Editorial Material
Chemistry, Physical
Claire C. Cody, Gary W. Brudvig
Summary: The key step in the oxidation of water to dioxygen is the formation of the O-O bond, which remains not fully understood. A recent report in Nature Chemistry features the structural characterization of a catalytically relevant elusive peroxo intermediate.
Article
Chemistry, Multidisciplinary
Jiajia Yi, Shaoqi Zhan, Lin Chen, Qiang Tian, Ning Wang, Jun Li, Wenhua Xu, Biaobiao Zhang, Marten S. G. Ahlquist
Summary: In this study, two facile and effective design strategies were introduced to facilitate the coupling of two catalytic units via electrostatic interactions, resulting in significantly improved catalytic performance. The intermolecular electrostatic interactions in these two systems were fully identified and found to play a key role in enhancing catalytic performance. The successful strategies demonstrated here can be utilized in designing other intercatalyst coupling systems for activation and synthesis of small molecules and organic compounds.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Multidisciplinary Sciences
Yuki Tanahashi, Kosuke Takahashi, Yuta Tsubonouchi, Shunsuke Nozawa, Shin-ichi Adachi, Masanari Hirahara, Eman A. Mohamed, Zaki N. Zahran, Kenji Saito, Tatsuto Yui, Masayuki Yagi
Summary: The formation of O-O bond is induced by deprotonation of one of the OH ligands of Ru-2(III)(OH)(2) and requires two RuIII centers to transfer two electrons to their ligands. The intersystem crossing between singlet and triple states of RuII2(mu-OOH) can be easily switched by exchange of H+ between the mu-OOH bridge and the auxiliary backbone ligand.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Zhao Sun, Shufan Yu, Sam Toan, Rufat Abiev, Maohong Fan, Zhiqiang Sun
Summary: In this study, CuCr2O4-based catalytic oxygen carriers were designed for low-temperature methanol reforming. The activation of methanol at relatively low temperatures was achieved through the reinforcement of the Cu-O-Cr structure and the induction of highly reactive lattice oxygen. The hydrogen production rate was significantly increased by 53.2% with the application of CuCr2O4-based catalytic oxygen carriers. Furthermore, the Cu-O-Cr structure demonstrated satisfactory cyclic stability.
Article
Chemistry, Multidisciplinary
Hong-Tao Zhang, Xiao-Jun Su, Fei Xie, Rong-Zhen Liao, Ming-Tian Zhang
Summary: This study highlights the significance of structure regulation in the O-O bond formation process in binuclear iron catalysts. While some catalysts proceed via oxo-oxo coupling, others with rigid ligands show negligible catalytic activity due to limited isomerization and rotation of Fe=O moieties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Xiang-Zhu Wei, Tian-Yu Ding, Yang Wang, Bing Yang, Qing-Qing Yang, Shengfa Ye, Chen-Ho Tung, Li-Zhu Wu
Summary: In this work, an electron-rich and oxidation-resistant ligand was introduced to stabilize high-valent iron-oxo species for water oxidation reactions. Advanced spectroscopies and electrochemical studies revealed the formation of a high-valent Fe-V(O) species in water. Kinetic and oxygen isotope labelling experiments, along with organic reactions, demonstrated that the Fe-V(O) species is responsible for O-O bond formation via water nucleophilic attack under real catalytic water oxidation conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Chul-Ho Yun, Jinhyun Kim, Frank Hollmann, Chan Beum Park
Summary: This article critically summarizes the current developments in photoredox biocatalysis, highlighting promising concepts and discussing current limitations.
Article
Chemistry, Organic
Jiaxing Chen, Yongzhuo Xu, Wen Shao, Jianhua Ji, Boqiang Wang, Muyang Yang, Guojiang Mao, Fuhong Xiao, Guo-Jun Deng
Summary: A Pd-catalyzed C-O cross-coupling reaction was reported, which allows for the synthesis of highly congested hydroxylamines with an α-quaternary carbon center without cleavage of the N-O bond. This strategy shows high chemoselectivity, broad substrate scope, and excellent functional group tolerance, and has been demonstrated by pharmaceutical derivatization and postcatalytic modifications.
