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
Chemistry, Physical
Olaf Morawski, Pawel Gawrys, Jaroslaw Sadlo, Andrzej L. Sobolewski
Summary: Under violet light irradiation, HATN catalyzes hydrogenation reactions in various alcohols, producing hydrogenated species. Experimental findings are consistent with theoretical predictions, demonstrating the impact of the excited state of the HATN-solvent molecular complex on hydrogen transfer reactions.
Article
Chemistry, Multidisciplinary
Biswajit Mondal, Soumitra Dinda, Neeta Karjule, Sanjit Mondal, Alagar Raja Kottaichamy, Michael Volokh, Menny Shalom
Summary: Electrolysis of water is a sustainable method to produce clean hydrogen, but it requires a high applied potential due to the pH-dependency of the hydrogen and oxygen evolution reactions. By combining proton-coupled electron transfer and single-electron transfer processes, we have achieved hydrogen production from water at low cell potentials by pH adjustment.
Article
Multidisciplinary Sciences
Nathan M. Ennist, Zhenyu Zhao, Steven E. Stayrook, Bohdana M. Discher, P. Leslie Dutton, Christopher C. Moser
Summary: Natural photosynthetic protein complexes are complex and fragile, making reengineering efforts challenging. In this study, researchers developed a simplified artificial photosynthetic reaction center protein that can efficiently convert solar energy into fuel. The protein showed high stability, modular structure, and nanometer-scale photochemical charge separation, making it ideal for light-activated catalysis. This study demonstrates the potential of synthetic biology in creating genetically encoded, light-powered catalysts for solar fuel production.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Hunter B. Vibbert, Christoph Bendel, Jack R. Norton, Aaron J. Moment
Summary: Direct illumination of anthraquinones with light in air produces H2O2 reliably and robustly for aqueous, electrolyte-free, highly pure H2O2 production. The mechanism of this transformation involves proton-coupled electron transfer from an organic solvent to an anthraquinone catalyst.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Shimin Chen, Yan Ju, Hao Zhang, Yingbing Zou, Si Lin, Yunbin Li, Shuaiqi Wang, En Ma, Weihua Deng, Shengchang Xiang, Banglin Chen, Zhangjing Zhang
Summary: In this study, a donor-acceptor p-p stacking hydrogen-bonded organic framework (HOF-FJU-36) with coupled proton-electron transfer was designed. Irradiation with 405 nm light induced photogenerated radicals, leading to photoswitchable electron and proton conductivity. The mechanism of this switchable conductivity was demonstrated using various analytical techniques.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
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
Chemistry, Multidisciplinary
Astrid Nilsen-Moe, Andrea Rosichini, Starla D. Glover, Leif Hammarstrom
Summary: Research suggests that in a solvated environment, oxidation reactions of tryptophan exhibit weakly pH-dependent proton-coupled electron transfer, potentially related to a concerted electron-proton transfer mechanism. These conclusions are crucial for understanding CEPT in water and PCET-mediated radical reactions with solvent-exposed tryptophan in natural systems.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Tong Wu, Khashayar Rajabimoghadam, Ankita Puri, David D. Hebert, Yi Lin Qiu, Sidney Eichelberger, Maxime A. Siegler, Marcel Swart, Michael P. Hendrich, Isaac Garcia-Bosch
Summary: In this research article, a 4H(+)/4e(-) electron-coupled-proton buffer (ECPB) based on Cu and a redox-active ligand is described. The ECPB system catalyzes both the reduction of O-2 to H2O and the dehydrogenation of organic substrates. Mechanistic analysis reveals that fast disproportionation reactions maintain the ECPB equilibrium.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Applied
Wen Zhang, Cai-Cai Song, Jia-Wei Wang, Shu-Ting Cai, Meng-Yu Gao, You-Xiang Feng, Tong-Bu Lu
Summary: In this study, it is demonstrated that ss-cyclodextrin-decorated CdS nanocrystals can effectively anchor cobalt tetraphenyl porphyrin (CoTPP) catalysts and alcohol reductants, achieving high yields and selectivity in artificial photosynthesis.
