Article
Chemistry, Physical
Ernest Antwi, Rachel E. Bush, Barbara Marchetti, Tolga N. V. Karsili
Summary: Criegee intermediates, highly reactive molecules with vital roles in various fields, were studied using state-of-the-art techniques. The study revealed the impact of long-range internal conversion on the products of photoinduced fragmentation.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Yen-Ju Wu, Kaito Takahashi, Jim Jr-Min Lin
Summary: The kinetics of the reaction between the simplest Criegee intermediate (CH2OO) and water vapor were investigated. The study found that the decay of CH2OO involves not only two water molecules, but also one and three water molecules. The results suggest that the decay can be described by a polynomial equation at 298K and 300 Torr. Additionally, the investigation of the kinetic isotope effect provided insights into the reaction mechanism involving hydrogen and oxygen atom motions.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Ernest Antwi, Jordyn M. Ratliff, Michael N. R. Ashfold, Tolga N. V. Karsili
Summary: Ab initio molecular dynamics studies of CH2OO molecules following excitation to the S-2 ((1)pi pi*) state reveal diverse behaviors, including high surface hopping probability, O-O bond fission, and twisted geometries.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Mahesh K. Sit, Subhasish Das, Kousik Samanta
Summary: High fidelity potential energy surfaces and nonadiabatic couplings were constructed using machine learning, and used to simulate the photodissociation of CH2OO. The results showed that there is an 88.4% probability of dissociation through the lower channel, and only a 11.6% probability of dissociation through the upper channel.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Guanghan Wang, Tianlin Liu, Adriana Caracciolo, Michael F. Vansco, Nisalak Trongsiriwat, Patrick J. Walsh, Barbara Marchetti, Tolga N. Karsili, Marsha Lester
Summary: The study examined the electronic spectrum of MVK-oxide on its second pi* & LARR; pi transition below and above 300 nm UV wavelengths, revealing different dissociation pathways and product characteristics upon electronic excitation.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Biochemistry & Molecular Biology
Ernest Antwi, Niamh A. A. Packer, Jordyn M. M. Ratliff, Barbara Marchetti, Tolga N. V. Karsili
Summary: This passage discusses the formation of Criegee intermediates (CIs) from isoprene ozonolysis and how the increasing molecular complexity affects their photodynamics. The excited state chemistry of CH2OO, MVK-oxide, and MACR-oxide is compared to understand the different product channels and quantum yields, providing insights into the atmospheric implications.
PHOTOCHEMISTRY AND PHOTOBIOLOGY
(2022)
Article
Chemistry, Physical
Jinfeng Liu, Yanqing Liu, Jinrong Yang, Xiao Cheng Zeng, Xiao He
Summary: The reaction of the smallest Criegee intermediate, CH2OO, with a water cluster was investigated through ab initio molecular dynamics simulations. The reaction was found to occur both at the air/water interface and inside the water cluster, requiring more than one reactive water molecule. Different reaction pathways were observed, with the involvement of transient H3O+ impacting the atmospheric budget of trace gases.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Courtney A. Poirier, Lily M. Guidry, Jordyn M. Ratliff, Vincent J. Esposito, Barbara Marchetti, Tolga N. V. Karsili
Summary: This study focuses on the ground- and excited-state chemistry of the simplest fluorinated Criegee intermediate (CI), fluoroformaldehyde oxide (HFCOO), formed from the ozonolysis of HFOs. The results show that HFCOO is more prone to undergo cyclization reactions in the ground state compared to the simplest CI. In the excited state, HFCOO undergoes O-O bond fission to produce various products. The implications of these findings are discussed in terms of both physical and atmospheric chemistry.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Meijun Zou, Tianlin Liu, Michael F. Vansco, Christopher A. Sojdak, Charles R. Markus, Raybel Almeida, Kendrew Au, Leonid Sheps, David L. Osborn, Frank A. F. Winiberg, Carl J. Percival, Craig A. Taatjes, Stephen J. Klippenstein, Marsha I. Lester, Rebecca L. Caravan
Summary: Methyl-ethyl-substituted Criegee intermediate (MECI) is a carbonyl oxide formed in the ozonolysis of asymmetric alkenes. It lacks resonance stabilization and reacts faster with SO2 compared to MVK-oxide + SO2, indicating the significant influence of resonance stabilization on Criegee intermediate reactivity.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Analytical
