Article
Chemistry, Multidisciplinary
Noura Rahbani, Piotr de Silva, Emmanuel Baudrin
Summary: Transition metal complexes are potential redox mediators for redox flow batteries due to their adjustable electrochemical potentials. However, there is a need for reliable and efficient tools to predict their reduction potentials. This study establishes a suitable density functional theory protocol for prediction by using experimental data of aqueous iron complexes with bidentate ligands, and cross-validates it with different complexes in the redox-flow literature. The accuracy of prediction is found to be more influenced by the solvation model than the functional or basis set. The smallest errors are obtained using the COSMO-RS solvation model (mean average error (MAE)=0.24 V), while a general deviation from experimental results is observed with implicit solvation models. For a set of similar ligands, linear regression can be used for correction (MAE=0.051 V for the initial set of iron complexes).
Article
Chemistry, Multidisciplinary
Amilcar Duque-Prata, Tiago B. Pinto, Carlos Serpa, Pedro J. S. B. Caridade
Summary: The performance of different functionals and basis sets in calculating the redox potentials of small organic compounds in acetonitrile has been evaluated. It was found that the redox potentials should be analyzed separately rather than jointly. The M06-2X functional showed a more consistent and uniform response in both reductions and oxidations.
Article
Chemistry, Physical
Melany Isabel Garcia Nicholson, Paulo Roberto Bueno, Gustavo Troiano Feliciano
Summary: Hybrid computational methods were used to successfully predict homogeneous electron exchange between ferrocene and its oxidized state, showing a deviation of no more than 15% compared to experimental values. Reorganization energy was found to have a subtle yet significant dependence on the nature and localization of the compensating countercharge.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Physical
Donghyeon Kang, Hyeon Yeong Lee, Joon-Ha Hwang, Sera Jeon, Dabin Kim, SeongMin Kim, Sang-Woo Kim
Summary: This study investigated the impact of molecular structure deformation on the triboelectric properties of PTFE induced by contact force using density functional theory (DFT). The results showed that deformation enhanced the negative triboelectric property of PTFE mainly due to the electron-deficient state of carbon atoms leading to enhanced local dipole.
Article
Engineering, Environmental
Fansong Liu, Qiujing Xu, Huizhi Liang, Haiying Wang, Cheng Zhong, Xiaobo Min, Liyuan Zhang
Summary: Stabilization of arsenic sulfur slag is crucial to prevent environmental pollution, but the molecular understanding of its stability is lacking, hindering the development of effective solutions. By studying the structure-stability relationship of As-S slag, the most stable structure was identified and a successful excess-S-based hydrothermal method was proposed to promote stabilization. This method significantly reduced the arsenic concentration in the leaching test, demonstrating its effectiveness compared to other methods.
JOURNAL OF HAZARDOUS MATERIALS
(2021)
Article
Chemistry, Physical
Christianna N. Lininger, Joseph A. Gauthier, Wan-Lu Li, Elliot Rossomme, Valerie Vaissier Welborn, Zhou Lin, Teresa Head-Gordon, Martin Head-Gordon, Alexis T. Bell
Summary: Density Functional Theory (DFT) is the most tractable choice for understanding mechanistic pathways in electrocatalytic processes like CO2 or CO reduction. The study found that the surface modified RPBE functional performs reliably in many benchmarks, while meta-GGA functionals also show promising results. Among them, B97M-rV predicts the correct site preference for CO binding on Ag and Au, while RTPSS performs well for surface relaxations and CO binding on Pt and Cu.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Adrian L. Orjuela, Francisco Nunez-Zarur, Jorge Ali-Torres
Summary: Iron complexes are important in biological processes and neurological disorders. The calculation of the standard reduction potential of iron complexes is challenging. This study presents a computational protocol that provides good results compared to experimental values and other methods.
Article
Environmental Sciences
Jianfeng Zhang, Chunyu Liu, Yu Wu, Xinyu Li, Jiejing Zhang, Jing Liang, Yongguang Li
Summary: This study investigates the adsorption of tetracycline (TC) on a prepared polycationic straw (MMS) and provides insights into its mechanism. The results show that the adsorption is a spontaneous, monolayer reaction involving electrostatic interaction and hydrogen bonds. Machine learning prediction confirms the feasibility and offers a novel strategy for reducing the cost of removing other pollutants.
ENVIRONMENTAL POLLUTION
(2024)
Article
Chemistry, Physical
Aaron D. Kaplan, Stewart J. Clark, Kieron Burke, John P. Perdew
Summary: Classical turning surfaces of Kohn-Sham potentials separate classically allowed regions (CARs) from classically forbidden regions (CFRs). The presence and distribution of CFRs vary in different materials based on factors such as material type and internuclear distances. Many semiconductors have no CFR at equilibrium, which is crucial for density functional construction.
