Article
Materials Science, Multidisciplinary
Atsushi Hariki, Keisuke Higashi, Tatsuya Yamaguchi, Jiebin Li, Curran Kalha, Manfred Mascheck, Susanna K. Eriksson, Tomas Wiell, Frank M. F. de Groot, Anna Regoutz
Summary: This paper explores the satellites of the Ti 1s and 2p core level spectra of SrTiO3 and TiO2 using hard x-ray PES. The theoretical analysis emphasizes the importance of higher-order Ti-O charge-transfer processes and provides a robust prescription for using the computationally cheap cluster model in fitting analyses of core level spectra.
Article
Multidisciplinary Sciences
J. Niskanen, A. Vladyka, J. Niemi, C. J. Sahle
Summary: In this study, we explore the sensitivity of several core-level spectroscopic methods to the atomistic structure using water molecule as a test system. We define a metric to measure the magnitude of spectral change as a function of structure, which enables us to identify structural regions with high spectral sensitivity. By employing machine-learning emulator-based decomposition of structural parameter space, we are able to recover more spectral variance and identify spectroscopically dominant degrees of freedom.
ROYAL SOCIETY OPEN SCIENCE
(2022)
Article
Chemistry, Physical
Yogesh Kumar, S. Tripathi, Mangla Nand, R. Jangir, V. Srihari, A. Das, R. Singh, U. Deshpande, S. N. Jha, A. Arya
Summary: This study investigated the effect of Nd doping on the structural, optical, and electronic properties of lanthanum monazite structure. Pure and Nd-doped LaPO4 powders were prepared and analyzed for their composition, oxidation states, crystal structure, and bandgaps. The results confirmed the successful substitution of Nd in the LaPO4 matrix and provided insights into the local structure using extended X-ray absorption fine structure analysis.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Biochemistry & Molecular Biology
Jean-Philippe Renault, Lucie Huart, Aleksandar R. Milosavljevic, John D. Bozek, Jerome Palaudoux, Jean-Michel Guigner, Laurent Marichal, Jocelyne Leroy, Frank Wien, Marie-Anne Herve Du Penhoat, Christophe Nicolas
Summary: X-ray photoelectron spectroscopy of BSA in a liquid jet provides insights into the electronic structure and charge transfer mechanisms in biological systems. The spectra show no structural damage to BSA and reveal carbon and nitrogen atoms in different chemical environments. Comparison between solid and solvated BSA shows higher sensitivity of valence bands to solvation effects. The ionization energy of solvated BSA is determined as 5.7 +/- 0.3 eV. Experimental results are compared with theoretical calculations, highlighting the role of water in hole delocalization in proteins.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Physical
Jade Barreto, Rubem Caetano, Maria I. Ramos, Astrid Ali, Guilherme Felix, Emilia Annese, Niklas Nilius, Hans -Joachim Freund, Braulio S. Archanjo, Carlos A. Achete, Paul S. Bagus, Fernando Stavale
Summary: Understanding the physical origin of core-level photoemission line shapes can provide valuable information about the chemical and physical properties of surfaces. This study investigates the interior, terrace, and edge-atom core-level binding energy shifts of MnO monolayers grown on an Au substrate, in order to distinguish the line shape contributions related to different types of atomic sites.
Article
Chemistry, Physical
Ritesh Verma, Ankush Chauhan, Khalid Mujasam Batoo, Muhammad Hadi, Emad H. Raslan, Rajesh Kumar, Muhammad Farzik Ijaz, Abdulaziz K. Assaifan
Summary: The synthesis of vanadium-doped BCZT ceramic oxides was reported in this paper, confirming the existence of a solubility limit of V in BCZT ceramics. Analysis revealed the influence of crystal structure and formation of oxygen vacancies on the luminescence and electrical properties of the material.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Multidisciplinary
Ziyi Chen, Andrew G. Walsh, Xiao Wei, Manzhou Zhu, Peng Zhang
Summary: This study investigates the electronic properties of Ag-25(SR)(18) and Au-25(SR)(18) and develops a unique method to analyze the charge transfer behavior of nanoclusters. Experimental X-ray spectroscopy is used to demonstrate the bonding properties of silver nanoclusters, with the staple motif shown to have a significant impact on their electronic properties. The effective X-ray analysis techniques developed here provide new opportunities for the site-specific study of other nanoclusters.
