Article
Chemistry, Medicinal
Bharath Raghavan, Florian K. Schackert, Andrea Levy, Sophia K. Johnson, Emiliano Ippoliti, Davide Mandelli, Jogvan Magnus Haugaard Olsen, Ursula Rothlisberger, Paolo Carloni
Summary: MiMiC is a flexible and scalable multiscale modeling framework that combines quantum mechanics (QM) and molecular mechanics (MM) codes. The paragraph introduces MiMiCPy, a user-friendly tool written in Python 3 that automates the preparation of MiMiC input files. It also highlights the modular structure of MiMiCPy, allowing for easy extensions to new program formats.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Article
Biochemistry & Molecular Biology
Sijin Chen, Xiaoyan Ding, Chao Sun, Anthony Watts, Xiao He, Xin Zhao
Summary: The study investigated the dynamic coupling of Y185 with the bR photocycle through calculations and simulations, revealing its significant role in regulating thermal equilibrium, stabilizing H-bond networks, participating in orientation switch, and opening the channel gate. These findings provide a detailed molecular mechanism of the dynamic couplings of Y185 and the bR photocycle from a structural perspective, with potential applications to other microbial photoreceptors.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2021)
Article
Chemistry, Physical
Marvin Asido, Rajiv K. Kar, Clara Nassrin Kriebel, Markus Braun, Clemens Glaubitz, Igor Schapiro, Josef Wachtveitl
Summary: A transient near-UV absorption signature was identified in Krokinobacter eikastus rhodopsin 2 (KR2) which could serve as a marker for retinal configuration. Hybrid quantum mechanics/molecular mechanics simulations revealed that this signature corresponds to S-0 -> S-3 and/or S-0 -> S-5 transitions, and these transitions show negligible spectral shift with changes in the protein environment. The study also explored potential optogenetic applications through near-UV quenching experiments, demonstrating ultrafast regeneration of the parent state of KR2.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Qiang Cui, Tanmoy Pal, Luke Xie
Summary: This article discusses the challenges and issues in QM/MM simulations, emphasizing the importance of these issues for applications in biomolecular systems. Despite its limited scope, the hope is to stimulate further developments in the field of QM/MM simulation methods.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Biochemistry & Molecular Biology
Phujinn Honorio, Supawadee Sainimnuan, Supa Hannongbua, Patchreenart Saparpakorn
Summary: The research discovered that protoberberine alkaloids isolated from natural resources are potent inhibitors of acetylcholinesterase (AChE) and have the potential to reduce symptoms of Alzheimer's disease. The key interactions of palmatine and berberine with AChE were identified as 7C-7C interactions with specific amino acids and H-bond interactions. In contrast, cyclanoline showed a different binding mode and preference for a deeper site within AChE.
CHEMICO-BIOLOGICAL INTERACTIONS
(2021)
Article
Biochemistry & Molecular Biology
Francisco Andres Peralta, J. Pablo Huidobro-Toro, Raul Mera-Adasme
Summary: QM/MM molecular dynamic simulations were used to study the allosteric modulator role of Zn(II) on P2X4R, revealing insights into the nature of Zn(II) modulation and the effects of mutations, potentially explaining elusive modulation mechanisms in other extracellular or membrane proteins.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2021)
Article
Multidisciplinary Sciences
Jingcheng Guan, You Lu, Kakali Sen, Jamal Abdul Nasir, Alec W. W. Desmoutier, Qing Hou, Xingfan Zhang, Andrew J. J. Logsdail, Gargi Dutta, Andrew M. M. Beale, Richard W. W. Strange, Chin Yong, Paul Sherwood, Hans M. M. Senn, C. Richard A. Catlow, Thomas W. W. Keal, Alexey A. A. Sokol
Summary: Vibrational spectroscopy is crucial for characterizing chemical systems, and recent theoretical developments in the ChemShell computational chemistry environment are reported to aid the interpretation of experimental infrared and Raman spectra. Computational vibrational intensities were calculated using a hybrid quantum mechanical and molecular mechanical approach, providing more realistic vibrational signatures for various materials and molecular systems. The efficient task-farming parallelism implemented in ChemShell on high-performance computing platforms enabled this work. This article is part of a discussion meeting issue on supercomputing simulations of advanced materials.
PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES
(2023)
Article
Biophysics
Peter Eberhardt, Chavdar Slavov, Janina Soermann, Christian Bamann, Markus Braun, Josef Wachtveitl
Summary: The study on the light-driven Na+ pump Krokinobacter rhodopsin 2 (KR2) revealed that with increasing temperature, the overall photocycle duration is accelerated, with the L-to-M transition exhibiting the most significant increase. This kinetic decoupling between the chromophore and the protein scaffold in KR2 could be utilized for fine-tuning biotechnological applications in the future.
BIOPHYSICAL JOURNAL
(2021)
Article
Chemistry, Physical
Yuzhuang Fu, Binju Wang, Zexing Cao
Summary: Detailed mechanisms for the chemical steps involved in the biodegradation of 2-oxoadipate (2OA) by HglS enzyme have been explored using MD simulations and QM/MM calculations. The study reveals the presence of two coordination modes of the Fe(IV)-oxo species, with the proximal mode responsible for C-H bond activation. Additionally, residues in the second coordination sphere play a crucial role in substrate binding and facilitate the ferryl-flip, leading to the proximal Fe(IV)-oxo conformation ideal for C-H bond activation.
JOURNAL OF CATALYSIS
(2023)
Article
Multidisciplinary Sciences
Zhaoxi Sun, Zhirong Liu
Summary: The study explores indirect free energy simulation methods at quantum mechanics and molecular mechanics levels, as well as attempts to optimize multi-scale treatment by changing the region for electronic structure calculations. The numerical tests show that the estimates from the indirect nonequilibrium perturbation framework are almost identical to the direct results, while the indirect equilibrium estimates deviate from the direct references.
ADVANCED THEORY AND SIMULATIONS
(2021)
Article
Chemistry, Multidisciplinary
Ankita Tripathi, Kshatresh Dutta Dubey
Summary: This study demonstrates a method to enhance promiscuity, called allostery-driven promiscuity, using molecular dynamics simulations and hybrid QM/MM calculations. By studying the AEE enzyme, the authors show that a single site mutation can induce conformational changes in the capping loop, allowing recognition of different substrates for different functions.
CHEMISTRY-AN ASIAN JOURNAL
(2022)
Article
Biochemistry & Molecular Biology
Bella Grigorenko, Tatiana Domratcheva, Alexander Nemukhin
Summary: The oxygenase activity of the flavin-dependent enzyme RutA is associated with the formation of flavin-oxygen adducts in the enzyme active site. Using quantum mechanics/molecular mechanics (QM/MM) modeling, we investigated potential reaction pathways initiated by triplet state complexes of molecular oxygen with reduced flavin mononucleotide (FMN) in protein cavities. The results show that these complexes can be located at different positions on the isoalloxazine ring of flavin, and the activated dioxygen attacks specific positions in the ring, resulting in covalent adducts or direct oxidation of flavin.
Article
Chemistry, Multidisciplinary
Vishal Kumar Porwal, Antoine Carof, Francesca Ingrosso
Summary: The presence of carboxyl groups in a molecule affects its affinity to metal cations and sensitivity to the chemical environment, mainly due to intermolecular hydrogen bonds. Carboxylate groups can also induce intramolecular interactions, impacting the conformational space of biomolecules. To accurately describe these modifications, a compromise between quantum chemical description and explicit solvent molecules is required. This study presents a bottom-up approach combining continuum solvent, microsolvation approach, and QM/MM molecular dynamics simulations to analyze the conformational space and solvation properties of carboxylated (bio)organic anions, providing a detailed description of the solvation shell and intermolecular hydrogen bonds.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Yuzhuang Fu, Fangfang Fan, Binju Wang, Zexing Cao
Summary: Enzymatic degradation of pesticides paraoxon (PON) and parathion (PIN) by phosphotriesterase (PTE) has been studied using QM/MM calculations and MD simulations. The results reveal that the hydrolysis reactions are driven by nucleophilic attack and the rate-limiting step is the two-step hydrolytic process.
