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, 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
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, Physical
Yonggang Yang, Ruigang Zhang, Yang Liu, Xueli Jia, Qingqing Zhang, Yuanyuan He, Hongsheng Zhai, Yufang Liu
Summary: In this study, the fluorescence behavior of firefly luciferin analogues DHC and DHC-OH was theoretically analyzed. The results show that DHC and water molecules undergo intermolecular proton transfer and form an anion configuration, while DHC-OH forms an intramolecular hydrogen bond and induces intramolecular proton transfer. The fluorescence peaks of both compounds are consistent with the experimental results, confirming the accuracy of the study.
CHEMICAL PHYSICS LETTERS
(2022)
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, Physical
Joseph E. Schneider, John S. Anderson
Summary: This study demonstrates through density functional theory calculations that a decrease in the thermodynamic parameters of proton transfer can lead to transition state imbalance in a nonadiabatic framework. The results provide a theoretical model that reproduces experimental trends and reconciles predictions from semiclassical transition state theory. It also suggests the importance of basicity for uphill CPET reactions and the possibility of similar treatments for other nonadiabatic reactions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(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
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
Spectroscopy
Xiao Luo, Wei Shi, Yunfan Yang, Yuzhi Song, Yongqing Li
Summary: In their experiment, Song et al. successfully synthesized two novel molecules BtyC-1 and BtyC-2 and observed different fluorescence peaks in each molecule. By studying the excited state intramolecular proton transfer (ESIPT) mechanisms, they found that the differences in the photochemical and photophysical properties of BtyC-1 and BtyC-2 are mainly due to the variations in hydrogen bonding interactions in their excited states.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2021)
Article
Chemistry, Multidisciplinary
Niklas von Wolff, Marc Robert
Summary: Electron serves as the ultimate redox reagent for building and reshaping molecular structures. Understanding and controlling the parameters involved in dissociative electron transfer (DET) reactivity and its coupling with proton transfer are crucial for enhancing selectivity, kinetics, and energy efficiency in molecular chemistry. Various applications, such as photoredox catalysis, CO2 reduction, and alcohol oxidation, highlight the broad range of processes encompassed by DET pathways and demonstrate the importance of studying the driving force-rate relationships for future developments in energy efficient catalytic schemes in redox organic chemistry.
Article
Chemistry, Physical
Sara Gomez, Natalia Rojas-Valencia, Alejandro Toro-Labbe, Albeiro Restrepo
Summary: This article explores the critical and vanishing points of reaction force and their corresponding important coordinates along the intrinsic reaction coordinate. The reaction path is divided into three well-defined regions: reactants, transition state, and products. It is found that for nonsynchronous reactions, electron activity extends beyond the transition state into the reactants and products regions.
JOURNAL OF CHEMICAL PHYSICS
(2023)
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.
Review
Physics, Multidisciplinary
Yi-Han Cheng, Yu-Cheng Zhu, Xin-Zheng Li, Wei Fang
Summary: Proton transfer is a crucial process in hydrogen-bonded systems, especially for multiple protons. Recent experimental and theoretical studies of cyclic H-bonded systems have provided insights into the quantum tunneling phenomena.
Article
Optics
Narissa Kanlayakan, Nawee Kungwan
Summary: Excited-state intramolecular proton transfer (ESIPT) reactions and electronic properties of NH-type hydrogen bonding molecules (APBI, APBO, APBT, and APIP) and their derivatives have been theoretically investigated. It was found that the introduction of a strong electron withdrawing group can cause a slight blue-shift in the emission peak.
JOURNAL OF LUMINESCENCE
(2021)
Article
Multidisciplinary Sciences
Yu Sugo, Keisuke Saito, Hiroshi Ishikita
Summary: This study focuses on the electron and proton transfer process of the secondary quinone QB in photosynthetic reaction centers from purple bacteria, identifying PT pathways involving Grotthuss-like pre-PT H-bond network and low-barrier H-bond formation. The findings also reveal a water molecule chain connecting protonated Glu-L212 and deprotonated His-L190, serving as a pathway for reprotonation of His-L190.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Multidisciplinary
Karl J. Koebke, Victor Sosa Alfaro, Tyler B. J. Pinter, Aniruddha Deb, Nicolai Lehnert, Cedric Tard, James E. Penner-Hahn, Vincent L. Pecoraro
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Physical
Cyrille Costentin, Benoit Limoges, Marc Robert, Cedric Tard
Summary: This article pays tribute to Prof. Jean-Michel Saveant's contributions in the field of electrochemistry, highlighting his decisive role in establishing the foundation of molecular electrochemistry and his achievements in the field of molecular and biomolecular catalysis.
