Article
Chemistry, Physical
Xinyang Li, Pengfei Huo
Summary: The ab initio RPMD approach was used to investigate tunneling-controlled reactions in methylhydroxycarbene, showing that nuclear tunneling effects can facilitate chemical reactions under low-temperature conditions, leading to the concept of tunneling-controlled chemical reactions as the third paradigm. The reaction kinetics of two competitive pathways were studied at various temperatures, with the obtained reaction rate constants matching well with experimental rates, demonstrating the feasibility of using ab initio RPMD rate calculations in realistic molecular systems for investigating reaction mechanisms dominated by quantum tunneling effects.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Review
Chemistry, Applied
Barakha Saxena, Roshan I. I. Patel, Anuj Sharma
Summary: Quaternary pyridinium compounds are widely used intermediates in organic synthesis and have gained popularity in the field. Traditional methods for transforming these compounds into C-C and C-X bonds require high temperatures, expensive catalysts, and specific conditions. However, researchers have sought alternative strategies that do not rely on transition metal or photocatalysis. Electron-donor-acceptor (EDA) complex reactions have emerged as an effective method, utilizing the electron-acceptor ability of quaternary pyridinium derivatives to generate radical intermediates without the need for photocatalysts. This review discusses the progress, mechanism, substrate scope, and limitations of EDA-complex mediated reactions involving quaternary pyridinium compounds.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Chemistry, Physical
Indra Narayan Chakraborty, Pradyut Roy, Pramod P. P. Pillai
Summary: The effectiveness of quantum dots (QDs) in photocatalyzing organic reactions is explored in this study. The use of QDs in efficiently catalyzing olefination reactions under visible-light irradiation at room temperature is demonstrated. Spectroscopic and electrochemical studies provide insights on the charge transfer mechanism involved in QD-photocatalyzed olefination.
Review
Chemistry, Physical
Dan Zhang, Xin Hui, Chunying Wu, Yunbo Zhu
Summary: Hydrogen evolution reactions, especially those combining hydrogen atom transfer (HAT) and metal-catalyzed hydrogen evolution (MCHE), have been shown to be a powerful and attractive strategy in organic synthesis for forming chemical bonds directly from available feedstocks. This review summarizes the current state of the art, highlighting mechanisms, synthetic applications, and offering insights into future developments in this area.
Article
Chemistry, Physical
Yangyi Lu, Dongping Zhong
Summary: This study provides the first exact solution to the time-independent Schrodinger equation of a model Hamiltonian for photo-induced electronic transfer reactions, offering a new direction for understanding vibronic effects in electron transfer dynamics.
Article
Chemistry, Physical
Xiaoliang Pan, Junjie Yang, Richard Van, Evgeny Epifanovsky, Junming Ho, Jing Huang, Jingzhi Pu, Ye Mei, Kwangho Nam, Yihan Shao
Summary: This study presents a protocol for machine-learning-assisted free energy simulation of solution-phase and enzyme reactions at the ab initio quantum-mechanical/molecular-mechanical (ai-QM/MM) level. The developed MLP and Delta MLP exhibit promising accuracy in reproducing energy and forces, offering a cost-effective alternative for studying enzymatic reactions.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Multidisciplinary
Tianhao Ma, He Huang, Yuling Liu, Yongjin Peng
Summary: The discovery of a simple and efficient detection method for biothiols and the theoretical insights into the fluorescence sensing mechanism of the probe provide inspiration for the development of highly convenient and efficient fluorescent probes for biothiol detection in vivo and in vitro.
FRONTIERS IN CHEMISTRY
(2023)
Review
Environmental Sciences
Laszlo Wojnarovits, Erzsebet Takacs
Summary: Chloride ions in natural waters, air at coastal regions, and wastewaters easily transform into chlorine containing radicals, impacting the degradation of organic molecules. The reaction of dichloride radical anion with organic molecules is suggested to occur via electron transfer mechanism.
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
(2021)
Article
Chemistry, Physical
Xiang Li, Yu Su, Zi-Hao Chen, Yao Wang, Rui-Xue Xu, Xiao Zheng, YiJing Yan
Summary: This study revisits the dissipaton equation of motion theory and introduces an equivalent dissipatons-embedded quantum master equation (DQME), which treats dissipatons as generalized Brownian particles. The DQME provides a direct approach to investigate the statistical characteristics of dissipatons and the underlying hybrid bath modes. Numerical demonstrations on an electron transfer model show the transient statistical properties of the solvation coordinate.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Sergey Doronin, Yury A. Budkov, Daniil M. Itkis
Summary: Based on the quantum-mechanical theory of electron transfer, a parameter was proposed to describe the electrochemical activity of doped graphenes, calculated using density of states and local density of state values obtained from density functional theory calculations, as well as reorganization energies of the redox system. The study showed that the proposed activity parameter correlates well with calculated ET rate constants, and the influence of doped elements on graphene activity follows a certain order in the oxygen reduction reaction.