CHEMISTRY-AN ASIAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Keisei Shibata, Kazumasa Oda, Tomohiro Nishizawa, Yuji Hazama, Ryohei Ono, Shunki Takaramoto, Reza Bagherzadeh, Hiromu Yaw, Osamu Nureki, Keiichi Inoue, Hudefumim Akiyama
Summary: Channelrhodopsins (ChRs) are light-gated ion channels that can control neuronal activity with high temporal resolution. The mechanism of how their channels open and close is still unknown. This study investigated the structural changes in the retinal chromophore of ChR C1C2 and the factors that limit the kinetics of the channel gating. The results showed that the retinal chromophore twists upon RSB deprotonation, causing the surrounding helices to move and open the channel, and the RSB reprotonation rate-limits the channel closing.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Claudia L. Gomez-Flores, Denis Maag, Mayukh Kansari, Van-Quan Vuong, Stephan Irle, Frauke Graeter, Tomas Kubar, Marcus Elstner
Summary: This paper investigates the generation of free energy surfaces in complex reactions using the semiempirical method DFTB and improves its accuracy by developing a specific reaction parametrization (SRP). Through the implementation of an artificial neural network (ANN), the authors successfully generate highly accurate free energy surfaces for thiol-disulfide exchange in two molecular complexes.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Sara Roosta, Farhad Ghalami, Marcus Elstner, Weiwei Xie
Summary: The present study systematically examines the performance of two approximations in the simulations of charge transport in organic semiconductors. The results show that the proposed methods can achieve consistent results with standard simulations at reduced computational cost. The study also highlights the importance of the reorganization energy in determining the charge carrier mobility and its sensitivity to the choice of DFT functionals.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Samaneh Inanlou, Rodrigo Cortes-Mejia, Ali Deniz Oezdemir, Sebastian Hoefener, Wim Klopper, Wolfgang Wenzel, Weiwei Xie, Marcus Elstner
Summary: In this study, the absorption spectra of CBP in gas and condensed phases were simulated using the TD-LC-DFTB method. The accuracy of the computed spectra was verified by comparing with experimental results. Static and dynamic disorders play a crucial role in accurately calculating absorption spectra, and a reasonable structural model is important for representing these disorders.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Ziwei Pang, Monja Sokolov, Tomas Kubar, Marcus Elstner
Summary: In this study, molecular dynamics simulations were used to investigate the mechanism of glucose binding in GGBP mutant and wild-type proteins. The simulations provided insights into changes in the hydrogen-bonding network and chromophore conformations upon glucose binding, which can help optimize the design of glucose sensors.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Correction
Chemistry, Physical
B. Hourahine, B. Aradi, V. Blum, F. Bonafe, A. Buccheri, C. Camacho, C. Cevallos, M. Y. Deshaye, T. Dumitrica, A. Dominguez, S. Ehlert, M. Elstner, T. van der Heide, J. Hermann, S. Irle, J. Jakowski, J. J. Kranz, C. Koehler, T. Kowalczyk, T. Kubar, I. S. Lee, V. Lutsker, R. J. Maurer, S. K. Min, I. Mitchell, C. Negre, T. A. Niehaus, A. M. N. Niklasson, A. J. Page, A. Pecchia, G. Penazzi, M. P. Persson, J. Rezac, C. G. Sanchez, M. Sternberg, M. Stohr, F. Stuckenberg, A. Tkatchenko, V. W. -Z. Yu, T. Frauenheim
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Julian Boeser, Tomas Kubar, Marcus Elstner, Denis Maag
Summary: This study investigates the mechanism of glutaredoxin catalyzed oxidation and reduction of protein disulfide bonds through both experimental and computational approaches. Molecular dynamics simulations and hybrid quantum mechanical/molecular mechanical metadynamics simulations were used to obtain the free energy profiles of the reactions. The results confirm the proposed pathway and provide insights into the regiospecificity of the reactions.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Lisa Ross, Julius Reitemeier, Farhad Ghalami, Wen-Shan Zhang, Jurgen H. Gross, Frank Rominger, Sven M. Elbert, Rasmus Schroeder, Marcus Elstner, Michael Mastalerz
Summary: In this study, the solution and solid-state behavior of two-dimensionally triptycene end-capped QPPs were investigated. QPPs were synthesized through condensation reactions with pyrene-based tetraketone and ortho-diamines, resulting in the formation of dimers in solution, supported by MALDI-TIMS-TOF-MS analysis. Single-crystal X-ray analysis showed a short p-p distance of 3.3-3.4 angstrom and a perfect shape match during the dimerization of triptycene end-capped QPPs, indicating its potential as a synthon for crystal engineering.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Review
Biophysics
T. Kubar, M. Elstner, Q. Cui
Summary: Hybrid quantum mechanical/molecular mechanical (QM/MM) methods are essential for studying biomolecules. This article reviews the methodology of QM/MM approaches and their application to energy transduction in biomolecular machines. The importance of balancing efficiency and accuracy is emphasized, and examples showcase the value and limitations of QM/MM methodologies. Suggestions for further development in making QM/MM analyses more quantitative and applicable to complex biological problems are discussed.
