Article
Chemistry, Multidisciplinary
Margaret D. D. Doyle, Asmit Bhowmick, David C. C. Wych, Louise Lassalle, Philipp S. S. Simon, James Holton, Nicholas K. K. Sauter, Vittal K. K. Yachandra, Jan F. F. Kern, Junko Yano, Michael E. E. Wall
Summary: The structural dynamics of water and its hydrogen-bonding networks are crucial for enzyme function. This study used crystalline molecular dynamics simulations to investigate the water oxidation reaction in Photosystem II (PS II). The simulations provided insights into water mobility and hydrogen-bonding networks, revealing potential pathways for proton transfer during the reaction cycle of PS II. These findings contribute to our understanding of the specific roles of each channel in the water oxidation reaction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Asmit Bhowmick, Rana Hussein, Isabel Bogacz, Philipp S. Simon, Mohamed Ibrahim, Ruchira Chatterjee, Margaret D. Doyle, Mun Hon Cheah, Thomas Fransson, Petko Chernev, In-Sik Kim, Hiroki Makita, Medhanjali Dasgupta, Corey J. Kaminsky, Miao Zhang, Julia Gaetcke, Stephanie Haupt, Isabela I. Nangca, Stephen M. Keable, A. Orkun Aydin, Kensuke Tono, Shigeki Owada, Leland B. Gee, Franklin D. Fuller, Alexander Batyuk, Roberto Alonso-Mori, James M. Holton, Daniel W. Paley, Nigel W. Moriarty, Fikret Mamedov, Paul D. Adams, Aaron S. Brewster, Holger Dobbek, Nicholas K. Sauter, Uwe Bergmann, Athina Zouni, Johannes Messinger, Jan Kern, Junko Yano, Vittal K. Yachandra
Summary: In natural photosynthesis, the light-driven splitting of water is the first step in converting solar energy into chemical energy. The reaction occurs in photosystem II, where the Mn4CaO5 cluster plays a crucial role in storing oxidizing equivalents and catalyzing the O-O bond formation. By using X-ray crystallography, we observed the structural changes during the S-3 ->[S-4]-> S-0 transition, which is the final step of the Kok's photosynthetic water oxidation cycle. Our findings provide insights into the complex events that occur during this process, including changes in the Mn4CaO5 cluster, ligands, water pathways, and proton release mechanism.
Article
Chemistry, Multidisciplinary
Ruoqing Yao, Yanxi Li, Yang Chen, Boran Xu, Changhui Chen, Chunxi Zhang
Summary: This study presents synthetic Mn4XO4 clusters that closely resemble the natural oxygen-evolving center in photosynthesis, providing new insights for the design of water-splitting catalysts in artificial photosynthesis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Plant Sciences
Hiroyuki Mino
Summary: The temperature dependence of the formation of the g similar to 5 S-2 state electron paramagnetic resonance (EPR) signal in photosystem II (PSII) was investigated. It was found that the g similar to 5 signal can be produced at an illumination above 200 K, and its formation is half inhibited at approximately 215 K. The study also estimated the activation energy, enthalpy, and entropy of the g similar to 5 state formation.
PHOTOSYNTHESIS RESEARCH
(2022)
Article
Green & Sustainable Science & Technology
Yuriy Shapovalov, Rustam Tokpayev, Tamina Khavaza, Mikhail Nauryzbayev
Summary: Photosynthesis is considered a promising area for cheap and environmentally friendly energy production. The process involves water oxidation to generate oxygen and hydrogen, with the mechanisms of H+, O-2 up arrow, e(-) production described in this review. The functioning mechanisms of PS-I and PS-II can potentially be used in developing environmentally friendly technologies for molecular hydrogen production.