Article
Chemistry, Multidisciplinary
Aditya Paul, Arunava Sengupta, Somnath Yadav
Summary: This paper reports a photoresponsive electron donor-acceptor (EDA) complex, which can be detected through absorption and emission spectroscopy. Irradiation of the EDA complex with visible light triggers photoinduced single electron transfer (SET) processes that are useful for the catalyst-free, regioselective acetylation of indoles. The photocatalytic reaction with excess DAIB is also used for the synthesis of isatins. DFT and TD-DFT studies are performed to model the excited states of the EDA complex and validate the photoinduced SET mechanism.
CHEMICAL COMMUNICATIONS
(2023)
Article
Engineering, Environmental
Jiliang Ma, Junqiang Zhang, Dongnv Jin, Shuangquan Yao, Runcang Sun
Summary: This study demonstrates the simultaneous photocatalytic water splitting and reforming of biomass-derived feedstock using co-doped graphitic carbon nitride. The resulting material showed enhanced photocatalytic activity and stability, leading to high yields of hydrogen and lactic acid.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Physical
Wei-Yu Mu, Wei Wang, Qiu-Yun Chen, Ling-Ling Qu
Summary: The polymer fused iron(III) nano-complex, PPaba-FeEu@GO, has been developed as an environmentally friendly material for treating phytopathogenic bacteria in hypoxia environments. This nano metal complex shows enhanced electron mobility and hole diffusion distance, converting water into oxygen under LED light irradiation without additional co-catalyst, and can also convert near-infrared light into heat.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2021)
Article
Materials Science, Multidisciplinary
Lin Yang, Jinxing Yu, Shufang Chang, Xiaoxiang Xu
Summary: Doping aluminum into LaTaON2 improves its photocatalytic performance by enhancing charge separation conditions and surface hydrophilicity, leading to more efficient water splitting under visible light illumination.
SCIENCE CHINA-MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Alice Paskin, Thais Couasnon, Jeffrey Paulo H. Perez, Sergey S. Lobanov, Roberts Blukis, Stefan Reinsch, Liane G. G. Benning
Summary: In this study, the nucleation and crystallization processes of vivianite were investigated. The formation of an intermediate amorphous phase and its transformation to crystalline vivianite were monitored. The results reveal that water molecules and ions play a crucial role in the nonclassical hydration-induced nucleation and transformation mechanism of vivianite.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Xiaonong Wang, Xiaoxia Li, Jingxiang Low
Summary: Loading plasmonic Au nanoparticles onto BiVO4 inverse opal can enhance the efficiency of photocatalytic water oxidation by improving light utilization and charge carrier utilization. Optimization of the Au-BiVO4 inverse opal structure can achieve high photocurrent density and long photogenerated charge carrier lifetime, resulting in superior photocatalytic activity.
Article
Chemistry, Multidisciplinary
Cagatay M. Oral, Martina Ussia, Martin Pumera
Summary: In this study, enzyme-immobilized self-propelled zinc oxide microrobots were proposed to effectively remove antibiotics released into water bodies. The presence of laccase enzyme on the microrobot surfaces enhanced the removal of antibiotics via oxidation. This concept provides an environmentally friendly strategy for the removal of released antibiotics from water bodies.
Article
Chemistry, Multidisciplinary
Renato N. Sampaio, David C. Grills, Dmitry E. Polyansky, David J. Szalda, Etsuko Fujita
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Physical
Lei Wang, David W. Shaffer, Gerald F. Manbeck, Dmitry E. Polyansky, Javier J. Concepcion
Article
Chemistry, Physical
Gerald F. Manbeck, Dmitry E. Polyansky, Etsuko Fujita
Article
Chemistry, Physical
Anna Lewandowska-Andralojc, Gordon L. Hug, Bronislaw Marciniak, Gerald Hoerner, Dorota Swiatla-Wojcik
JOURNAL OF PHYSICAL CHEMISTRY B
(2020)
Article
Chemistry, Inorganic & Nuclear
Laura Rotundo, Dmitry E. Polyansky, Roberto Gobetto, David C. Grills, Etsuko Fujita, Carlo Nervi, Gerald F. Manbeck
INORGANIC CHEMISTRY
(2020)
Article
Chemistry, Physical
Laura Rotundo, David C. Grills, Roberto Gobetto, Emanuele Priola, Carlo Nervi, Dmitry E. Polyansky, Etsuko Fujita
Summary: The influence of phenyl, phenol, aniline, amino, and CF substituents of the 2,2'-bipyridine ligand on the photochemical CO2 reduction in dimethylacetamide was examined. The presence of Ph-NH2 moiety was found to enhance both electrochemical and photochemical activity, leading to higher turnover numbers for CO production. The complexes with Ph-OH group in the second coordination sphere also showed promising activity in photochemical CO2 reduction, despite the formation of a stable 6-coordinate intermediate under electrochemical conditions.