ANNUAL REVIEW OF BIOPHYSICS
(2023)
Article
Chemistry, Physical
Denis Maag, Josua Boeser, Henryk A. Witek, Ben Hourahine, Marcus Elstner, Tomas Kubar
Summary: Coupled-perturbed equations for degenerate orbitals were implemented to study proton-coupled electron transfer reactions. The method was tested for both QM and QM/MM setups and showed stable enhanced sampling simulations. The obtained potentials of the mean force successfully described the thermodynamic and kinetic features of the reactions, making it a promising tool for investigating more complex systems like proteins.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Philipp M. Dohmen, Mila Kramer, Patrick Reiser, Pascal Friederich, Marcus Elstner, Weiwei Xie
Summary: In this study, the surface hopping method is used to simulate charge transport in organic semiconductors. Nonadiabatic molecular dynamics simulations are performed to study hole transport in anthracene and pentacene. Neural network based Hamiltonians are employed in two different nuclear relaxation schemes, and their performance in reproducing hole mobilities and inverse participation ratios is evaluated. The results show that the neural network models are able to accurately reproduce the desired properties with significantly reduced computational cost compared to traditional methods.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Ali Deniz Ozdemir, Samaneh Inanlou, Franz Symalla, Weiwei Xie, Wolfgang Wenzel, Marcus Elstner
Summary: This paper investigates the impact of structural disorder in amorphous organic semiconductors (OSCs) on the transfer parameters and charge mobilities. A sampling strategy for incorporating static and dynamic structural disorder is developed using QM/MM methods and extensive MD sampling. The results show that dynamic disorder causes an order of magnitude difference in the calculated mobility between morphologies of the same material. The method allows for the sampling of disorder in HOMO energies and couplings, and the statistical analysis characterizes the relevant time scales for charge transfer in these complex materials.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Hematology
Fabian Kutzki, Diego Butera, Angelina J. Lay, Denis Maag, Joyce Chiu, Heng-Giap Woon, Tomas Kubar, Marcus Elstner, Camilo Aponte-Santamaria, Philip J. Hogg, Frauke Graeter
Summary: This study revealed the oxidation state of disulfide bridges in the VWF-C4 domain and its implications for VWF's platelet binding function. It was found that two major force-bearing disulfide bonds are partially reduced in human blood, leading to conformational changes within C4 that affect the accessibility of the integrin-binding motif and impair integrin-mediated platelet binding. Additionally, specific thiol/disulfide exchanges between the reduced species and the remaining disulfide bridges were observed, with mechanical force potentially enhancing the proximity of reactant cysteines and further affecting integrin binding propensity.
JOURNAL OF THROMBOSIS AND HAEMOSTASIS
(2023)
Article
Materials Science, Multidisciplinary
Niklas J. Herrmann, Nadine von Coelln, Robin M. Teichgreber, Sebastian Hoefener, Christian Huck, Farhad Ghalami, Simon Settele, Manuel Hertzog, Marcus Elstner, Petra Tegeder, Eva M. Herzig, Jana Zaumseil
Summary: In this study, meniscus-guided zone-casting was used to selectively deposit two different polymorphs of PDIF-CN2 from solution. The two polymorphs can be distinguished by their characteristic low-wavenumber Raman modes and distinctive photoluminescence spectra, reflecting different intermolecular coupling. Despite having different crystalline structures, field-effect transistors based on thin films of both polymorphs show similar electron mobilities.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Optics
Kaito Wada, Rudy Raymond, Yu-ya Ohnishi, Eriko Kaminishi, Michihiko Sugawara, Naoki Yamamoto, Hiroshi C. Watanabe
Summary: This paper proposes a method to optimize arbitrary single-qubit gates in parametrized quantum circuits for simulating real- and imaginary-time evolution. The method fully utilizes the degrees of freedom of single-qubit gates and optimizes both the axis and angle simultaneously. Numerical experiments show its effectiveness in finding ground states and real-time evolution.
Article
Chemistry, Physical
Hiroshi C. Watanabe, Masayuki Yamada, Yohichi Suzuki
Summary: The QM/MM method is a hybrid molecular simulation technique that increases the accessibility of local electronic structures of large systems. However, applying this method to solution systems, particularly for proton transfer dynamics, is challenging. This paper proposes a new numerical expression and control algorithm that can stably and accurately simulate proton transfer dynamics in bulk water.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
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)