Article
Electrochemistry
Jagadeeswari Sivanadanam, Raja Murugan, Harun Khan, Indrapal Singh Aidhen, Kothandaraman Ramanujam
Summary: This study explores the application of 2,5-bis((dimethylamino)methyl)benzene-1,4-diol and its derivatives as catholyte in aqueous redox flow batteries. The compound exhibits good solubility and stability in sulfuric acid solution, but its capacity gradually fades after cycling, possibly due to fast chemical reactions under acidic conditions.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Clorice R. Reinhardt, Elvira R. Sayfutyarova, Jiayun Zhong, Sharon Hammes-Schiffer
Summary: Ribonucleotide reductase (RNR) is an essential enzyme in DNA synthesis, with the active form of E. coli Ia RNR consisting of two subunits, alpha and beta, involved in a series of proton-coupled electron transfer (PCET) reactions. Quantum mechanical/molecular mechanical simulations suggest thermodynamically favored forward radical transfer in the pre-turnover state and backward radical transfer in the post-turnover state between Y731 and Y730. The simulations also propose that E623 plays a key role in influencing the directionality of PCET and predict the impact of mutation of E623 on catalysis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Yusuke Yoneda, S. Jimena Mora, James Shee, Brian L. Wadsworth, Eric A. Arsenault, Diptarka Hait, Gerdenis Kodis, Devens Gust, Gary F. Moore, Ana L. Moore, Martin Head-Gordon, Thomas A. Moore, Graham R. Fleming
Summary: This study investigates the photoinduced PCET dynamics of a biomimetic model system using various spectroscopic techniques and computational methods, providing insights into the complex dynamics and synergistic motions involved in the process. Specifically, the evolution of the 2DEV line shape, sensitive to the mixing of vibronic states, is interpreted through accurate computational modeling of the charge separated state, revealing a gradual change in electron density distribution associated with a dihedral twist occurring on a 120 fs time scale.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Electrochemistry
Jean-Francois Longevial, Iryna Knysh, Shaymaa Al Shehimy, Lhoussain Khrouz, Aramugam Pandurangan, Simon Pascal, Gabriel Canard, Christophe Bucher, Denis Jacquemin, Olivier Siri
Summary: Researchers have synthesized and characterized the soluble 6,13-dipivaloyl-5,14-dihydro-5,7,12,14-tetraazapentacene and its aromatic counterpart. Using complementary chemical, (spectro)-electrochemical, theoretical, and spectroscopic techniques, all the intermediates generated during the electrochemical processes of these compounds were fully characterized. The results demonstrate the ambipolar redox behavior of 6,13-dipivaloyl-5,14-dihydro-5,7,12,14-tetraazapentacene, leading to drastic color changes through proton-coupled electron transfer in a totally reversible fashion.
ELECTROCHIMICA ACTA
(2023)
Article
Chemistry, Multidisciplinary
Petra Walter, Olaf Hubner, Elisabeth Kaifer, Hans-Jorg Himmel
Summary: In this study, the PCET reactivity of a series of 1,4-bisguanidino-benzenes with varying redox potentials and proton affinities was evaluated and successfully applied in various oxidative aryl-aryl coupling reactions. The compounds were sorted based on their PCET reactivity through comparative experiments and quantum-chemical calculations, showcasing their potential as valuable alternatives to traditional high-potential benzoquinones in synthetic chemistry.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Multidisciplinary Sciences
Ye Tian, Jiani Hong, Duanyun Cao, Sifan You, Yizhi Song, Bowei Cheng, Zhichang Wang, Dong Guan, Xinmeng Liu, Zhengpu Zhao, Xin-Zheng Li, Li-Mei Xu, Jing Guo, Ji Chen, En-Ge Wang, Ying Jiang
Summary: The nature of hydrated proton on solid surfaces has been visualized using cryogenic qPlus-based atomic force microscopy. Eigen cations self-assemble into monolayer structures with local order, while Zundel cations form long-range ordered structures stabilized by nuclear quantum effects. It is found that Zundel configuration is preferred over Eigen on Pt(111), but such preference is absent on Au(111).
Article
Chemistry, Organic
Lena Steuer, Elisabeth Kaifer, Hans-Joerg Himmel
Summary: The first synthesis of redox-active dendrimer-like oligoguanidines was reported, which showed stable redox states and exhibited good performance in catalytic reactions.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Miji E. Joy, Anand Kumar Tripathi, Rubul Das, Rajan Maurya, Manoj Neergat
Summary: The research found that the actual resistance increased significantly with time and rotation speed on Nafion-containing glassy carbon electrodes, possibly due to the sulfonate group of the polymer attacking the redox couple. Internal and external mass transfer characteristics were better resolved compared to their inorganic counterparts.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Inorganic & Nuclear
Bo-Hong Luo, Ya-Jie Ren, Hai-Bin Cui, Qiang Fu, Hao-Dong Jiang, Huan-Fa Du, Qin Xie, Peng Li, Hua-Xin Zhang, Tian-Shun Wang
Summary: The aqua-coordinated oxo-bridged diruthenium(III) complex demonstrates electronic absorption properties, redox behavior, and catalytic capabilities for water oxidation reaction. The complex displays different visible absorption bands under different pH conditions and exhibits proton-coupled electron transfer behaviors at different pH values.