Article
Chemistry, Physical
Brian N. DiMarco, Dmitry E. Polyansky, David C. Grills, Ping Wang, Yutaka Kuwahara, Xuan Zhao, Etsuko Fujita
Summary: In this study, the catalytic performance of a series of Co hydrogen evolution catalysts were analyzed by combining electrochemical and transient pulse radiolysis studies. The key factor determining the activity for hydrogen evolution was found to be the hydricity of the [Co-II-H](+) intermediate.
Editorial Material
Chemistry, Physical
Laura Rotundo, David C. Grills, Roberto Gobetto, Emanuele Priola, Carlo Nervi, Dmitry E. Polyansky, Etsuko Fujita
Review
Chemistry, Multidisciplinary
Etsuko Fujita, David C. Grills, Gerald F. Manbeck, Dmitry E. Polyansky
Summary: The conversion of carbon dioxide to fuels and chemicals is a promising strategy for renewable energy storage. Molecular catalysts, particularly coordination complexes of transition metals, play a crucial role in the photo- and electrochemical reduction of CO2. The interactions between catalytic intermediates and promoting factors, such as acids and solvents, have a significant impact on the efficiency of catalysis. Mechanistic studies are essential for the design and improvement of efficient catalysts.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Article
Chemistry, Physical
Dmitry E. Polyansky, David C. Grills, Mehmed Z. Ertem, Ken T. Ngo, Etsuko Fujita
Summary: The use of bimetallic catalysts in CO2 reduction can significantly enhance efficiency and reduce overpotential. Experimental and theoretical studies have confirmed the key role of bimetallic reactivity in the reduction of CO2 to CO, revealing the formation of a bimetallic intermediate and the assistance of a coordinating species.
Article
Chemistry, Inorganic & Nuclear
Laura Rotundo, Shahbaz Ahmad, Chiara Cappuccino, Dmitry E. Polyansky, Mehmed Z. Ertem, Gerald F. Manbeck
Summary: A dicationic Re bipyridine-type complex has been synthesized and studied for its electrochemical behavior under Ar and CO2. The presence of tetra-alkylammonium cations shifts the electrocatalytic potential for CO2 reduction. Cyclic voltammetry, infrared spectroelectrochemistry, and theoretical calculations were used to analyze the electrochemical mechanisms in different solvents and in the presence of weak acids.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Ruben Ramirez Grau, Anna Lewandowska-Andralojc, Ana Primo, Hermenegildo Garcia
Summary: The Nb2C sample obtained by chemical etching and 4-hour sonication showed the highest hydrogen generation rate due to its high specific surface area. The improved performance of this sample can be attributed to the influence of the exposed surface area and level of exfoliation of the MXene sheets.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Samuel R. Bottum, Taylor S. Teitsworth, Qi Han, Andre D. Orr, Jin-Sung Park, Xiaofan Jia, Chiara Cappuccino, Bobby H. Layne, Nilay Hazari, Javier J. Concepcion, Carrie L. Donley, Dmitry E. Polyansky, Matthew R. Lockett, James F. Cahoon, David C. Grills
Summary: In situ mid-infrared spectroscopy is a powerful technique for understanding the mechanism of CO2 reduction catalysts, while hybrid photoelectrodes, composed of a semiconductor and a molecular catalyst, are promising for sunlight-driven catalysis. We developed a new strategy using ATR-IR spectroscopy coupled with electrochemistry to characterize catalysts directly integrated with a semiconductor surface under applied potential. This technique allows for the investigation of redox processes associated with CO2 reduction catalysts on Si electrode surfaces with high sensitivity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Dmitry E. Polyansky, Gerald F. Manbeck, Mehmed Z. Ertem
Summary: The formal reduction potentials of highly oxidizing and short-lived radical cations of substituted biphenyls generated in 1,2-dichloroethane (DCE) were measured using a redox equilibrium ladder method. The effect of halide ion-radical interactions on the reduction potentials of biphenyls was investigated, and it was found that the measured potentials saturated at high Hammett sigma values, indicating the influence of ion-pairing and hemicolligation interactions. This study provides a convenient way to manipulate the energetics of electron transfer involving organic redox species.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Xiaolei Hu, Grzegorz Szczepaniak, Anna Lewandowska-Andralojc, Jaepil Jeong, Bingda Li, Hironobu Murata, Rongguan Yin, Arman Moini Jazani, Subha R. Das, Krzysztof Matyjaszewski