Article
Chemistry, Physical
Mauricio Lopez Luna, Janis Timoshenko, David Kordus, Clara Rettenmaier, See Wee Chee, Adam S. Hoffman, Simon R. Bare, Shamil Shaikhutdinov, Beatriz Roldan Cuenya
Summary: The study investigates the structural and chemical evolution of oxide-supported iron nanoparticles during the activation stages and the CO2 hydrogenation reaction, revealing the preferential formation of iron surface oxides under reaction conditions. The results highlight the important role played by the oxide support in the final structure and composition of nanosized catalysts.
Article
Multidisciplinary Sciences
Yang Ling, Tu Sun, Linshuo Guo, Xiaomeng Si, Yilan Jiang, Qing Zhang, Zhaoxi Chen, Osamu Terasaki, Yanhang Ma
Summary: This article reports the atomic-level ab initio structure determinations of microcrystals by combining 3D electron diffraction and environmental transmission electron microscope. The study reveals the stimuli-responsive structures of crystals under various environmental conditions.
NATURE COMMUNICATIONS
(2022)
Article
Physics, Multidisciplinary
T. P. H. Sidiropoulos, N. Di Palo, D. E. Rivas, S. Severino, M. Reduzzi, B. Nandy, B. Bauerhenne, S. Krylow, T. Vasileiadis, T. Danz, P. Elliott, S. Sharma, K. Dewhurst, C. Ropers, Y. Joly, K. M. E. Garcia, M. Wolf, R. Ernstorfer, J. Biegert
Summary: The detection of energy conversion pathways between photons, charge carriers, and the lattice is crucial for understanding fundamental physics and advancing materials and devices. Attosecond core-level x-ray absorption fine-structure spectroscopy (XANES) provides a clear and simultaneous view of the temporal evolution of the photon-carrier-phonon system, revealing surprising new results. By applying this method to graphite, complex mechanisms involving electrons, holes, and optical phonons were elucidated, showcasing the utility of core-level XANES with attosecond temporal resolution for studying energy flow inside materials.
Article
Chemistry, Physical
Tom Philipp, Gregor Neusser, Ebrahim Abouzari-Lotf, Shirin Shakouri, Franziska D. H. Wilke, Maximilian Fichtner, Mario Ruben, Manuel Mundszinger, Johannes Biskupek, Ute Kaiser, Philipp Scheitenberger, Mika Linden, Christine Kranz
Summary: In this study, FIB/SEM tomography combined with an optimized embedding procedure and osmium tetroxide staining was used to trace and visualize the self-conditioning step and degradation processes of CuDEPP composite electrodes. The results revealed the insertion of the electrolyte into the active material of the electrode and the formation of an interphase. Raman spectroscopy confirmed the degradation processes of the metalloporphyrin complex.
JOURNAL OF POWER SOURCES
(2022)
Article
Chemistry, Multidisciplinary
Laure Decamps, Derek B. Rice, Serena DeBeer
Summary: This study provides experimental evidence that the cofactor of the iron nitrogenase contains a carbide, making the Fe6C core a common feature among all nitrogenase cofactors.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Alberto Garcia-Fernandez, Sebastian Svanstrom, Cody M. Sterling, Abhijeet Gangan, Axel Erbing, Chinnathambi Kamal, Tamara Sloboda, Birgit Kammlander, Gabriel J. Man, Hakan Rensmo, Michael Odelius, Ute B. Cappel
Summary: This study investigates the surface properties and electronic structure of lead halide perovskite single crystals using synchrotron-based soft X-ray photoelectron spectroscopy, molecular dynamics simulations, and density functional theory. The results provide reference spectra for photoelectron spectroscopy investigations of polycrystalline thin films and can be used to optimize the design of device interfaces.