INORGANICA CHIMICA ACTA
(2021)
Article
Chemistry, Physical
Gabriela Hernandez-Padilla, Marisela Cruz-Ramirez, Juan Pablo F. Rebolledo-Chavez, Janet Ocampo-Hernandez, Angel Mendoza, Francisco J. Tenorio, Lenin Dominguez Ramirez, Luis Ortiz-Frade
Summary: This study investigates the redox mediation of glucose oxidase (GOD) with a series of Co(II) polypyridine complexes and Ferrocenecarboxylic acid, analyzing the molecular interactions and electron transfer process. The results suggest that the GOD-mediator interaction plays a crucial role in describing the electron transfer process, providing insights for potential bioelectronic applications.
JOURNAL OF MOLECULAR STRUCTURE
(2021)
Article
Chemistry, Multidisciplinary
Quinton J. Bruch, Akira Tanushi, Peter Muller, Alexander T. Radosevich
Summary: This study demonstrates that hydride transfer catalysis can be enabled by a transition metal-bound low symmetry tricoordinate phosphorus ligand. The reactivity of the phosphorus ligand enables catalytic hydrodechlorination, making it a significant finding in the field of catalysis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Analytical
Kwok Kiong Chan, Muhammad Shafique Bin Hamid, Richard D. Webster
Summary: The electrochemical study of the active ingredient in chili pepper, phenol capsaicin (CAPH), was conducted in dried and wet acetonitrile on a glassy carbon electrode. It was found that as water was added, hydrogen bonding interactions between water and phenolic groups caused the oxidation potentials to shift more negatively. Under wet conditions, the mechanism of the oxidation process involves a -2e(-)/-H+ oxidation, hydrolysis reaction, and loss of a methoxy group to form a 1,2-benzoquinone moiety.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Physical
Wencong Sun, Dong Yao, Yuehua Tai, Li Zhou, Wenxue Tian, Min Yang, Chunxiang Li
Summary: Polyoxometalates (POMs) can effectively catalyze the electrocatalytic CO2 reduction reaction (CO2RR) through multistep proton-coupled electron transfer (PCET) processes. In this study, a combination of commercial indium electrodes with Keggin-type POMs (PVnMo(12-n)O40)(n+3)- (n = 1, 2, 3) achieved a Faradaic efficiency toward ethanol of 93.4% at -0.3V (vs. RHE). The PCET processes in POMs activated CO2 molecules and caused the oxidation of the electrode, resulting in the loss of active sites. The addition of POM electrolyte additives regulated the interface microenvironment and improved CO2RR performance.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Review
Chemistry, Physical
Feng Zhu, Wenbin Zhang, Jiao Xun, Bi-Jun Geng, Qing-Man Liang, Yang Yang
Summary: This review focuses on the effects of proton donor/acceptor on several typical electrocatalytical reactions, including species, concentration, pKa, and steric hindrance. Specifically, the proton transfer pathway arising from ligand design strategy of molecular catalysts and modification of electrode-electrolyte interface is presented.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Nanoscience & Nanotechnology
Yuanfeng Gao, Qingyu Xue, Jiayuan Li, Mingkai Zhang, Yuanyuan Ma, Yongquan Qu
Summary: Coupling acid-electrolyte proton exchange membrane fuel cells with cathodic hydrogenation shows potential in energy and chemical industry. The use of phytate coordination on Cu surface enhances the kinetic of proton adsorption/activation and hydrogenation activity. This work provides a promising approach to integrate electricity generation and chemical production.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Han Li, Fei Xie, Ming-Tian Zhang
Summary: In this study, a strong hydrogen atom abstracting reagent was generated via an electrochemical method, which could catalyze water oxidation to produce H2O2 under metal-free conditions using a two-electron pathway.
Article
Fisheries
Jun Pan, Xing Zhang, Yunshan Zhang, Bingyu Yan, Kun Dai, Min Zhu, Zi Liang, Yaping Dai, Mingtian Zhang, Ziyao Zhang, Hanxue Zhu, Yuchao Gu, Manman Cao, Renyu Xue, Guangli Cao, Xiaolong Hu, Chengliang Gong
Summary: Our study identified 32 grass carp reovirus (GCRV)-derived circRNAs (vcircRNAs) in infected Ctenopharyngodon idellus kidney (CIK) cells, with most vcircRNAs derived from antisense strands of dsRNA segments. The expression levels of vcircRNAs increased following GCRV infection and competed with host or viral genes via miRNAs. Moreover, vcircRNAs transfected into cells caused significant apoptosis and suppressed GCRV gene expression, indicating a novel viral transcript that modulates gene regulation during viral infection.