Summary: This article introduces the first example of fully oxygen-tolerant red/NIR-light-mediated photoinduced atom transfer radical polymerization under biologically relevant conditions, using commercially available methylene blue as the catalyst. The method exhibits excellent oxygen tolerance and enables high-throughput synthesis of well-defined polymers and DNA-polymer bioconjugates in a short time.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Sergey Yu. Ketkov, Sheng-Yuan Tzeng, Elena A. Rychagova, Anton N. Lukoyanov, Wen-Bih Tzeng
Summary: Metallocenes, including methylcobaltocene, play important roles in various fields of chemistry. The ionization energy and vibrational structure of (Cp ')(Cp)Co can be influenced by introducing methyl substituents. The mass-analyzed threshold ionization spectrum and DFT calculations provide accurate information about the properties and transformations of (Cp ')(Cp)Co.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Review
Chemistry, Physical
Qifeng Mu, Jian Hu
Summary: Polymer mechanochemistry has experienced a renaissance due to the rapid development of mechanophores and principles governing mechanochemical transduction or material strengthening. It has not only provided fundamental guidelines for converting mechanical energy into chemical output, but also found applications in engineering and smart devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Da Hye Yang, Francesco Ricci, Fredrik L. Nordstrom, Na Li
Summary: Through systematic evaluation of the oiling-out behavior of procaine, we identified both stable and metastable liquid-liquid phase separation, and established phase diagrams to assist in rational selection of crystallization strategies.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Vikki Anand Varma, Simmie Jaglan, Mohd Yasir Khan, Sujin B. Babu
Summary: Designing engineering structures like nanocages, shells, and containers through self-assembly of colloids is a challenging problem. This work proposes a simple model for the subunit, which leads to the formation of monodispersed spherical cages or containers. The model with only one control parameter can be used to design cages with the desired radius.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Hainan Jiang, Yaolong He, Xiaolin Li, Zhiyao Jin, Huijie Yu, Dawei Li
Summary: The cycling lifespan and coulombic efficiency of lithium-ion batteries are crucial for high C-rate applications. The Li-ion concentration plays a crucial role in determining the mechanical integrity and structural stability of electrodes. This study focuses on graphite as the working electrode and establishes an experimental system to investigate the mechanical properties of composite graphite electrode at different C-rates. Considering the effect of Li-ion concentration in stress analysis is found to be significant.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Zhiye Wang, Yunchuan Li, Mingjun Sun
Summary: This study investigates the influence of intramolecular pi-pi interactions on the electronic transport capabilities of molecules. By designing and analyzing three pi-conjugated molecules, the researchers observe that different pi-conjugated structures have varying effects on electron transport. The findings provide a theoretical foundation for designing single-molecule electronic devices with multiple electron channels based on intramolecular pi-pi interactions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Yuandong Xu, Haoyang Feng, Chaoyang Dong, Yuqing Yang, Meng Zhou, Yajun Wei, Hui Guo, Yaqing Wei, Jishan Su, Yingying Ben, Xia Zhang
Summary: Hollow MoS2 cubes and spheres were successfully synthesized using a one-step hydrothermal method with the hard template method. The hollow MoS2 cubes exhibited higher specific capacitance and energy density compared to the hollow MoS2 spheres. The symmetrical supercapacitors assembled with these hollow structures showed good performance and high capacity retention after multiple cycles. These findings suggest that controlling the pore structure and surface characteristics of MoS2 is crucial for enhancing its electrochemical properties.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Ainhoa Oliden-Sanchez, Rebeca Sola-Llano, Joaquin Perez-Pariente, Luis Gomez-Hortiguela, Virginia Martinez-Martinez
Summary: The combination of photoactive molecules and inorganic structures is important for the development of advanced materials in optics. In this study, bulky dyes were successfully encapsulated in a zeolitic framework, resulting in emission throughout the visible spectrum.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Miaomiao Zhang, Cunyuan Pei, Qiqi Xiang, Lintao Liu, Zhongxu Dai, Huijuan Ma, Shibing Ni