Article
Biochemistry & Molecular Biology
Miriam Izzo, Silvio Osella, Margot Jacquet, Malgorzata Kiliszek, Ersan Harputlu, Alicja Starkowska, Anna Lasica, C. Gokhan Unlu, Tomasz Uspienski, Pawel Niewiadomski, Dariusz Bartosik, Bartosz Trzaskowski, Kasim Ocakoglu, Joanna Kargul
Summary: By rationally designing and optimizing the structure of bioelectrodes, the efficiency of direct electron transfer between graphene and cytochrome was significantly improved, leading to a substantial increase in cathodic photocurrent output. The tilted orientation was found to favor cathodic photocurrent generation, providing new possibilities for fine-tuning electronic communication within complex bio-organic nanostructures and interfaces.
BIOELECTROCHEMISTRY
(2021)
Article
Electrochemistry
Savisha Mahalingam, Abreeza Manap, Ramisha Rabeya, Kam Sheng Lau, Chin Hua Chia, Huda Abdullah, Nowshad Amin, Puvaneswaran Chelvanathan
Summary: The goal of this study is to investigate the impact of the chemical treatment of titanium tetrachloride (TiCl4) on graphene quantum dots (GQDs)-based dye-sensitized solar cells (DSSCs). The mechanism of how the TiCl4 treatment provides high surface area and porosity to enhance the adsorption of GQDs and dye is proposed. The electron transport analysis showed that the treatment reduced electron recombination rate and increased electron injection efficiency, resulting in improved performance of the DSSC.
ELECTROCHIMICA ACTA
(2023)
Article
Engineering, Environmental
Yonghyeon Lee, Jeehyeong Khim
Summary: The study revealed that the effects of electrolytes on the degradation of phenol by a photoelectrochemical cell are mainly reflected in interfacial parameters, kinetic constants, and quantum efficiency. The differences in anions may affect the decomposition of phenol due to different pathways of radical generation.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Multidisciplinary Sciences
Sindhana Pannir-Sivajothi, Jorge A. Campos-Gonzalez-Angulo, Luis A. Martinez-Martinez, Shubham Sinha, Joel Yuen-Zhou
Summary: The study focuses on molecules exhibiting laser-like phenomena at room temperature and investigates the impact of vibrational polariton condensate on chemical reactivity. It demonstrates the potential of using condensates to drive chemical reactions by bypassing the constraints of fast intramolecular vibrational redistribution typically seen in condensed phase environments.
NATURE COMMUNICATIONS
(2022)
Article
Optics
Yicheng Zhang, Lev Vidmar, Marcos Rigol
Summary: A new emergent eigenstate construction method is discussed, allowing the construction of new local Hamiltonians, of which one eigenstate captures the entire generalized thermalization process following a global quantum quench.
Article
Engineering, Environmental
Zhihao Chen, Xuchun Li, Shujuan Zhang, Jiyuan Jin, Xiaojie Song, Xiaomeng Wang, Paul G. Tratnyek
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2019)
Article
Chemistry, Multidisciplinary
Miranda J. Bradley, Paul G. Tratnyek
ACS EARTH AND SPACE CHEMISTRY
(2019)
Article
Engineering, Environmental
Chris M. D. Kocur, Dimin Fan, Paul G. Tratnyek, Richard L. Johnson
ENVIRONMENTAL SCIENCE & TECHNOLOGY LETTERS
(2020)
Article
Engineering, Environmental
Shichao Cai, Bo Chen, Xiaojiang Qiu, Jiamei Li, Paul G. Tratnyek, Feng He
Summary: Sulfidation of microscale ZVI using elemental sulfur as a reactant can achieve high efficiency in contaminant removal, with higher sulfidation efficiency compared to traditional sulfidation agents. The sulfidated mZVI has shown significantly enhanced reactivity and electron efficiency when reacting with trichloroethylene, making it a promising product for engineering applications.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Engineering, Environmental
Bingdang Wu, Shouyun Yu, Guoyang Zhang, Shujuan Zhang, Pengfei Shen, Paul G. Tratnyek
JOURNAL OF HAZARDOUS MATERIALS
(2020)
Article
Engineering, Environmental
Yidan Gao, Shifa Zhong, Tifany L. Torralba-Sanchez, Paul G. Tratnyek, Eric J. Weber, Yiling Chen, Huichun Zhang
Summary: This study developed predictive models for the abiotic reduction of 60 organic compounds using both conventional chemical descriptor-based and machine learning approaches, finding that the machine learning model provided similar prediction accuracy to conventional QSARs across all compound classes and conditions.