NPJ COMPUTATIONAL MATERIALS
(2021)
Article
Materials Science, Multidisciplinary
S. Emad Rezaei, Mona Zebarjadi, Keivan Esfarjani
Summary: The BoltzWann code uses density-functional theory to calculate the material's response to electric field, temperature gradient, and magnetic field. This work introduces a generalized method for calculating the thermomagnetic properties of materials.
COMPUTATIONAL MATERIALS SCIENCE
(2022)
Article
Materials Science, Multidisciplinary
Akio Ishii
Summary: In this study, the nucleation process of Zr hydrides was investigated using density functional theory calculations and minimum energy path detection. The findings show that, although ZrH and ZrH2 are more energetically stable than Zr4H and Zr2H at 0K, the latter have lower activation energies for nucleation. At finite temperatures, ZrH becomes the most possible candidate with the lowest activation energy.
COMPUTATIONAL MATERIALS SCIENCE
(2022)
Article
Engineering, Chemical
Qian Zhang, Shuming Wen, Qi Zuo, Qicheng Feng
Summary: In this study, microflotation experiments and density functional theory (DFT) calculations were conducted to investigate the influence of ammonium salts on azurite sulfidization. The results showed that the combined treatment of ammonium salt and Na2S resulted in a higher flotation recovery of azurite compared to Na2S treatment alone. DFT calculations demonstrated that HS- could chemically adsorb on the azurite surface and form copper sulfide species. The presence of NH3 enhanced the adsorption of S species and stability of Cu-S species, acting as a catalyst in azurite sulfidization.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Chemistry, Physical
Jiyoon Choi, Hyungjun Kim
Summary: Photoredox catalysts (PCs) have advanced organic chemistry by utilizing reactive electrons in excited states, with chemists seeking new promising PCs. Quantum chemical simulations offer efficient exploration of chemical space. A theoretical protocol was designed to predict excited-state redox properties with high accuracy, focusing on three critical factors: solvent effects on geometries, Hartree-Fock exchange, and double-excitation character.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Physical
Mengna Bai, Zhiheng Song, Zheng Yang, Zhiqing Guo, Yizhou Liu, Haoran Guo, Hanwu Lei, Erguang Huo
Summary: The catalytic conversion mechanism of guaiacol on the MgO surface, as a model compound of methoxy phenols, was investigated in this study using density functional theory calculations. The results showed that the presence of a pre-adsorbed hydrogen atom on the MgO surface resulted in lower adsorption energy and lower energy barrier for the conversion of guaiacol into o-cresol compared to the clean MgO surface. This indicates that the presence of a hydrogen source promotes the conversion of methoxy phenols into alkylated phenols over the MgO catalyst.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Inorganic & Nuclear
Krithika Ganesan, Ilakya Kaliyaperumal, Prabha Vadivelu
Summary: The study compared the reactivities of [Mn(13-TMC)(OOH)](2+) and [Mn(13-TMC)-(O-2)](+) in the sulfoxidation of thioanisole, showing that the former is kinetically and thermodynamically preferred due to feasible heterolytic O1-O2 bond cleavage and proton transfer steps in the reaction mechanism. Incorporating electron donating substituents in thioanisole and non-redox metal ions such as Y3+ can enhance the reactivity of [Mn(13-TMC)-(O-2)](+) species, making it comparable to [Mn(13-TMC)(OOH)](2+) in the sulfoxidation process, especially with Y3+ present.
INORGANIC CHEMISTRY
(2021)
Review
Chemistry, Analytical
Songbai Zhang, Shuang Li, Rixin Yan, Zhiyun Zhou, Yuting Wu, Yi Lu
Summary: This review summarizes the recent advances of PGM-based biosensors for non-glucose targets, including signal transduction, signal amplification, and target molecule recognition and analysis. Current challenges and future directions are also discussed.
CURRENT ANALYTICAL CHEMISTRY
(2022)
Review
Materials Science, Multidisciplinary
Nantao Li, Bin Zhao, Robert Stavins, Ana Sol Peinetti, Neha Chauhan, Rashid Bashir, Brian T. Cunningham, William P. King, Yi Lu, Xing Wang, Enrique Valera
Summary: The COVID-19 pandemic has highlighted limitations in current infectious disease diagnosis models, but efforts are underway to develop more effective rapid tests and address cost and time barriers for new test kits. Nanomaterials and nanochemistry show promise in enabling simpler workflows, high sensitivity, and scalable manufacturing for improved virus detection.