Article
Chemistry, Physical
Ruwen Wang, Etienne Boutin, Nicolas Barreau, Fabrice Odobel, Julien Bonin, Marc Robert
Summary: The challenge of converting CO2 into valuable compounds, such as fuels, using renewable energy sources and sustainable compounds is being addressed through artificial photosynthesis research. One promising approach involves solar-assisted electrochemical processes where electrons are supplied by a photovoltaic cell. A PV-EC system has been developed that can reduce CO2 to CO and then convert it to methanol with limited bias voltage. The efficiency of this CO2-to-CH3OH reaction is around 28% under ideal conditions.
Review
Chemistry, Inorganic & Nuclear
Alessandro Perazio, Grace Lowe, Roberto Gobetto, Julien Bonin, Marc Robert
Summary: This review focuses on recent advances in photocatalytic CO2 reduction using heterogenized molecular catalysts. It discusses the chemistry of attaching catalysts to different supports to produce hybrid materials and explores the impact on photocatalytic performance, as well as the potential future impact of these systems on solar fuels research.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Bing Ma, Matias Blanco, Laura Calvillo, Lingjing Chen, Gui Chen, Tai-Chu Lau, Goran Drazic, Julien Bonin, Marc Robert, Gaetano Granozzi
Summary: The cobalt quaterpyridine complexes covalently linked to graphene surfaces with carboxylic acid groups showed high activity and exceptional stability in visible-light-driven CO2 catalytic conversion, with the ability to control product selectivity without compromising efficiency.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Multidisciplinary Sciences
Marine Elmaalouf, Mateusz Odziomek, Silvia Duran, Maxime Gayrard, Mounib Bahri, Cedric Tard, Andrea Zitolo, Benedikt Lassalle-Kaiser, Jean-Yves Piquemal, Ovidiu Ersen, Cedric Boissiere, Clement Sanchez, Marion Giraud, Marco Faustini, Jennifer Peron
Summary: The study demonstrates that short-range ordering is the key factor driving activity independently of the initial oxidation state and composition of the calcined iridium oxides. By producing iridium-based mixed oxides, the electronic processes can be decoupled from the structural transformation, allowing for higher electrochemical activity.
NATURE COMMUNICATIONS
(2021)
Article
Electrochemistry
Silvia Duran, Marine Elmaalouf, Mateusz Odziomek, Jean-Yves Piquemal, Marco Faustini, Marion Giraud, Jennifer Peron, Cedric Tard
Summary: ECSA is a critical property to describe, analyze and compare electrocatalysts, and Hg-UPD method can be used to estimate ECSA for ultraporous electrocatalysts with excellent reproducibility. The method shows promise for stability and degradation monitoring of electrocatalysts.
Review
Chemistry, Multidisciplinary
Sara Navarro-Jaen, Mirella Virginie, Julien Bonin, Marc Robert, Robert Wojcieszak, Andrei Y. Khodakov
Summary: This review compares different pathways for CO2 reduction to methanol and discusses the advantages and drawbacks of various catalysts, concluding that heterogeneous hydrogenation catalysis and electrocatalysis show the most promise for large-scale methanol synthesis from CO2.
NATURE REVIEWS CHEMISTRY
(2021)
Article
Chemistry, Physical
Martin Kientz, Grace Lowe, Blaine G. McCarthy, Garret M. Miyake, Julien Bonin, Marc Robert
Summary: We have evaluated six phenoxazine derivatives as visible light photosensitizers for the photochemical reduction of CO2 to CO with an iron porphyrin catalyst in organic media. The phenoxazine core was functionalized with electron-donating or -withdrawing groups to modify the photophysical properties. Our observation shows that there is no correlation between the production of CO and the excited state potential of the phenoxazine, but a clear correlation can be made between the oxidation potentials of the phenoxazine and the production of CO. This indicates that the process was limited by photosensitizer regeneration and that electron transfers not directly related to the catalyst activation could play a key role in homogeneous photocatalytic systems.
