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, 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
Pooja J. Ayare, Noelle Watson, Maizie R. Helton, Matthew J. Warner, Tristan Dilbeck, Kenneth Hanson, Aaron K. Vannucci
Summary: This research demonstrates the photocatalytic synthesis of H2 using a multiphoton mechanism, where both a molecular photocatalyst and a substituted naphthol are excited in the presence of a sacrificial electron donor and proton source. The unique use of a naphthol molecule as both a light absorber and H2 producing catalyst offers a new paradigm for the production of solar fuels in uphill reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Shuanglin He, Fang Huang, Qianqian Wu, Ping Zhang, Ying Xiong, Jie Yang, Rong Zhang, Fang Wang, Lin Chen, T. Leo Liu, Fei Li
Summary: A rare mononuclear manganese complex was reported as a mimic of [FeFe]-hydrogenase, successfully mimicking the functions of its active site by utilizing two consecutive MS-CPET processes to achieve low overpotential in electrochemical hydrogen production.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Electrochemistry
Donald C. Janda, Kiran Barma, Niraja Kurapati, Oleksiy V. Klymenko, Alexander Oleinick, Irina Svir, Christian Amatore, Shigeru Amemiya
Summary: This study presents a theoretical framework for distinguishing the mechanisms of adsorption-coupled electron-transfer reactions. A common adsorption step model is proposed, and characteristic cyclic voltammetry shapes for different mechanisms during reversible adsorption are predicted. The model is validated through experimental analysis.
ELECTROCHIMICA ACTA
(2022)
Article
Chemistry, Physical
Rong-Zhen Liao, Jing-Xuan Zhang, Zhenyang Lin, Per E. M. Siegbahn
Summary: QM/MM calculations were used to investigate the reduction of acetylene to ethylene catalyzed by the DCCPCh enzyme with an [Fe8S9] double-cubane cluster. Various reaction pathways involving different oxidation states and protonation states were analyzed to find the most favorable one. The reaction proceeds via a special double-electron transfer induced proton transfer mechanism with the anti-ferromagnetically coupled [Fe8S8] cluster delivering electrons to the substrate.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Meng Huang, Xuanpeng Wang, Junjun Wang, Jiashen Meng, Xiong Liu, Qiu He, Lishan Geng, Qinyou An, Jinlong Yang, Liqiang Mai
Summary: In this study, it is found that proton co-insertion into tunnel materials is determined jointly by interface derivation and inner diffusion. The co-inserted/lattice H2O molecules block the Mg2+ diffusion while facilitate the proton diffusion. Through detailed investigations, it is demonstrated that protons dominate the subsequent insertion and inner diffusion, leading to excellent performances of the monoclinic vanadium dioxide (VO2(B)) anode in Mg(CH3COO)(2) aqueous solution.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Francesco Rigodanza, Nadia Marino, Alessandro Bonetto, Antonio Marcomini, Marcella Bonchio, Mirco Natali, Andrea Sartorel
Summary: The cobalt substituted polyoxotungstate Co6 displays fast electron transfer kinetics to photogenerated Ru-III(bpy)(3)(3+), significantly faster than cobalt oxide nanoparticles. Mechanistic evidence suggests that the oxidation and transformation processes of Co6 under different pH conditions involve specific Co(II) aquo and hydroxo groups, and proceed through bimolecular kinetics or concerted proton electron transfer (CPET) mechanisms.
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
Mirco Natali, Agnese Amati, Nicola Demitri, Elisabetta Iengo
Summary: Aromatic amino acids such as l-tyrosine and l-tryptophan play a role in mediating electron transfer reactions in natural systems. This study prepared and characterized two novel conjugates based on porphyrin chromophores and l-tryptophan as electron/proton donor. Photophysical investigation showed different quenching mechanisms operating upon visible-light excitation, highlighting the unique role of l-tryptophan in proton-coupled electron transfer.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Chen Qiao, Zahid Usman, Jie Wei, Lin Gan, Jianhua Hou, Yingying Hao, Youqi Zhu, Jiatao Zhang, Chuanbao Cao
Summary: A catalyst kinetics optimization strategy is proposed based on tuning active site intermediates adsorption. The construction of M-OOH on the catalytic site before the rate-determining step is crucial in this strategy, as it optimizes the overall catalytic kinetics by preventing competition from other intermediates. Through significantly reducing the kinetic energy barrier, M-OOH is formed on the active site at low overpotential, resulting in improved kinetics.
Article
Energy & Fuels
Fei Ai, Zengyue Wang, Nien-Chu Lai, Qingli Zou, Zhuojian Liang, Yi-Chun Lu
Summary: Researchers report a heteropoly acid electrolyte that enables high-performance aqueous redox flow batteries (ARFBs) at low temperatures, thanks to its exceptionally low freezing point and high conductivity. This electrolyte shows promise in achieving stable and high-power operation of ARFBs in cold climate conditions.
Article
Chemistry, Multidisciplinary
Yaming Hao, Yikun Kang, Shaoyan Wang, Zhe Chen, Can Lei, Xueting Cao, Lin Chen, Yefei Li, Zhipan Liu, Ming Gong
Summary: In this study, an electrode/electrolyte synergy strategy was developed to enhance both proton and electron transfers, resulting in efficient neutral water oxidation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Shicong Zhang, Xiaolin Zhao, Yifan Zhang, Yaoyao Zhao, Tao Li, Jianjun Liu, Fuqiang Huang, Tianquan Lin
Summary: By investigating the special energy storage mechanism of carbonyl materials in neutral electrolyte, we have discovered that the diffusion-free mechanism of water molecule adsorption and proton insertion by carbonyl groups can improve power density and energy density. Therefore, carbonyl materials have the potential to be the electrodes for low-cost and high-performance neutral aqueous batteries in the future.
JOURNAL OF POWER SOURCES
(2022)
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, 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.