Article
Chemistry, Multidisciplinary
Ambrose Ashwin Melvin, Bhavana Gupta, Kostiantyn Tieriekhov, Wojciech Nogala, Patrick Garrigue, Stephane Reculusa, Alexander Kuhn
Summary: An actuator controlled by light and electric field in a synergistic manner was reported, allowing for better control and a wider range of potential applications, especially in soft robotics. The actuator demonstrated reversible actuation in an aqueous solution through electrochemical reactions, leading to controlled motion based on logic gate operations. Such synergistic switching enables the development of original actuation schemes for complex mechanical tasks triggered by multiple stimuli.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Bhavana Gupta, Lin Zhang, Ambrose Ashwin Melvin, Bertrand Goudeau, Laurent Bouffier, Alexander Kuhn
Summary: The article introduces a design of an electromechanical system based on conducting polymers to drive a wireless microfluidic pump through asymmetric polarization induced by an electric field, eliminating the need for a physical connection to a power source. The performance of the electrochemically active soft pump can be fine-tuned by optimizing the material's wall thickness, length, and inner diameter, offering new opportunities for actuators in the field of fluidic or microfluidic devices.
Article
Biophysics
Serena Arnaboldi, Gerardo Salinas, Giorgia Bonetti, Roberto Cirilli, Tiziana Benincori, Alexander Kuhn
Summary: This study proposes a novel dynamic system for the recognition of chiral redox active molecules and measurement of enantiomeric excess. The approach is based on selective oxidation and asymmetric proton flux, and has been successfully used to measure enantiomeric ratios of different molecules.
BIOSENSORS & BIOELECTRONICS
(2022)
Article
Electrochemistry
Elena Villani, Naoki Shida, Shinsuke Inagi
Summary: In this study, electrochemiluminescence (ECL) was successfully generated from entirely pure conducting polymer films in alkaline aqueous solution, using PEDOT and PPy films prepared by constant current electrolysis as bipolar electrodes. ECL intensity profiles showed gradient emission on both materials, with different light-emitting regions. Imaging analysis allowed evaluation of ECL behavior of both CPs as a function of applied voltage and conductivity, showing potential applications in ECL and bipolar electrochemistry fields.
ELECTROCHIMICA ACTA
(2021)
Article
Chemistry, Multidisciplinary
Ian E. Jacobs, Yue Lin, Yuxuan Huang, Xinglong Ren, Dimitrios Simatos, Chen Chen, Dion Tjhe, Martin Statz, Lianglun Lai, Peter A. Finn, William G. Neal, Gabriele D'Avino, Vincent Lemaur, Simone Fratini, David Beljonne, Joseph Strzalka, Christian B. Nielsen, Stephen Barlow, Seth R. Marder, Iain McCulloch, Henning Sirringhaus
Summary: Molecular doping using redox-active small molecules as dopants for organic semiconductors has attracted increased research interest for various emerging applications. A recent breakthrough in ion-exchange based doping separates the redox and charge compensation steps, leading to high conductivity and ion exchange efficiencies in excess of 99%. Factors enabling high performance include the choice of solvent and increased doping strength, illustrating a connection between electrochemical doping and ion exchange while highlighting limitations in stability at high redox potential.
ADVANCED MATERIALS
(2022)
Article
Materials Science, Multidisciplinary
Chunyan Qin, Zhilian Yue, Xu-Feng Huang, Robert J. Forster, Gordon G. Wallace, Jun Chen
Summary: Utilizing organic conducting polymers for bipolar electrostimulation has enhanced communication with living cells, particularly in terms of cell differentiation. The new BPES system shows potential for clinical applications related to translational models of human mental disorders.
APPLIED MATERIALS TODAY
(2022)
Article
Chemistry, Multidisciplinary
Keiichi Imato, Taichi Hino, Naoki Kaneda, Ichiro Imae, Naoki Shida, Shinsuke Inagi, Yousuke Ooyama
Summary: This study reports on wireless electrochemical soft actuators composed of hydrogels, which demonstrate muscle-like shrinking and swelling at microscopic and even macroscopic scales.