Article
Engineering, Environmental
Li Gong, Xiaojiang Qiu, Paul G. Tratnyek, Chengshuai Liu, Feng He
Summary: FeNX species can be the active sites for adsorption and activation of reactants in Fe single-atom catalysts. The combination of FeNX species with granular zero-valent iron (ZVI) can result in catalyzed reductive decontamination of groundwater contaminants. The newly developed N-C-mZV(Ibm) material showed higher dechlorination rates for trichloroethylene (TCE) than bare mZV(Ibm), especially at a wide range of pH values.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Review
Chemistry, Multidisciplinary
Jianzhi Huang, Adele Jones, T. David Waite, Yiling Chen, Xiaopeng Huang, Kevin M. Rosso, Andreas Kappler, Muammar Mansor, Paul G. Tratnyek, Huichun Zhang
Summary: This review focuses on the redox reactivity of four types of Fe(II) species and discusses their formation pathways, factors governing the reactivity, potential mechanisms, reactivity comparison, and characterization techniques. It also covers the roles of Fe(II) species in environmental applications and abiotic oxidation related processes in natural and engineered systems.
Article
Engineering, Environmental
Chengwu Zhang, Chuipeng Kong, Paul G. Tratnyek, Chuanyu Qin
Summary: In this study, the relationship between the Fe2+/TPP ratio and the degradation mechanism of p-nitrophenol (PNP) in Fe2+/O-2 systems under neutral conditions was investigated. It was found that the Fe2+/TPP ratio regulated the degradation pathways of PNP, with different reactive oxygen species (ROS) involved at different ratios. By controlling the Fe2+/TPP ratio, the oxidation/reduction removal of pollutants can be selectively achieved.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Eric J. Bylaska, Paul G. Tratnyek, Tifany L. Torralba-Sanchez, Kyle C. Edwards, David A. Dixon, Joseph J. Pignatello, Wenqing Xu
Summary: Hydrolysis of organic compounds can significantly affect their fate in the environment. This study investigated the alkaline hydrolysis mechanisms of TNT and DNAN using various computational methods. The results showed that for TNT, the most favorable hydrolysis steps involved Meisenheimer complex formation and proton abstraction. For DNAN, the most favorable hydrolysis reaction was a two-step process.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Engineering, Environmental
Li Gong, Jingting Chen, Yao Hu, Kai He, Eric J. Bylaska, Paul G. Tratnyek, Feng He
Summary: This study developed a method of simultaneous sulfidation and nitridation of zerovalent iron (ZVI) through mechanochemical ball milling, which improved the degradation of chloroform (CF). The composite material (S-N(C)-ZVI) exhibited synergistic effects of nitridation and sulfidation on CF degradation. Material characterizations showed that sulfidation and nitridation promoted the formation of Fe3O4 on the S-N(C)-ZVI particles.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Analytical
Han Cao, Ania S. Pavitt, Jeffrey M. Hudson, Paul G. Tratnyek, Wenqing Xu
Summary: This study uses square-wave voltammetry (SWV) and mediated chronoamperometry (MCA) to determine the electron-exchange capacity (EEC) of pyrogenic dissolved organic matter (pyDOM). SWV gives larger EEC values than MCA, making it suitable for measuring the EEC of natural organic matter and pyDOM.
ENVIRONMENTAL SCIENCE-PROCESSES & IMPACTS
(2023)
Article
Chemistry, Analytical
Ania S. Pavitt, Paul G. Tratnyek
ENVIRONMENTAL SCIENCE-PROCESSES & IMPACTS
(2019)
Article
Chemistry, Analytical
Tifany L. Torralba-Sanchez, Eric J. Bylaska, Alexandra J. Salter-Blanc, Douglas E. Meisenheimer, Molly A. Lyon, Paul G. Tratnyek
ENVIRONMENTAL SCIENCE-PROCESSES & IMPACTS
(2020)
Review
Chemistry, Analytical
Feng He, Li Gong, Dimin Fan, Paul G. G. Tratnyek, Gregory V. V. Lowry
ENVIRONMENTAL SCIENCE-PROCESSES & IMPACTS
(2020)