CURRENT OPINION IN SOLID STATE & MATERIALS SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Nantao Li, Xiaojing Wang, Joseph Tibbs, Congnyu Che, Ana Sol Peinetti, Bin Zhao, Leyang Liu, Priyash Barya, Laura Cooper, Lijun Rong, Xing Wang, Yi Lu, Brian T. Cunningham
Summary: This study introduces a label-free biosensing method for quickly detecting and quantifying intact viruses in human saliva with high selectivity and sensitivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Biochemistry & Molecular Biology
Aaron P. Ledray, Sudharsan Dwaraknath, Khetpakorn Chakarawet, Madeline R. Sponholtz, Claire Merchen, Casey Van Stappen, Guodong Rao, R. David Britt, Yi Lu
Summary: A biosynthetic model of oxidases was constructed by replacing tyrosine with tryptophan, and it was demonstrated that tryptophan can also promote the oxygen reduction reaction, although with lower activity. Structural analysis and experimental results indicate that the difference in activity is due to the higher reduction potential of tryptophan. This study provides the first evidence that tryptophan can promote the oxygen reduction reaction and offers a structural basis for the observation of varying activities.
Article
Chemistry, Multidisciplinary
Yu Zhou, Evan N. Mirts, Sangdo Yook, Matthew Waugh, Rachel Martini, Yong-Su Jin, Yi Lu
Summary: We report a biocatalytic system for direct generation of TAL derivatives under mild conditions by rationally engineering the 2PS active site and rewiring the biocatalytic pathway in the metabolic network of E. coli. The system can produce high-value products, such as kavalactone precursors, with yields up to 17 mg/L culture. Computer modeling suggests that sterics and hydrogen-bond interactions play key roles in tuning the selectivity, efficiency, and yield.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xiaojing Wang, Skye Shepherd, Nantao Li, Congnyu Che, Tingjie Song, Yanyu Xiong, Isabella Rose Palm, Bin Zhao, Manish Kohli, Utkan Demirci, Yi Lu, Brian T. T. Cunningham
Summary: In this study, an efficient target recycling amplification process (TRAP) using photonic resonator absorption microscopy was developed for the digital detection of exosomal microRNAs (miRNAs). The TRAP approach demonstrated high sensitivity, robust selectivity, and a broad dynamic range, making it ideal for quantifying miRNA biomarkers in low concentrations or sample volume. Compared to traditional qRT-PCR, TRAP showed similar accuracy in profiling exosomal miRNAs derived from cancer cells, but with significantly enhanced detection limits for miRNA-375 and miRNA-21.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biophysics
Shanni Hong, Zhenglin Yang, Quanbing Mou, Yunxia Luan, Bingbo Zhang, Renjun Pei, Yi Lu
Summary: This study presents a fluorescence aptamer sensor that can monitor the rapid leaching kinetics of quantum dots and the concentration of ions in living cells in real time. The sensor shows high specificity and can be used to study the biosafety and cytotoxicity mechanisms of various cadmium-based quantum dots.
BIOSENSORS & BIOELECTRONICS
(2023)
Article
Nanoscience & Nanotechnology
Tingrui Xu, Xuejiao Li, Yang Wang, Zhongfeng Tang
Summary: In this work, the relationships between the structures and thermophysical properties of molten MgCl2-NaCl and MgCl2-KCl eutectic salts were systematically studied using deep potential molecular dynamics simulations. It was found that molten MgCl2-KCl salt has higher specific heat capacity, while molten MgCl2-NaCl salt exhibits higher thermal conductivity and lower viscosity. The reliability of the microscopic structures and macroscopic properties of these salts were verified at different temperatures.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Yunling Deng, Sudharsan Dwaraknath, Wenhao O. Ouyang, Cory J. Matsumoto, Stephanie Ouchida, Yi Lu
Summary: Researchers have synthesized cobalt porphyrin substituted myoglobin (CoMb) as a homogeneous catalyst for photo-driven CO2 to CO conversion in water. By optimizing the activity and product selectivity through varying pH and concentrations of the enzyme and the photosensitizer, they achieved high efficiency of CO generation. They further enhanced the CO2-reducing performance by introducing positively charged residues near the active site of CoMb.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Zhimei Huang, Xianbo Ma, Fengze Jiang, Rong Wang, Zhenkun Wu, Yi Lu
Summary: DNAwalkers have been widely used in biosynthesis, biocomputing, and biosensing due to their programmability, biocompatibility, and signal amplification capacity. A dual spatially localized DNA walker was designed to drive high-speed stochastic movement along three-dimensional tracks using bipedal catalysts. The colocalization of autocatalytic circuits and the use of bipedal catalysts significantly increased the reaction kinetics. An RNA-responsive PCHA walker was constructed for mRNA imaging in live cells, providing a novel and efficient tool for biomolecule detection and biological functions regulation.