Article
Chemistry, Physical
Daniel Wolverson, Benjamin Smith, Enrico Da Como, Charles Sayers, Gary Wan, Luca Pasquali, Mattia Cattelan
Summary: A simple first-principles approach is used to estimate the core level shifts observed in X-ray photoelectron spectroscopy for the 4f electrons of Hf, Ta, W, and Re. The results show that this approach can provide insights into modifications of the commensurate charge density wave and the surface termination of MXenes.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Bing-Bing Zhang, Jing Ming, Hao-Qing Li, Xiu-Neng Song, Chuan-Kui Wang, Weijie Hua, Yong Ma
Summary: Heterogeneous atomic doping, especially with nitrogens, can enhance the interfacial properties and electrical conductivity of carbon-based materials like y-graphyne (y-GY), leading to improved energy storage capacity and expanded electrical applications. The local structures around the impurity atoms have a significant impact on the properties of doped structures, which can be sensitively determined by X-ray photoelectron (XPS) and near-edge X-ray absorption fine-structure (NEXAFS) spectra. In this study, the XPS and NEXAFS spectra of both pristine y-GY and five nitrogen-doped y-GYs at the C and N K-edges were successfully simulated using density functional theory.
Article
Biochemistry & Molecular Biology
Giovanni Canil, Juan Gurruchaga-Pereda, Simona Braccini, Lorella Marchetti, Tiziana Funaioli, Fabio Marchetti, Alessandro Pratesi, Luca Salassa, Chiara Gabbiani
Summary: Photoactivatable Pt(IV) prodrugs have great potential as metal-based drugs due to their chemical inertness in oxidized form and selective targeting compared to Pt(II) compounds. A new Pt(IV) complex, soluble in water and unreactive until reduction, was synthesized. The complex exhibited rapid and efficient photoreduction with visible light, facilitated by a catalytic system based on flavin and NADH. The reactivity of the prodrug against biological targets was only observed after photoreduction to its Pt(II) analogue.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Physical
Alexander A. . Guda, Mikhail V. Kirichkov, Viktor V. Shapovalov, Alexey I. Muravlev, Danil M. Pashkov, Sergey A. . Guda, Anton P. Bagliy, Sergey A. . Soldatov, Sergey V. Chapek, Alexander V. Soldatov
Summary: Gold nanoparticles are important functional nanomaterials with wide applications in optoelectronics, biomedical applications, and catalysis. This study focuses on the controllable synthesis of nanoparticles with specified size and shape. The researchers applied uniform sampling of the reaction parameter space and in situ UV-vis control to explore the relevant chemical questions related to nanoparticle formation, shape, and growth period.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Physics, Condensed Matter
Yu Rusalev, A. Motseyko, A. A. Guda, S. A. Guda, A. Soldatov, N. Ter-Oganessian
Summary: In this study, an ReaxFF potential for the Au-Pd system was constructed based on ab initio DFT calculations and validated using molecular dynamics and Monte-Carlo simulations. Several optimal parameterizations were obtained to describe the bulk properties, phase transition temperatures, and crystal structures of the system.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2023)
Article
Chemistry, Physical
Zdenek Sofer, Yunpeng Zuo, Nikolas Antonatos, Lukas Dekanovsky, Jan Luxa, Joshua D. Elliott, Diego Gianolio, Jir Saturala, Fabrizio Guzzetta, Stefanos Mourdikoudis, Jakub Regner, Roman Melek
Summary: Transition-metal tellurides have emerged as attractive catalysts for hydrogen evolution reaction, but their intrinsic activity hinders practical applications. This study successfully fabricated PdTe2-based catalysts with different types of vacancies, demonstrating remarkable HER activity. The defect engineering strategy used in this work can be extended to other two-dimensional materials, expanding their potential application fields.