Article
Chemistry, Multidisciplinary
Gerardo Salinas, Serena Arnaboldi, Patrick Garrigue, Alexander Kuhn
Summary: This work presents a method to generate localized resistance gradient patterns using the properties of polypyrrole and wireless polarization triggered by bipolar electrochemistry. The reduction and overoxidation of polypyrrole result in highly resistive regions at predefined positions, allowing for the fine-tuning of the spatial distribution of the electrochemical modification. Energy-dispersive X-ray spectroscopy analysis confirms the localized physicochemical modifications. This approach offers the advantages of wireless bipolar electrochemistry and precise control over pattern formation compared to conventional methods.
ADVANCED MATERIALS INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Miaoxia Liu, Gerardo Salinas, Jing Yu, Antoine Cornet, Haidong Li, Alexander Kuhn, Neso Sojic
Summary: Multimodal imaging is a powerful approach that integrates multiple optical modalities in a single device, with potential applications in various fields. In this study, we developed wireless multimodal light-emitting chemical systems by coupling two light sources based on different physical principles. The results provide a novel alternative for designing autonomous hybrid systems with multimodal and multicolor optical readouts for complex bio-chemical systems.
Article
Chemistry, Multidisciplinary
Miaoxia Liu, Gerardo Salinas, Jing Yu, Antoine Cornet, Haidong Li, Alexander Kuhn, Neso Sojic
Summary: In this study, we developed a wireless multimodal light-emitting chemical device by combining two light sources based on different physical principles. This device integrates optical imaging and electrochemical reactions, providing a novel approach for complex bio-chemical systems.
Article
Chemistry, Physical
Seyyed Mohsen Beladi-Mousavi, Gerardo Salinas, Nikolas Antonatos, Vlastimil Mazanek, Patrick Garrigue, Zdenek Sofer, Alexander Kuhn
Summary: Graphene has unique characteristics that make it appealing for energy-related applications, but generating functional graphene sheets is challenging. This study presents a novel approach based on bipolar electrochemistry to control the dispersibility and conductivity of graphene sheets, which can be used in organic battery and catalysis applications.
Article
Chemistry, Multidisciplinary
Jemin Jeon, Johannes Elbert, Ching-Hsiu Chung, Junice Chae, Xiao Su
Summary: Synthetic chiral platforms coupled with redox-mediated electrochemical processes can exhibit powerful enantioselective interactions. Chiral redox-metallopolymers, designed based on Ugi's amine-inspired chiral monomers, demonstrate enantioselective recognition of ionic enantiomers using electrochemical control. The supramolecular chirality resulting from intramolecular interactions enhances the recognition towards target enantiomers. The study highlights the potential of chiral redox-metallopolymers as platforms for electrochemically-modulated enantioselective interactions towards amino acids and pharmaceutical carboxylates.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Tianci Xu, Wenliang Ji, Yue Zhang, Xiaofang Wang, Nan Gao, Lanqun Mao, Meining Zhang
Summary: We have demonstrated a facile and general approach to achieve synergistic charge percolation in conducting polymers by incorporating carbon nanotubes and post-processing. This approach not only improves the electrochemical properties of the polymers but also enables selective electrochemical sensing and high-performance neurosensing.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Physical
Robert J. Forster
Summary: It is increasingly recognized that electron and ion transfer reactions, potentials, and electric fields generated in electrochemical experiments can influence biological systems in various ways. This review discusses recent studies on interfacing electrochemistry with living systems using wirefree, bipolar, or wireless strategies. The focus is on the application of biocompatible, electronically conducting polymers with optimized 2D and 3D structures in wire-free electrochemical systems, as well as the emerging role of 3D structured films and bipolar and feeder electrodes. The remaining challenges and prospects in the field of electroceuticals are also considered.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Chunhua Zhang, Huiting Zhang, Junying Pi, Lin Zhang, Alexander Kuhn
Summary: The study introduces a method for regenerating reduced NADH using electrocatalytically active modified microparticles in a bipolar electrochemical cell. The efficiency of the system can be fine-tuned by controlling the electric field and the number of dispersed microelectrodes, offering new possibilities for bioelectrocatalytic synthesis in the bulk phase.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Medicinal
Gerardo Salinas, Filippo Malacarne, Giorgia Bonetti, Roberto Cirilli, Tiziana Benincori, Serena Arnaboldi, Alexander Kuhn
Summary: A microfluidic valve based on chemically responsive materials is reported, which is triggered by bipolar electrochemistry and chiral recognition. The valve can be opened and closed by reversible deflection of a conducting polymer actuator, allowing the release of dye from a reservoir. The device works well even in the presence of chemically different chiral analytes in the same solution, opening up new possibilities in microfluidics, including controlled drug delivery applications.