Article
Energy & Fuels
Ifan E. L. Stephens, Karen Chan, Alexander Bagger, Shannon W. Boettcher, Julien Bonin, Etienne Boutin, Aya K. Buckley, Raffaella Buonsanti, Etosha R. Cave, Xiaoxia Chang, See Wee Chee, Alisson H. M. da Silva, Phil de Luna, Oliver Einsle, Balazs Endrodi, Maria Escudero-Escribano, Jorge V. Ferreira de Araujo, Marta C. Figueiredo, Christopher Hahn, Kentaro U. Hansen, Sophia Haussener, Sara Hunegnaw, Ziyang Huo, Yun Jeong Hwang, Csaba Janaky, Buddhinie S. Jayathilake, Feng Jiao, Zarko P. Jovanov, Parisa Karimi, Marc T. M. Koper, Kendra P. Kuhl, Woong Hee Lee, Zhiqin Liang, Xuan Liu, Sichao Ma, Ming Ma, Hyung-Suk Oh, Marc Robert, Beatriz Roldan Cuenya, Jan Rossmeisl, Claudie Roy, Mary P. Ryan, Edward H. Sargent, Paula Sebastian-Pascual, Brian Seger, Ludmilla Steier, Peter Strasser, Ana Sofia Varela, Rafael E. Vos, Xue Wang, Bingjun Xu, Hossein Yadegari, Yuxiang Zhou
Summary: This article reviews recent progress in electrochemical CO2 reduction, discusses the challenges towards commercialization, and highlights opportunities for further research. The goal is to establish a low- or zero-emission carbon cycle.
JOURNAL OF PHYSICS-ENERGY
(2022)
Article
Energy & Fuels
Douglas Keller Jr, Vishal Somanna, Philippe Drobinski, Cedric Tard
Summary: This study examines the optimal locations for a methanol island powered by solar or wind energy in the Mediterranean Sea, which can capture atmospheric CO2 through the ocean and combine it with hydrogen gas to produce synthetic fuel. The simulation results show that the Alboran, Cretan, and Levantine Sea are the most suitable locations due to their availability of solar and wind power, while also avoiding areas with higher environmental risks. Production tests at these locations demonstrated promising results with potential benefits for island communities in terms of energy resource diversification and independence. However, further investigation on the environmental impact of such systems is necessary.
Article
Chemistry, Multidisciplinary
Sean M. M. Treacy, Daniel R. R. Vaz, Syed Noman, Cedric Tard, Tomislav Rovis
Summary: gamma-Lactams, which are commonly found in small-molecule pharmaceuticals, can be used as precursors for highly substituted pyrrolidines. Previously, redox approaches to gamma-Lactam synthesis required additional electron withdrawing functionality and N-aryl substitution to promote electrophilicity and prevent undesired reactions. However, a new strategy using alpha-bromo imides and alpha-olefins enables the synthesis of monosubstituted protected gamma-Lactams in a formal [3 + 2] fashion, offering opportunities for further derivatization.
Article
Chemistry, Physical
Marcella Bonchio, Julien Bonin, Osamu Ishitani, Tong-Bu Lu, Takeshi Morikawa, Amanda J. Morris, Erwin Reisner, Debashrita Sarkar, Francesca M. Toma, Marc Robert
Summary: Visible-light-driven conversion of CO2 to fuels and valuable compounds has been highly active in recent years. However, these processes and catalytic systems are still in early stages of development, with fundamental mechanistic challenges needing to be addressed. Collaborative efforts are needed to explore various approaches and establish robust practices to advance our understanding of these necessary processes.
Article
Chemistry, Multidisciplinary
Marine Elmaalouf, Alexandre Da Silva, Silvia Duran, Cedric Tard, Miguel Comesana-Hermo, Sarra Gam-Derouich, Valerie Briois, Damien Alloyeau, Marion Giraud, Jean-Yves Piquemal, Jennifer Peron
Summary: Highly porous iridium oxide nanostructured cages were synthesized using cheap Cu2O cubes as templates via a water-based process at room temperature. The resulting IrO2 hierarchical porous structures exhibited outstanding activity after calcination and acid leaching.
Article
Chemistry, Physical
Srinivasulu Parshamoni, Cedric Viravaux, Marc Robert, Caroline Mellot-Draznieks, Gui Chen, Pierre Mialane, Anne Dolbecq, Julien Bonin
Summary: In this study, cobalt complexes were immobilized in two different metal-organic frameworks (MOFs) and characterized through solid state characterization techniques and density functional theory calculations. The resulting composite materials showed efficient and selective reduction of CO2 to CO under visible-light irradiation, with the favorable environment provided by the MOF scaffold.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)