Article
Chemistry, Inorganic & Nuclear
Juan Sanchez-Camacho, Sonia Infante-Tadeo, Ana C. Carrasco, Stefano Scoditti, A'lvaro Martinez, Fabienne Barroso-Bujans, Emilia Sicilia, Ana M. Pizarro, Luca Salassa
Summary: In this study, two new asymmetric Pt(IV) derivatives were designed and synthesized, which could be effectively activated into toxic Pt(II) species by incubation with nicotinamide adenine dinucleotide, sodium ascorbate, and glutathione in the dark and under light irradiation. One of the derivatives displayed enhanced toxicity in MDA-MB-231 breast cancer cells preincubated with ascorbate, suggesting selective triggering of oxaliplatin generation through redox activation. Covalent binding of the flavin to the Pt complex was shown to be pivotal for this effect.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jonathan Ruiz Esquius, David J. Morgan, Gerardo Algara Siller, Diego Gianolio, Matteo Aramini, Leopold Lahn, Olga Kasian, Simon A. Kondrat, Robert Schloegl, Graham J. Hutchings, Rosa Arrigo, Simon J. Freakley
Summary: The oxygen evolution reaction (OER) is crucial for future energy systems based on water electrolysis. Iridium oxides show promise as catalysts due to their corrosion resistance in acidic and oxidizing conditions. The transformation of highly active iridium (oxy)-hydroxides prepared using alkali metal bases into rutile IrO2 at high temperatures (>350 degrees C) results in poor activity, but the transformation into Li-intercalated IrOx retains comparative activity and improved stability. This nanocrystalline lithium iridate form could be more resistant to industrial procedures and help stabilize the high populations of redox active sites in amorphous iridium (oxy)hydroxides.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Dmitry Galyamin, Jorge Torrero, Isabel Rodriguez, Manuel J. Kolb, Pilar Ferrer, Laura Pascual, Mohamed Abdel Salam, Diego Gianolio, Veronica Celorrio, Mohamed Mokhtar, Daniel Garcia Sanchez, Aldo Saul Gago, Kaspar Andreas Friedrich, Miguel A. Pena, Jose Antonio Alonso, Federico Calle-Vallejo, Maria Retuerto, Sergio Rojas
Summary: The study finds that low-ruthenium-content pyrochlores (R2MnRuO7, R = Y, Tb, and Dy) exhibit high activity and durability for the oxygen evolution reaction (OER) in acidic media. Among them, Y2MnRuO7 is the most stable catalyst, showing a voltage of 1.5 V at 10 mA cm(-2) for 40 h, or 5000 cycles up to 1.7 V. Experimental and computational results indicate that the excellent performance is attributed to the Ru sites embedded in RuMnOx surface layers. A water electrolyzer with Y2MnRuO7 and only 0.2 mgRu cm(-2) achieves a current density of 1 A cm(-2) at 1.75 V, remaining stable at 200 mA cm(-2) for over 24 h. These findings suggest further investigation on Ru catalysts with the goal of enhancing OER performance through a partial replacement of Ru with inexpensive cations. Ru-pyrochlores can serve as alternative anodes of PEM water electrolyzers, and their high performance is attributed to the Ru sites embedded in RuMnOx surface layers. The durability of a water electrolyzer with Y2MnRuO7 and only 0.2 mgRu cm(-2) has been successfully demonstrated.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Diego Gianolio, Michael D. Higham, Matthew G. Quesne, Matteo Aramini, Ruoyu Xu, Alex I. Large, Georg Held, Juan-Jesus Velasco-Velez, Michael Haevecker, Axel Knop-Gericke, Chiara Genovese, Claudio Ampelli, Manfred Erwin Schuster, Siglinda Perathoner, Gabriele Centi, C. Richard A. Catlow, Rosa Arrigo
Summary: Operando soft and hard X-ray spectroscopic techniques were used to investigate Zn-containing Cu nanostructured electrocatalysts in CO2 hydrogenation reaction. The study reveals that Zn is alloyed with Cu in the bulk of the nanoparticles, while low reducible Cu(I)-O species are consumed at the interface. The Cu-Zn system represents the optimal active ensembles with stabilized Cu(I)-O, which activates CO2 and supplies H atoms for the hydrogenation reaction.
Article
Computer Science, Interdisciplinary Applications
A. S. Algasov, S. A. Guda, V. I. Kolesnikov, V. V. Ilicheva, A. V. Soldatov
Summary: The rational choice of sampling points is crucial for supervised machine learning algorithms. Adaptive sampling ensures optimal distribution of points in the multidimensional space and provides higher approximation accuracy with respect to the random sampling. We introduce a fast adaptive sampling algorithm with accuracy comparable to that of the best-known adaptive sampling methods and demonstrate a comparative study of different approaches to minimization of approximation errors.