CHINESE JOURNAL OF CATALYSIS
(2023)
Review
Chemistry, Inorganic & Nuclear
Akinobu Nakada, Takeshi Matsumoto, Ho-Chol Chang
Summary: The hybridization of functional ligands with metal atoms is a central issue in the design of reactions and catalysts based on metal complexes. Recent studies have shown that redox-active/non-innocent ligands can play various roles, such as spectators, moderators, electron/H+/0/- suppliers/poolers, cooperators, or actors, in reactions. This review highlights stoichiometric or catalytic reactions driven by substituted ethylenes and dithiolenes, as well as six-membered ligands like catecholato, benezendithiolato, aminophenolato, and o-phenelyenediamine derivatives. The chemically, electrochemically, and photochemically induced lability of these ligands is expected to provide a rich platform for useful bond-activation and bond-formation processes.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Shujiao Yang, Jinxiu Han, Wei Zhang
Summary: This article introduces the importance of proton-coupled electron transfer (PCET) in energy conversion and water splitting, and prospects the future development of PCET in reaction mechanisms and electrocatalyst design.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Robin Tyburski, Tianfei Liu, Starla D. Glover, Leif Hammarstrom
Summary: Proton-coupled electron transfer (PCET) reactions play a fundamental role in energy transformation reactions and are increasingly important in catalysis and synthetic chemistry. The interplay between proton and electron transfer leads to a richness of reactivity, with various sequential and concerted mechanisms. Understanding and distinguishing between different PCET mechanisms is crucial for the design and optimization of reactions utilizing PCET.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Yayong Sun, Jing Wei, Zhihua Fu, Minyi Zhang, Sangen Zhao, Gang Xu, Chunsen Li, Jian Zhang, Tianhua Zhou
Summary: A series of hydrogen-bonded organic frameworks (HOFs) with high stability and proton conductivity have been successfully developed based on the self-assembly of lipid bilayer membranes.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Applied
Hamid Ghorbani Shiraz, Mikhail Vagin, Tero-Petri Ruoko, Viktor Gueskine, Krzysztof Karon, Mieczyslaw Lapkowski, Tobias Abrahamsson, Thomas Ederth, Magnus Berggren, Xavier Crispin
Summary: Green hydrogen is considered a key clean energy carrier, and liquid organic hydrogen carriers (LOHCs) are explored as a low-cost and safe solution for hydrogen transport. Electrochemical hydrogen storage (EHS) using proton-coupled electron transfer (PCET) is investigated as a method to extract hydrogen from LOHCs. The study validates this concept through a model reaction.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Alexander M. Prophet, Kritanjan Polley, Gary J. Van Berkel, David T. Limmer, Kevin R. Wilson
Summary: The oxidation kinetics of iodide by ozone at the air-water interface is studied in single microdroplets. Molecular simulations and kinetic modeling are used to understand the underlying multiphase mechanism.
Article
Chemistry, Multidisciplinary
Rong Zhang, Jiajing Lan, Fei Wang, Shumei Chen, Jian Zhang
Summary: By utilizing 1,1'-ferrocene dicarboxylic acid as a chelating and surface protection ligand, we have synthesized multi-nuclear indium oxide clusters with varying nuclear sizes, including heptanuclear and thirteen-nuclear clusters. These clusters possess labile coordination sites, allowing for structural modification and self-assembly, resulting in the formation of various cluster structures.
Article
Chemistry, Multidisciplinary
Hui Wang, Hui Liu, Mingsen Wang, Jiaheng Hou, Yongjun Li, Yuancheng Wang, Yingjie Zhao
Summary: Two supramolecular complexes were prepared using CBs and M1, and their single-crystal structures were analyzed by SCXRD. The unexpected 1:2 self-assembly structure between M1 and CB[8] was discovered for the first time. These complexes exhibit unique photophysical properties and provide valuable information about the structure and photophysical properties of supramolecular complexes.
Article
Chemistry, Multidisciplinary
Chang-Hee Lee, Sookil Park, Sanggil Kim, Ji Young Hyun, Hyun Soo Lee, Injae Shin
Summary: The epidermal growth factor receptor (EGFR) is a cell-surface glycoprotein involved in cell proliferation and tumor development. This study used a fluorescently labeled EGFR to investigate its time-dependent endocytosis in live cells and found that appended glycans affect EGFR internalization. Additionally, the study detected sialic acid residues attached to EGFR on the live cell surface using FRET-based imaging. This research provides valuable insights into the cellular functions of EGFR.
Article
Chemistry, Multidisciplinary
Subhankar Sahu, Lokesh Kumar, Sumita Das, Dipti Gupta, Ruchi Anand
Summary: This study proposes a strategy that combines organic electronics with biosensor scaffolds to create a compact device for monitoring environmental aromatic pollution. By coupling biosensing protein MopR with an organic electrochemical transistor (OECT), a sensor module capable of efficient detection of phenol was designed. Exclusive phenol detection with minimal loss of sensitivity could be achieved in complex pollutant mixtures and real environmental samples.