Article
Biotechnology & Applied Microbiology
Yuan Ma, Weijie Guo, Quanbing Mou, Xiangli Shao, Mingkuan Lyu, Valeria Garcia, Linggen Kong, Whitney Lewis, Carson Ward, Zhenglin Yang, Xingxin Pan, S. Stephen Yi, Yi Lu
Summary: GlycoRNA imaging in cells is achieved through a proximity ligation assay called ARPLA. This assay allows visualization of glycoRNAs, a recently discovered class of glycosylated molecules, in single cells with high sensitivity and selectivity. ARPLA enables the detection of spatial distributions of glycoRNAs on the cell surface, their colocalization with lipid rafts, and the intracellular trafficking of glycoRNAs.
NATURE BIOTECHNOLOGY
(2023)
Article
Multidisciplinary Sciences
Yuting Wu, Seyed-Fakhreddin Torabi, Ryan J. Lake, Shanni Hong, Zhengxin Yu, Peiwen Wu, Zhenglin Yang, Kevin Nelson, Weijie Guo, Gregory T. Pawel, Jacqueline Van Stappen, Xiangli Shao, Liviu M. Mirica, Yi Lu
Summary: By developing DNAzyme-based fluorescent turn-on sensors, we can selectively visualize either Fe2+ or Fe3+, revealing a decreased Fe3+/Fe2+ ratio during ferroptosis and an increased Fe3+/Fe2+ ratio in Alzheimer's disease mouse brain. The elevated Fe3+/Fe2+ ratio was mainly observed in amyloid plaque regions, suggesting a correlation between amyloid plaques and the accumulation of Fe3+ and/or conversion of Fe2+ to Fe3+. Our sensors can provide deep insights into the biological roles of labile iron redox cycling.
Article
Chemistry, Multidisciplinary
Huanhuan Fan, Claire E. E. McGhee, Ryan J. J. Lake, Zhenglin Yang, Zijian Guo, Xiao-Bing Zhang, Yi Lu
Summary: Manganese is an essential element in the human body and its detection in living cells is important. However, specific fluorescent sensors for Mn2+ are rare due to its paramagnetism and poor selectivity against other metal ions. This study reports the development of an RNA-cleaving DNAzyme with high selectivity for Mn2+ and its conversion into a fluorescent sensor. The sensor has been successfully used to detect Mn2+ in immune cells and tumor cells, as well as monitor the degradation of manganese-based nanomaterials in tumor cells.
Article
Chemistry, Inorganic & Nuclear
Yiwei Liu, Nicholas M. Marshall, Sheng-Song Yu, Wantae Kim, Yi-Gui Gao, Howard Robinson, Mark J. Nilges, Yan Zhang, Siu Yee New, Yi Lu
Summary: A study was conducted to investigate the effects of M13F, M44F, and G116F mutations on E & DEG; in azurin. The introduction of Phe residues at different positions and in different combinations can modulate E & DEG; in various ways, with a maximum change of 64 mV. X-ray crystal structures revealed that the spatial orientations of the Phe residues and H-bonding networks around the T1Cu-coordinating His117 are responsible for these effects. Furthermore, the study demonstrated the differential influence of M13F, M44F, and G116F mutations on the E & DEG; of T1Cu, with M13F decreasing E & DEG;, M44F increasing E & DEG;, and G116F showing a negligible effect. Combining certain mutations also resulted in cooperative effects on E & DEG;. Crystal structures provided insight into the steric effects and fine-tuning of hydrogen bond networks that contribute to these changes. Overall, the findings of this study contribute to the understanding and development of redox-active proteins with tunable properties.
INORGANIC CHEMISTRY
(2023)
Proceedings Paper
Optics
Nantao Li, Xiaojing Wang, Joseph Tibbs, Taylor D. Canady, Qinglan Huang, Glenn A. Fried, Xing Wang, Laura Cooper, Lijun Rong, Yi Lu, Brian T. Cunningham
Summary: Interferometric scattering microscopy is a promising technique for biomedical research and diagnostic testing, allowing the detection of nano-objects through their elastic light scattering. The photonic resonator interferometric scattering microscopy (PRISM) amplifies scattered light through a photonic crystal resonator, enabling improved signal-to-noise ratio. The technology has shown potential in virus and protein detection, with results comparable to conventional nucleic acid tests.
INTEGRATED OPTICS: DEVICES, MATERIALS, AND TECHNOLOGIES XXVI
(2022)
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)