Summary: The design of a solid electrolyte interphase (SEI) plays a crucial role in improving the electrochemical performance of anode materials. In this study, lithium difluoro(oxalate)borate (LiDFOB) is used as an electrolyte additive to form a protective SEI film on Li3VO4 (LVO) anodes. The addition of LiDFOB results in a dense, uniform, stable, and LiF-richer SEI, which enhances the Li-ion storage kinetics. The generated SEI also prevents further decomposition of the electrolyte and maintains the morphology of LVO anodes during charge/discharge processes. This work demonstrates the effectiveness of LiDFOB as a multi-functional additive for LiPF6 electrolytes and provides insights into SEI construction for high-performance LVO anodes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
B. V. Andryushechkin, T. V. Pavlova, V. M. Shevlyuga
Summary: The atomic structure of the Ag(111)-p(4 x 4)-O phase was reexamined and two phases with the same periodicity were discovered. It was demonstrated that the accepted Ag6 model is incompatible with high-resolution oxygen-sensitive STM images.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
S. L. Romo-Avila, D. Marquez-Ruiz, R. A. Guirado-Lopez
Summary: In this study, we used density functional theory (DFT) calculations to investigate the interaction between model graphene oxide (GO) nanostructures and chlorine monoxide ClO. We aimed to understand the role of this highly oxidizing species in breaking C-C bonds and forming significant holes on GO sheets. Our results showed that C-C bonds in a single graphene oxide sheet can be broken through a simple mechanism involving the dissociation of two chemically attached ClO molecules. The formation of carbonyl groups and holes on the GO surface was also observed. This study provides important insights into the degradation of carbon nanotubes and the stability of GO during the myeloperoxidase (MPO) catalytic cycle.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Alberto Garcia-Fernandez, Birgit Kammlander, Stefania Riva, Hakan Rensmo, Ute B. Cappel
Summary: In this study, the X-ray stability of five different lead halide perovskite compositions (MAPbI3, MAPbCl3, MAPbBr3, FAPbBr3, CsPbBr3) was investigated using photoelectron spectroscopy. Different degradation mechanisms and resistance to X-ray were observed depending on the crystal composition. Overall, perovskite compositions based on the MA+ cation were found to be less stable than those based on FA+ or Cs+. Metallic lead formation was most easily observed in the chloride perovskite, followed by bromide, and very little in MAPbI3. Multiple degradation processes were identified for the bromide compositions, including ion migration, formation of volatile and solid products, as well as metallic lead. CsBr was formed as a solid degradation product on the surface of CsPbBr3.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Timofei Rostilov, Vadim Ziborov, Alexander Dolgoborodov, Mikhail Kuskov
Summary: The shock-loading behavior of nanomaterials is investigated in this study. It is found that shock compaction waves exhibit a distinct two-step structure, with the formation of faster precursor waves that travel ahead of the main compaction waves. The complexity of the shock Hugoniot curve of the tested nanomaterial is described, and the effect of initial porosity on the compressed states is demonstrated.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Alexey A. Markov, Mikhail V. Patrakeev
Summary: The stability of La1/3Sr2/3Fe1-xMnxO3-delta, a perovskite-type oxide, under reducing conditions is dependent on the manganese content. Increasing the manganese content leads to a decrease in stability. The behavior of iron and manganese in the oxide shows distinct differences, which can be attributed to the difference in the enthalpy of oxidation reactions. Additionally, the change in the La/Sr ratio affects the concentration of iron and manganese ions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Mosayeb Naseri, Shirin Amirian, Mehrdad Faraji, Mohammad Abdur Rashid, Maicon Pierre Lourenco, Venkataraman Thangadurai, D. R. Salahub
Summary: Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3, this study assessed the structural stability and investigated the electronic, optical, and thermoelectric properties of a group of two-dimensional perovskite-type materials called perovskenes. The findings revealed that these materials are wide bandgap semiconductors with potential application in UV shielding. Moreover, they exhibit better electrical and thermal conductivity at high temperatures, enabling efficient power generation in thermoelectric devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)