JOURNAL OF COMPUTATIONAL SCIENCE
(2023)
Article
Chemistry, Physical
Elizaveta G. Kozyr, Peter N. Njoroge, Sergei V. Chapek, Viktor V. Shapovalov, Alina A. Skorynina, Anna Yu. Pnevskaya, Alexey N. Bulgakov, Alexander V. Soldatov, Francesco Pellegrino, Elena Groppo, Silvia Bordiga, Lorenzo Mino, Aram L. Bugaev
Summary: Photocatalytic hydrogen production is a promising alternative energy route. In this study, operando spectroscopy was used to understand the structure-activity relationships of a catalytic system during the photodeposition of Pt on TiO2 and photostimulated H-2 production. XAS showed an increase in Pt fluorescence correlated with H-2 production, and the final Pt/TiO2 catalyst contained Pt(0) particles. UV-Vis spectroscopy revealed the disappearance of electronic features corresponding to Pt4+ species in the presence of formic acid, resulting in the presence of Pt(0) particles.
Article
Crystallography
Margarita A. A. Marchenkova, Sergei V. V. Chapek, Petr V. V. Konarev, Ksenia B. B. Ilina, Georgy S. S. Peters, Yury V. V. Pisarevsky, Vladimir A. A. Shishkov, Alexander V. V. Soldatov, Mikhail V. V. Kovalchuk
Summary: A multichannel microfluidic cell(MFC)obtained using 3D printing was used to study the structure of complex solutions by small-angle X-ray scattering(SAXS)at the BioMUR beamline of the Kurchatov synchrotron. A comparative analysis of SAXS signal showed that MFC has significant advantages over the standard capillary. The dynamics of SAXS scattering curves for lysozyme solutions were investigated, and the obtained data were consistent with known data.
Article
Chemistry, Applied
M. Giordano, G. Volpi, C. Garino, F. Cardano, C. Barolo, G. Viscardi, A. Fin
Summary: A series of new emissive imidazo[5,1-a]isoquinolines were synthesized, and their electronic properties were investigated. The electronic spectra showed absorption bands around 330-350 nm and intense fluorescence emissions between 440 nm and 460 nm. The emission quantum yield in dichloromethane solution was enhanced from 9% to 37% depending on the position and electronic properties of the substituents on the imidazo[5,1-a]isoquinoline nucleus. The data suggest that steric hindering and electronic effects are responsible for the enhanced emission.
Article
Chemistry, Physical
Peng Tang, Po-Yuan Huang, Jack E. N. Swallow, Chenbo Wang, Diego Gianolio, Hua Guo, Jamie H. Warner, Robert S. Weatherup, Mauro Pasta
Summary: The synthesis and catalytic performance of trapped platinum single atoms in carbon substrates are studied. It is found that platinum single atoms can be synthesized by adsorbing H2PtCl6 on the polyaniline substrate and undergoing pyrolysis. In situ heated scanning transmission electron microscopy and temperature-dependent X-ray photoelectron spectroscopy reveal the thermal evolution of platinum during pyrolysis. The results show that nitrogen atoms in polyaniline can coordinate with platinum ions and capture platinum sites at pyridinic nitrogen defects formed during substrate graphitization. Operando X-ray absorption spectroscopy confirms the stability of the trapped platinum single atoms at the working potentials of the hydrogen evolution reaction but with lower electrocatalytic activity compared to metallic platinum nanoparticles. First principle calculations suggest that the lower activity of trapped platinum single atoms is due to their unfavorable hydrogen chemisorption energy relative to metallic platinum (111) surfaces. These results deepen the understanding of the structure-property relationship in trapped platinum single atoms and also motivate a detailed techno-economic analysis to evaluate their commercial applicability.