Article
Chemistry, Physical
Takumi Matsubara, Yuichiro Shimada, Tomomi Kitajima-Ihara, Ryo Nagao, Takumi Noguchi
Summary: In this study, the photoactivation process of cyanobacterial PSII was monitored using time-resolved Fourier transform infrared spectroscopy, revealing the molecular mechanism of the initial Mn2+ coordination and the conformational changes of proteins during the dark rearrangement process.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Inorganic & Nuclear
Tomoyo Misawa-Suzuki, Sota Mafune, Hirotaka Nagao
Summary: This study presents a diruthenium(III,IV) complex with a doubly oxido-bridged core and a carbonato bridged between the two ruthenium centers, exploring interactions with cations. In acidic aqueous solutions, the carbonato ligand remained bound to the doubly bridged core, undergoing reversible protonation/deprotonation reactions. The structures of the protonated complexes were successfully characterized.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Hiroshi Isobe, Mitsuo Shoji, Takayoshi Suzuki, Jian-Ren Shen, Kizashi Yamaguchi
Summary: In photosystem II, water is oxidized to dioxygen through a Mn4CaO5 cluster, with two competing reaction routes, stepwise and concerted, affecting the formation of the final stable closed structure.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2021)
Article
Plant Sciences
Hiroyuki Mino, Mizue Asada
Summary: This study identified two Mn2+ sites in PSII using PELDOR, with one Mn2+ ion binding to apo-PSII during deactivation of the oxygen-evolving complex. The site between His332 and Glu189 in the D1 polypeptide was found to be in close proximity to the Mn1 site in mature PSII. Additionally, the position between Asp170 and Glu189 in the D1 polypeptide was suggested as a potential initial high-affinity site for photoactivation based on comparisons with electron microscope structures.
PHOTOSYNTHESIS RESEARCH
(2022)
Article
Biochemistry & Molecular Biology
Mehar Fatma, Noushina Iqbal, Zebus Sehar, Mohammed Nasser Alyemeni, Prashant Kaushik, Nafees A. Khan, Parvaiz Ahmad
Summary: The study showed that application of MeJA during heat stress in wheat plants increased enzymatic antioxidant activity, reduced hydrogen peroxide and TBARS content, and enhanced photosynthetic efficiency.
Article
Biology
Stefania Viola, William Roseby, Stefano Santabarbara, Dennis Nurnberg, Ricardo Assuncao, Holger Dau, Julien Selles, Alain Boussac, Andrea Fantuzzi, A. William Rutherford
Summary: The study compares the turnover efficiency, electron transfer, reactions, and photodamage of different types of photosystem II (PSII). The results show that Chl-d-PSII is more sensitive to photodamage compared to Chl-a-PSII and Chl-f-PSII, but generates more singlet oxygen in the recombination via PD1+Phe repopulation. Chl-f-PSII avoids harmful reactions by adjusting energy gaps, making it more resilient to photodamage.
Article
Biochemistry & Molecular Biology
Ingrid Pereira, Joyce K. Dare, Elaine F. F. da Cunha, Matheus P. Freitas
Summary: This study combines two congeneric series of benzamide herbicides and models their herbicidal activities against PSII. It predicts the pIC(50) of new agrochemical candidates and identifies the most promising compound based on chemical features and ligand-enzyme interactions.
JOURNAL OF BIOMOLECULAR STRUCTURE & DYNAMICS
(2023)
Article
Biochemistry & Molecular Biology
Casper de Lichtenberg, Anton P. Avramov, Minquan Zhang, Fikret Mamedov, Robert L. Burnap, Johannes Messinger
Summary: This study investigated the impact of the V185N mutation in the D1 protein on water oxidation by measuring the exchange kinetics of substrate waters in PSII core complexes. The mutation was found to affect the rate of substrate water binding and the signals of the Mn4Ca cluster in different states. Additionally, it was observed that the V185N mutation may stabilize an additional water-derived ligand at the Mn1 site via hydrogen bonding, affecting the binding sites of substrate waters.
BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS
(2021)
Review
Plant Sciences
Thomas Oliver, Tom D. Kim, Joko P. Trinugroho, Violeta Cordon-Preciado, Nitara Wijayatilake, Aaryan Bhatia, A. William Rutherford, Tanai Cardona
Summary: Recent advances in understanding the origin and evolution of photosystem II are reviewed and discussed, revealing that water oxidation occurred early in the history of life. Photosystem II has remained relatively unchanged for billions of years, but constant duplication of the D1 subunit has allowed the enzyme to adapt to different environments and even develop enzymatic functions beyond water oxidation. This adaptability could be utilized to develop novel light-powered enzymes for sustainable biocatalysis.
ANNUAL REVIEW OF PLANT BIOLOGY
(2023)
Article
Biochemistry & Molecular Biology
Richard J. Debus
Summary: In this study, the impact of the D1-D170E mutation on the Mn4Ca cluster in PSII was characterized using Fourier transform infrared difference spectroscopy. The mutation altered the hydrogen bond network surrounding the Mn4Ca cluster and led to the production of a high-spin form of the S-2 state during the S-1-to-S-2 transition. Additionally, the mutation may change the coordination mode of the carboxylate group at position 170.
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)