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)
Review
Chemistry, Inorganic & Nuclear
Qi-Fa Chen, Yu-Hua Guo, Yi-Han Yu, Ming-Tian Zhang
Summary: Water oxidation is a crucial step in producing hydrogen using solar energy in artificial photosynthetic systems. Inspired by the oxygen evolution complex (OEC) in PSII, research has shifted towards non-precious metal catalysts, deepening our understanding of the mechanism of water oxidation.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Qi-Fa Chen, Ze-Yu Cheng, Rong-Zhen Liao, Ming-Tian Zhang
Summary: Researchers have developed a copper cluster inspired by multicopper oxidases, which shows remarkable catalytic reactivity towards water oxidation for efficient four-electron reduction of O-2 to water. This synthetic mimic demonstrates the effectiveness of cooperation between multiple metals in regulating O-O bond formation in water oxidation catalysis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Multidisciplinary Sciences
Ruipu Zhang, Runze Zhang, Ruijun Jian, Long Zhang, Ming-Tian Zhang, Yu Xia, Sanzhong Luo
Summary: In this study, the authors demonstrate that an open-shell semi-quinone anionic radical species, complexed with lanthanum, can act as a highly efficient aerobic oxidation catalyst under ambient conditions. This research is of great importance for organic synthesis and the chemical industry as it provides a sustainable and economic oxidation process.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Applied
Fei Xie, Ming-Tian Zhang
Summary: A binuclear complex was reported as a stable and efficient homogeneous catalyst for electrocatalytic water oxidation, operating via a one-site catalysis with two-sites oxidation mechanism. The O-O bond formation was found to occur by single-site water nucleophilic attack.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Qingqing Chen, Tengfang Long, Jie Zheng, Wangjian Sheng, Shuaishuai Sun, Wei Wei, Jing Zhao, Huan Wang
Summary: Chlorooxime derivatives are cysteine-specific peptide bioconjugation and stapling reagents that can generate stable thiohydroximate linkages, expanding the structural diversity of cyclic peptides.
Article
Chemistry, Multidisciplinary
Qi-Fa Chen, Yao Xiao, Rong-Zhen Liao, Ming-Tian Zhang
Summary: In this study, a molecular trinuclear nickel (TNC-Ni) catalyst for water oxidation was reported. The catalyst exhibited high catalytic performance and stability under neutral conditions (pH 7). The cooperation among the three nickel sites was found to play a vital role in charge accumulation and O-O bond formation.
Article
Chemistry, Multidisciplinary
Yu-Fan Wang, Ming-Tian Zhang
Summary: This study reports that the interaction between electron donor and proton donor can overcome the barrier of direct O2 activation via a concerted electron-proton transfer mechanism, providing a new strategy for developing direct PCET activation of nonpolar bonds.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Xianhao Zhang, Qi-Fa Chen, Jintao Deng, Xinyu Xu, Jirui Zhan, Hao-Yi Du, Zhengyou Yu, Meixian Li, Ming-Tian Zhang, Yuanhua Shao
Summary: This study directly observed and identified key intermediates during the water oxidation catalyzed by a cobalt-tetraamido macrocyclic ligand complex using a newly developed in situ electrochemical mass spectrometry method, which further confirmed the rationality of the mechanism.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Hong-Tao Zhang, Yu-Hua Guo, Yao Xiao, Hao-Yi Du, Ming-Tian Zhang
Summary: We reported here the development of a heterobimetallic NiFe molecular platform to investigate the synergistic effect of NiFe in water oxidation catalysis. Compared to homonuclear bimetallic compounds (NiNi and FeFe), the NiFe complex exhibited significant catalytic activity in water oxidation. Mechanistic studies showed that this enhanced activity is attributed to the effective promotion of O-O bond formation by NiFe synergy. The formation of Ni-III(mu-O)Fe-IV=O intermediate is the key step for O-O bond formation through intramolecular oxyl-oxo coupling between bridged O radical and terminal Fe-IV=O moiety.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Hong-Tao Zhang, Fei Xie, Yu-Hua Guo, Yao Xiao, Ming-Tian Zhang
Summary: We report the first nonheme CuFe oxygen reduction catalyst, which shows exceptional selectivity and turnover frequency in the reduction of oxygen to water. The collaborative efforts of copper and iron play a crucial role in achieving these outstanding catalytic properties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Applied
Jing Shi, Yu-Hua Guo, Fei Xie, Ming -Tian Zhang, Hong-Tao Zhang
Summary: The process of water oxidation is a challenging task in the development of artificial photosynthetic systems. The use of redox-active ligands in conjunction with metals has been recognized as an effective approach for managing this process. However, the detailed mechanisms of how the electronic effect of these ligands affects the reactivity of the catalytic centers are still unclear. In this study, the electronic effect of a series of mononuclear Ru complexes with redox-active ligands was investigated, and it was found that the ligand-centered oxidation plays a crucial role in the water oxidation process. This study provides important insights into the role of redox-active ligands in controlling the water oxidation process.
CHINESE JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Applied
Qifa Chen, Haoyi Du, Mingtian Zhang
Summary: Water oxidation is a key process in artificial photosynthesis, and transition metal-based catalysts have been widely used to study this mechanism. This study focuses on the redox properties of a Cu-III complex and its reactivity towards catalytic water oxidation, highlighting the importance of ligands and buffer solutions in the stability of water oxidation catalysts.
CHINESE JOURNAL OF CATALYSIS
(2021)