Article
Chemistry, Physical
Margherita Cavallo, Cesare Atzori, Matteo Signorile, Ferdinando Costantino, Diletta Morelli Venturi, Athanasios Koutsianos, Kirill A. Lomachenko, Lucia Calucci, Francesca Martini, Andrea Giovanelli, Marco Geppi, Valentina Crocella, Marco Taddei
Summary: F4_MIL-140A(Ce), a recently discovered phase-change metal-organic framework (MOF) adsorbent, exhibits a non-hysteretic step-shaped CO2 adsorption isotherm and exceptional CO2/N-2 selectivity and reverse CO2/C2H2 selectivity. Through a combination of various characterization techniques and periodic density functional theory simulations, evidence is provided for the existence of a unique cooperative CO2 adsorption mechanism in F4_MIL-140A(Ce), involving the concerted rotation of perfluorinated aromatic rings.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Sintu Ganai, Puspal Mukherjee, Kalachand Mahali, Avishek Saha, Aslam Hossain, A. V. Soldatov, A. M. A. Henaish, Jahangeer Ahmed, Sanjay Roy
Summary: In this study, we investigated the solubility of coumarin in different solvent systems. Experimental measurements using UV-Vis spectroscopy were carried out at various temperatures. Water-DMF mixture showed the highest solubility, while water-ACN system exhibited the lowest solubility. Theoretical studies were employed to optimize the molecular structure of coumarin and provide insights into the thermodynamic stability of the compound in solution.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Physical
Sergey Yu. Ketkov, Sheng-Yuan Tzeng, Elena A. Rychagova, Anton N. Lukoyanov, Wen-Bih Tzeng
Summary: Metallocenes, including methylcobaltocene, play important roles in various fields of chemistry. The ionization energy and vibrational structure of (Cp ')(Cp)Co can be influenced by introducing methyl substituents. The mass-analyzed threshold ionization spectrum and DFT calculations provide accurate information about the properties and transformations of (Cp ')(Cp)Co.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Review
Chemistry, Physical
Qifeng Mu, Jian Hu
Summary: Polymer mechanochemistry has experienced a renaissance due to the rapid development of mechanophores and principles governing mechanochemical transduction or material strengthening. It has not only provided fundamental guidelines for converting mechanical energy into chemical output, but also found applications in engineering and smart devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Da Hye Yang, Francesco Ricci, Fredrik L. Nordstrom, Na Li
Summary: Through systematic evaluation of the oiling-out behavior of procaine, we identified both stable and metastable liquid-liquid phase separation, and established phase diagrams to assist in rational selection of crystallization strategies.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Vikki Anand Varma, Simmie Jaglan, Mohd Yasir Khan, Sujin B. Babu
Summary: Designing engineering structures like nanocages, shells, and containers through self-assembly of colloids is a challenging problem. This work proposes a simple model for the subunit, which leads to the formation of monodispersed spherical cages or containers. The model with only one control parameter can be used to design cages with the desired radius.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Hainan Jiang, Yaolong He, Xiaolin Li, Zhiyao Jin, Huijie Yu, Dawei Li
Summary: The cycling lifespan and coulombic efficiency of lithium-ion batteries are crucial for high C-rate applications. The Li-ion concentration plays a crucial role in determining the mechanical integrity and structural stability of electrodes. This study focuses on graphite as the working electrode and establishes an experimental system to investigate the mechanical properties of composite graphite electrode at different C-rates. Considering the effect of Li-ion concentration in stress analysis is found to be significant.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Zhiye Wang, Yunchuan Li, Mingjun Sun
Summary: This study investigates the influence of intramolecular pi-pi interactions on the electronic transport capabilities of molecules. By designing and analyzing three pi-conjugated molecules, the researchers observe that different pi-conjugated structures have varying effects on electron transport. The findings provide a theoretical foundation for designing single-molecule electronic devices with multiple electron channels based on intramolecular pi-pi interactions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Yuandong Xu, Haoyang Feng, Chaoyang Dong, Yuqing Yang, Meng Zhou, Yajun Wei, Hui Guo, Yaqing Wei, Jishan Su, Yingying Ben, Xia Zhang
Summary: Hollow MoS2 cubes and spheres were successfully synthesized using a one-step hydrothermal method with the hard template method. The hollow MoS2 cubes exhibited higher specific capacitance and energy density compared to the hollow MoS2 spheres. The symmetrical supercapacitors assembled with these hollow structures showed good performance and high capacity retention after multiple cycles. These findings suggest that controlling the pore structure and surface characteristics of MoS2 is crucial for enhancing its electrochemical properties.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Ainhoa Oliden-Sanchez, Rebeca Sola-Llano, Joaquin Perez-Pariente, Luis Gomez-Hortiguela, Virginia Martinez-Martinez