Pei-Ling Luo, I-Yun Chen
Summary: In this study, a spectrometer based on synchronized two-color time-resolved dual-comb spectroscopy was developed for simultaneous spectral acquisitions in two molecular fingerprint regions. By using high-resolution rovibrational absorption spectroscopy, the concentration of target molecules can be quantitatively detected and simulated, enabling exploration of reaction mechanisms and pathways related to the formation of HOx radicals.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Lei Yang, Mixtli Campos-Pineda, Jingsong Zhang
Summary: This study indirectly measured the yield of thermalized formaldehyde oxide produced from the ozonolysis of ethene, and found that the yield decreases with decreasing pressure. Kinetic models were used to better evaluate and understand different measurement methods of thermalized Criegee intermediates.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Spectroscopy
Carlos Cabezas, Adam M. Daly, Yasuki Endo
Summary: The reaction system between the simplest Criegee intermediate, CH2OO, and the greenhouse gas CO2 has been investigated using Fourier transform microwave spectroscopy. A weakly bound CH2OO-CO2 complex was identified in the rotational spectrum, and the torsional energy difference between two tunneling states was accurately determined. The limited reactivity of CIs toward CO2 was confirmed by the non-observation of the cycloaddition reaction product.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2021)
Article
Chemistry, Physical
Yang Chen, Haotian Jiang, Siyue Liu, Jiayu Shi, Yuqi Jin, Xueming Yang, Wenrui Dong
Summary: The kinetics of the reaction between the simplest Criegee intermediate (CH2OO) and tert-butylamine ((CH3)3CNH2) were studied. The reaction rate coefficient was found to be (4.95 ± 0.64) × 10^-12 cm3 molecule^-1 s^-1 at 298K. The reaction was observed to be negative temperature-dependent, with an activation energy of (-2.82 ± 0.37) kcal mol^-1 and a pre-exponential factor of (4.21 ± 0.55) × 10^-14 cm3 molecule^-1 s^-1.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Tien Pham, Hoang T. T. Trang
Summary: The detailed reaction mechanism and kinetics of the C3H3 + CH2OO system have been explored using the CBS-QB3 method and ME/vRRKM theory. The dominant reaction channel is C3H3 + CH2OO-* CH2-[cyc-CCHCHOO] + H. The rate constants of the reaction are dependent on temperature and pressure, with the highest branching ratio observed for the CH2-[cyc-CCHCHOO] + H channel.
Article
Chemistry, Physical
Amit Kumar, Subhasish Mallick, Pradeep Kumar
Summary: In this study, the reaction of nitrous acid with the simplest Criegee intermediate was investigated using chemical kinetics and quantum chemical calculations. It was found that the reaction can proceed through four different paths, involving hydrogen atom transfer, cycloaddition, and oxygen atom transfer, leading to the formation of different products. The possibility of in situ generation of HNO3 and formic acid from HONO was reported for the first time. The hydrogen atom transfer path was found to be the fastest and dominant in the Criegee reaction with HONO. However, compared to other dominant Criegee reactions, the reaction with a water molecule outweighs its significance.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Mica C. Smith, Guozhu Liu, Zachary J. Buras, Te-Chun Chu, Jeehyun Yang, William H. Green
JOURNAL OF PHYSICAL CHEMISTRY A
(2020)
Article
Multidisciplinary Sciences
Rebecca L. Caravan, Michael F. Vansco, Kendrew Au, M. Anwar H. Khan, Yu-Lin Li, Frank A. F. Winiberg, Kristen Zuraski, Yen-Hsiu Lin, Wen Chao, Nisalak Trongsiriwat, Patrick J. Walsh, David L. Osborn, Carl J. Percival, Jim Jr-Min Lin, Dudley E. Shallcross, Leonid Sheps, Stephen J. Klippenstein, Craig A. Taatjes, Marsha Lester
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2020)
Article
Chemistry, Physical
Mei-Tsan Kuo, Kaito Takahashi, Jim Jr-Min Lin
Article
Chemistry, Physical
Te-Chun Chu, Mica C. Smith, Jeehyun Yang, Mengjie Liu, William H. Green
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS
(2020)
Article
Chemistry, Multidisciplinary
Yu-Lin Li, Chun-Yu Lin, Yen-Hsiu Lin, Jim Jr-Min Lin
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
(2020)
Article
Chemistry, Multidisciplinary
Yen-Hsiu Lin, Cangtao Yin, Kaito Takahashi, Jim Jr-Min Lin
Summary: The study reveals that anti-MACRO reacts quickly with SO2 but slowly with water vapor, leading to a longer atmospheric lifetime, higher steady-state concentration, and greater impact on the oxidation of atmospheric SO2.
