to investigate the factors controlling species oxidation selectivity in seawater electrolysis and found that the metal redox activity determines the strength of oxygen chemisorption. The study also revealed a strong correlation between oxygen and chlorine chemisorption, posing a fundamental challenge for seawater electrode material design.
ADVANCED THEORY AND SIMULATIONS
(2023)
Editorial Material
Chemistry, Physical
Emily A. Carter, Mark A. Johnson, Stephen R. Leone
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Biographical-Item
Chemistry, Physical
Emily A. Carter, Mark A. Johnson, Stephen R. Leone
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Lesheng Li, Marcos Calegari F. Andrade, Roberto Car, Annabella Selloni, Emily A. Carter
Summary: In this study, the influence of different TiS2 surface terminations on its interface with water was revealed through deep potential molecular dynamics simulations. Zigzag-L was identified as the only interface that favors water dissociation thermodynamically and kinetically, with the coexistence of four-fold-coordinated Ti and one-fold-coordinated S atoms on the surface playing a crucial role in proton transfer. This work provides new insights for the future design and optimization of TiS2-based CDI devices for water desalination.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Biographical-Item
Chemistry, Physical
Emily A. Carter, Mark A. Johnson, Stephen R. Leone
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Jin Cai, Qing Zhao, Wei-You Hsu, Chungseok Choi, Yang Liu, John Mark P. Martirez, Chih Chen, Jin Huang, Emily A. Carter, Yu Huang
Summary: A highly (111)-oriented Cu foil electrocatalyst with dense twin boundaries (tw-Cu) is demonstrated to exhibit high selectivity towards CH4 in the electrochemical carbon dioxide reduction reaction. The tw-Cu catalyst achieves a high Faradaic efficiency of 86.1 +/- 5.3% for CH4 production. Theoretical studies suggest that tw-Cu reduces the reduction barrier for the rate-determining hydrogenation of CO compared to planar Cu(111), leading to the observed high CH4 selectivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
John Mark P. Martirez, Emily A. Carter
Summary: Simulations of carbon dioxide in water can help understand its impact on aquatic environments and advance carbon capture and utilization technologies. Only by using quantum mechanical simulations and rare-event sampling, combined with energy corrections, can the theoretical results closely match experimental data. These multilevel simulations can serve as benchmarks for simpler models and provide insights into their potential errors.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Pengcheng Chen, Dingxin Fan, Annabella Selloni, Emily A. Carter, Craig B. Arnold, Yunlong Zhang, Adam S. Gross, James R. Chelikowsky, Nan Yao
Summary: By using high-resolution noncontact atomic force microscopy, the authors successfully identified two adjacent transition-metal atoms (Fe and Co) within phthalocyanine molecules. The AFM imaging showed that the Co atom was brighter and had four distinct lobes on the horizontal plane, while the Fe atom had a square morphology. Pico-force spectroscopy measurements revealed a larger repulsion force exerted by Co compared to Fe. The experimental and theoretical results demonstrated that the distinguishable features in AFM images and the variation in measured forces were due to Co's higher electron orbital occupation above the molecular plane. The ability to directly observe orbital signatures using HR-AFM provides a promising approach for characterizing the electronic structure of individual atoms in molecular species and understanding mechanisms of certain chemical reactions.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Jan-Niklas Boyn, Emily A. Carter
Summary: The dehydration dynamics of aqueous Ca2+ and Mg2+ cations are important in chemical and biological phenomena and have particular relevance in carbon capture techniques. This study investigates the dehydration process of these cations using rare event sampling and provides insights into the effect of pH on their stability.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Robert B. Wexler, Gopalakrishnan Sai Gautam, Robert T. Bell, Sarah Shulda, Nicholas A. Strange, Jamie A. Trindell, Joshua D. Sugar, Eli Nygren, Sami Sainio, Anthony H. McDaniel, David Ginley, Emily A. Carter, Ellen B. Stechel
Summary: This study demonstrates the synthesis of the perovskite Ca2/3Ce1/3Ti1/3Mn2/3O3, which has high phase purity, stability, and desirable redox thermodynamics for solar thermochemical H2 production (STCH) with a predicted average neutral oxygen vacancy formation energy of 3.30 eV. Experimental results indicate that this material has comparable or greater H2 production capacity than other promising metal oxide perovskites. Quantum-based modeling reveals that Ce4+ reduction dominates the redox activity of Ca2/3Ce1/3Ti1/3Mn2/3O3, and X-ray absorption spectroscopy measurements confirm reversible Ce4+ to Ce3+ reduction. The refinement of Ce stoichiometry has the potential to further enhance the performance of this material.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Ziyang Wei, John Mark P. Martirez, Emily A. Carter
Summary: This article introduces the random phase approximation (RPA) as a method for treating electron correlation, which has been shown to outperform standard density functional theory (DFT) approximations in cases such as extended surfaces. By using sub-system embedding schemes, the RPA can be used to simulate heterogeneous reactions at a reduced computational cost. The authors explore two embedded RPA approaches, periodic emb-RPA and cluster emb-RPA, and validate them in the H-2 dissociative adsorption on Cu(111) surface, finding that cluster emb-RPA accurately reproduces the energy profile while significantly reducing computational cost.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Jan-Niklas Boyn, Emily A. Carter
Summary: The dehydration of aqueous calcium and magnesium cations is a fundamental process controlling their reactivity and plays a crucial role in carbon capture techniques. Understanding the dehydration dynamics of these cations is important for utilizing seawater as a source of carbon storage through the formation of carbonate minerals. However, there is limited atomic-scale understanding of the dehydration process.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Andrew M. Teale, Trygve Helgaker, Andreas Savin, Carlo Adamo, Balint Aradi, Alexei Arbuznikov, Paul W. Ayers, Evert Jan Baerends, Vincenzo Barone, Patrizia Calaminici, Eric Cances, Emily A. Carter, Pratim Kumar Chattaraj, Henry Chermette, Ilaria Ciofini, T. Daniel Crawford, Frank De Proft, John F. Dobson, Claudia Draxl, Thomas Frauenheim, Emmanuel Fromager, Patricio Fuentealba, Laura Gagliardi, Giulia Galli, Jiali Gao, Paul Geerlings, Nikitas Gidopoulos, Peter M. W. Gill, Paola Gori-Giorgi, Andreas Gorling, Tim Gould, Stefan Grimme, Oleg Gritsenko, Hans Jorgen Aagaard Jensen, Erin R. Johnson, Robert O. Jones, Martin Kaupp, Andreas M. Koster, Leeor Kronik, Anna Krylov, Simen Kvaal, Andre Laestadius, Mel Levy, Mathieu Lewin, Shubin Liu, Pierre-Francois Loos, Neepa T. Maitra, Frank Neese, John P. Perdew, Katarzyna Pernal, Pascal Pernot, Piotr Piecuch, Elisa Rebolini, Lucia Reining, Pina Romaniello, Adrienn Ruzsinszky, Dennis R. Salahub, Matthias Scheffler, Peter Schwerdtfeger, Viktor N. Staroverov, Jianwei Sun, Erik Tellgren, David J. Tozer, Samuel B. Trickey, Carsten A. Ullrich, Alberto Vela, Giovanni Vignale, Tomasz A. Wesolowski, Xin Xu, Weitao Yang
Summary: This paper provides an informal review and discussion on the history, present status, and future of density-functional theory (DFT) by 70 workers in the field. The format of a roundtable discussion allowed participants to express their views through 302 individual contributions to a preset list of 26 questions. Supported by a bibliography of 777 entries, the paper offers a comprehensive snapshot of DFT in 2022.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)