Summary: The combination of photoactive molecules and inorganic structures is important for the development of advanced materials in optics. In this study, bulky dyes were successfully encapsulated in a zeolitic framework, resulting in emission throughout the visible spectrum.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Miaomiao Zhang, Cunyuan Pei, Qiqi Xiang, Lintao Liu, Zhongxu Dai, Huijuan Ma, Shibing Ni
Summary: The design of a solid electrolyte interphase (SEI) plays a crucial role in improving the electrochemical performance of anode materials. In this study, lithium difluoro(oxalate)borate (LiDFOB) is used as an electrolyte additive to form a protective SEI film on Li3VO4 (LVO) anodes. The addition of LiDFOB results in a dense, uniform, stable, and LiF-richer SEI, which enhances the Li-ion storage kinetics. The generated SEI also prevents further decomposition of the electrolyte and maintains the morphology of LVO anodes during charge/discharge processes. This work demonstrates the effectiveness of LiDFOB as a multi-functional additive for LiPF6 electrolytes and provides insights into SEI construction for high-performance LVO anodes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
B. V. Andryushechkin, T. V. Pavlova, V. M. Shevlyuga
Summary: The atomic structure of the Ag(111)-p(4 x 4)-O phase was reexamined and two phases with the same periodicity were discovered. It was demonstrated that the accepted Ag6 model is incompatible with high-resolution oxygen-sensitive STM images.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
S. L. Romo-Avila, D. Marquez-Ruiz, R. A. Guirado-Lopez
Summary: In this study, we used density functional theory (DFT) calculations to investigate the interaction between model graphene oxide (GO) nanostructures and chlorine monoxide ClO. We aimed to understand the role of this highly oxidizing species in breaking C-C bonds and forming significant holes on GO sheets. Our results showed that C-C bonds in a single graphene oxide sheet can be broken through a simple mechanism involving the dissociation of two chemically attached ClO molecules. The formation of carbonyl groups and holes on the GO surface was also observed. This study provides important insights into the degradation of carbon nanotubes and the stability of GO during the myeloperoxidase (MPO) catalytic cycle.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Alberto Garcia-Fernandez, Birgit Kammlander, Stefania Riva, Hakan Rensmo, Ute B. Cappel
Summary: In this study, the X-ray stability of five different lead halide perovskite compositions (MAPbI3, MAPbCl3, MAPbBr3, FAPbBr3, CsPbBr3) was investigated using photoelectron spectroscopy. Different degradation mechanisms and resistance to X-ray were observed depending on the crystal composition. Overall, perovskite compositions based on the MA+ cation were found to be less stable than those based on FA+ or Cs+. Metallic lead formation was most easily observed in the chloride perovskite, followed by bromide, and very little in MAPbI3. Multiple degradation processes were identified for the bromide compositions, including ion migration, formation of volatile and solid products, as well as metallic lead. CsBr was formed as a solid degradation product on the surface of CsPbBr3.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Timofei Rostilov, Vadim Ziborov, Alexander Dolgoborodov, Mikhail Kuskov
Summary: The shock-loading behavior of nanomaterials is investigated in this study. It is found that shock compaction waves exhibit a distinct two-step structure, with the formation of faster precursor waves that travel ahead of the main compaction waves. The complexity of the shock Hugoniot curve of the tested nanomaterial is described, and the effect of initial porosity on the compressed states is demonstrated.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Alexey A. Markov, Mikhail V. Patrakeev
Summary: The stability of La1/3Sr2/3Fe1-xMnxO3-delta, a perovskite-type oxide, under reducing conditions is dependent on the manganese content. Increasing the manganese content leads to a decrease in stability. The behavior of iron and manganese in the oxide shows distinct differences, which can be attributed to the difference in the enthalpy of oxidation reactions. Additionally, the change in the La/Sr ratio affects the concentration of iron and manganese ions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Mosayeb Naseri, Shirin Amirian, Mehrdad Faraji, Mohammad Abdur Rashid, Maicon Pierre Lourenco, Venkataraman Thangadurai, D. R. Salahub
Summary: Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3, this study assessed the structural stability and investigated the electronic, optical, and thermoelectric properties of a group of two-dimensional perovskite-type materials called perovskenes. The findings revealed that these materials are wide bandgap semiconductors with potential application in UV shielding. Moreover, they exhibit better electrical and thermal conductivity at high temperatures, enabling efficient power generation in thermoelectric devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)