COMMUNICATIONS CHEMISTRY
(2021)
Article
Meteorology & Atmospheric Sciences
Mica C. Smith, Julia M. Carlstad, P. Quinby Hunter, John Randazzo, Kristie A. Boering
Summary: The study found that N2O produced under specific conditions has a unique isotopic composition, which can be used to determine the different sources of N2O through isotope measurements. Isotopic composition research helps to further understand the formation and destruction mechanisms of N2O and can be used to identify the sources of changes in atmospheric N2O concentrations.
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
(2021)
Article
Chemistry, Physical
Mei-Tsan Kuo, Jie-Ning Yang, Jim Jr-Min Lin, Kaito Takahashi
Summary: The study revealed that 3-aminopropanol exhibits higher reactivity towards Criegee intermediates compared to other amines or alcohols, with a significant decrease in reactivity observed in the case of vinyl substitution. Theoretical calculations and experimental data showed that the vinyl substitution has a substantial impact on the reactivity, with the rate coefficient decreasing by two orders of magnitude. These findings are valuable for estimating the impact of similar reactions in the atmosphere and suggest potential applications of the B2PLYP-D3BJ method for predicting reactions involving larger Criegee intermediates.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Yen-Hsiu Lin, Jim Jr-Min Lin
Summary: A method is demonstrated to determine the absolute value of the photodissociation cross section of a molecule in a cell without knowing its absolute concentration. The method involves monitoring the UV-visible absorption spectra of the target molecule before and after photodissociation by a pulsed laser beam, with corrections made for systematic errors caused by inhomogeneity of the photolysis laser beam. Post-photolysis reactions can affect measurements, but can be estimated and corrected if the kinetics of these reactions are known.
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Jie-Ning Yang, Kaito Takahashi, Jim Jr-Min Lin
Summary: This study investigated the reaction kinetics between HNO3 and four Criegee intermediates and found that these reactions are fast and occur under specific conditions. Under high-humidity conditions, these reactions may not be important.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Yen-Hsiu Lin, Yen-Ju Wu, Jim Jr-Min Lin
Summary: The oxidation flow reactor system allows studying the effect of VOC oxidation on aerosol formation. It can accelerate the oxidation process and be used to investigate the properties and sources of the generated secondary organic aerosols.
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Yen-Ju Wu, Kaito Takahashi, Jim Jr-Min Lin
Summary: The kinetics of the reaction between the simplest Criegee intermediate (CH2OO) and water vapor were investigated. The study found that the decay of CH2OO involves not only two water molecules, but also one and three water molecules. The results suggest that the decay can be described by a polynomial equation at 298K and 300 Torr. Additionally, the investigation of the kinetic isotope effect provided insights into the reaction mechanism involving hydrogen and oxygen atom motions.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Yen-Hsiu Lin, Kaito Takahashi, Jim Jr-Min Lin
Summary: Methyl vinyl ketone oxide (MVKO) and methacrolein oxide (MACRO) are resonance-stabilized Criegee intermediates formed in the ozonolysis reaction of isoprene. Their photodissociation cross sections and synthesis yields have been measured, providing insights into the impact of isoprene on the atmosphere.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Jeehyun Yang, Mica C. Smith, Matthew B. Prendergast, Te-Chun Chu, William H. Green
Summary: This study experimentally confirms that single-radical HACA can play a significant role in the formation of PAHs larger than naphthalene, in line with the predictions of a kinetic model and the HACA mechanism.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Mengjie Liu, Te-Chun Chu, Agnes Jocher, Mica C. Smith, Istvan Lengyel, William H. Green
Summary: The RMG-generated model accurately predicts major species profiles but underestimates the formation of anthracene, phenanthrene, and pyrene, with PAHs beyond pyrene not captured.
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS
(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)