Review
Chemistry, Multidisciplinary
Changseok Lee, Hyung-Joon Kang, Sungwoo Hong
Summary: The formation of C-N bonds through hydroamination reactions catalyzed by nickel hydrides has been a topic of recent interest. This approach offers a way to efficiently transform a variety of alkene and alkyne substrates into compounds enriched with C-N bonds. The review provides a concise overview of the underlying reaction mechanisms and aims to stimulate further progress in NiH-catalytic techniques and catalyst design.
Article
Chemistry, Multidisciplinary
Yueci Wu, Lu-Lu Sun, Hai-Hao Han, Xiao-Peng He, Weiguo Cao, Tony D. James
Summary: Drug-induced liver injury (DILI) is a common cause of acute liver failure in the USA and Europe, but most cases can be recovered or prevented by discontinuing the offending drug. Recent research has found that peroxynitrite (ONOO-) can be used as a potential indicator for early diagnosis of DILI, and there is an urgent need to establish a method to detect and track peroxynitrite in DILI cases. In this study, a FRET-based nano fluorescent probe CD-N-I was developed, which showed high selectivity and sensitivity in detecting peroxynitrite. The probe successfully detected exogenous peroxynitrite in live cells and endogenous peroxynitrite in APAP-induced liver injury of HepG2 cells.
Article
Chemistry, Multidisciplinary
Dmitry L. Lipilin, Mikhail O. Zubkov, Mikhail D. Kosobokov, Alexander D. Dilman
Summary: This article describes a direct photocatalytic method for the thiolation of unprotected acids, which was previously challenging. By using a thionocarbonate reagent with an N-O bond, the efficient conversion of carboxylic acids to thiols is achieved.
Article
Chemistry, Multidisciplinary
Jason Malenfant, Lucille Kuster, Yohann Gagne, Kouassi Signo, Maxime Denis, Sylvain Canesi, Mathieu Frenette
Summary: Raman microscopy can reveal compound-specific vibrational fingerprints without sample preparation. The combination of efficient theoretical calculations and a user-friendly software can accurately predict peak positions and provide match scores to assist with structure determination.
Article
Chemistry, Multidisciplinary
Jayoh A. Hernandez, Paul S. Micus, Sean Alec Lois Sunga, Luca Mazzei, Stefano Ciurli, Gabriele Meloni
Summary: Essential trace metals play crucial roles in the survival and virulence of bacterial pathogens. Helicobacter pylori requires nickel for colonization and persistence in the stomach, and NixA is an essential nickel transporter in this process. This study characterizes the selectivity and electrogenic nature of NixA-mediated nickel transport.
Article
Chemistry, Multidisciplinary
Tarali Devi, Kuheli Dutta, Jennifer Deutscher, Stefan Mebs, Uwe Kuhlmann, Michael Haumann, Beatrice Cula, Holger Dau, Peter Hildebrandt, Kallol Ray
Summary: This study emphasizes the importance of subtle electronic changes and secondary interactions in the stability of biologically relevant metal-dioxygen intermediates. It also shows that the role of the chloride ligand in stabilizing the Fe-III-(OOBu)-Bu-t moiety can extend to other anions, including the thiolate ligand.
Article
Chemistry, Multidisciplinary
Jacqueline R. Santhouse, Jeremy M. G. Leung, Lillian T. Chong, W. Seth Horne
Summary: By studying the folding kinetics and mechanism of the BdpA sequence, researchers found that altering the backbone connectivity can affect protein folding. This suggests that protein mimetic chains have a significant degree of plasticity in transitioning between unfolded and folded states.
Article
Chemistry, Multidisciplinary
Divanshu Gupta, Ralf Einholz, Holger F. Bettinger
Summary: This study presents the first direct spectroscopic evidence of a cyclic seven-membered iminoborane. Compared to linear amino-iminoboranes, this cyclic iminoborane exhibits weakened bond strength and lower Lewis acidity value. The study suggests that the reduced ring strain of cyclic iminoborane prevents nitrogen fixation but allows facile (2 + 2) cycloaddition reaction with C2H4.
Article
Chemistry, Multidisciplinary
Renny Mathew, Aniruddha Mazumder, Praveen Kumar, Julie Matula, Sharmarke Mohamed, Petr Brazda, Mahesh Hariharan, Brijith Thomas
Summary: This study reveals the packing arrangement of partially disordered nitro-perylenediimide (NO2-PDI) using a synergistic approach that combines 3D ED, ssNMR, and DFT techniques. By overcoming these challenges, this methodology opens up new avenues for material characterization, driving exciting advancements in the field.