Article
Electrochemistry
Gerardo Salinas, Angelica A. Villegas-Barron, Javier Tadeo-Leon, Bernardo A. Frontana-Uribe
Summary: N-substituted-2,5-dithienil-pyrroles have shown potential as a promising option for the synthesis of pi-conjugated polymers with excellent electrochromic properties. In this study, the chemical synthesis and electrochemical behavior of 4-(4-(2,5-di(thiophen-2-yl)-1H-pyrrol-1-yl)benzyl)aniline (TPTBA) were investigated. The obtained film was characterized using electrochemical and spectroelectrochemical techniques. The resulting polyTPTBA exhibited a quasi-symmetrical reversible redox system, which can be attributed to the cross-linking of the polymer backbone facilitated by the presence of the aniline moiety. Spectroelectrochemical studies demonstrated a moderate and rapid electrochromic transition between the discharged and charged states, with a switching time of 2 seconds between colors at 430 nm and 800 nm.
ELECTROCHIMICA ACTA
(2023)
Article
Chemistry, Multidisciplinary
Anne de Poulpiquet, Neso Sojic, Laurent Bouffier, Alexander Kuhn, Dodzi Zigah
Summary: Electrochemistry is an important topic taught in undergraduate chemistry programs, but students often find it difficult due to the combination of various physical concepts involved. Bipolar electrochemistry is of special interest for teaching purposes, as it has a simple setup and allows for the tuning of electrochemical reactions through manipulating the electric field. Basic experiments using a commercially available light emitting diode (LED) as a bipolar electrode are introduced here, illustrating the key parameters driving electrochemical reactions and providing an eye-catching introduction to general electrochemistry.
JOURNAL OF CHEMICAL EDUCATION
(2023)
Article
Chemistry, Physical
Gerardo Salinas, Cara Lozon, Alexander Kuhn
Summary: The theory of electromagnetism has played a crucial role in understanding physicochemical phenomena and remains relevant in various scientific fields. Magnetohydrodynamics (MHD), which uses electromagnetism to induce physical flux in a fluid containing ions, has been explored in electrochemistry to create chiral structures and overcome mass transport limitations. This review discusses the principles of MHD convection and recent unconventional approaches to integrating magnetic fields in electrochemical systems.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Gerardo Salinas, Serena Arnaboldi, Patrick Garrigue, Alexander Kuhn
Summary: This work presents a method to generate localized resistance gradient patterns using the properties of polypyrrole and wireless polarization triggered by bipolar electrochemistry. The reduction and overoxidation of polypyrrole result in highly resistive regions at predefined positions, allowing for the fine-tuning of the spatial distribution of the electrochemical modification. Energy-dispersive X-ray spectroscopy analysis confirms the localized physicochemical modifications. This approach offers the advantages of wireless bipolar electrochemistry and precise control over pattern formation compared to conventional methods.
ADVANCED MATERIALS INTERFACES
(2023)
Article
Chemistry, Organic
Fabio Buonsenso, Marta Colombo, Andrea Marchesi, Francesca Romana Mammone, Francesco Sannicolo, Roberto Cirilli, Marco Pierini
Summary: An experimental and theoretical study was conducted to analyze the configurational lability of drugs with a non-planar seven-membered cycloheptadiene ring, which confers chirality to these compounds. The study investigated the energy barrier opposing the inversion of the chiral tricyclic scaffold, which is dependent on appropriate substituents on the external cycles. Structural changes were made to accurately control the stereolability of the tricyclic framework, providing interesting insights.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Gerardo Salinas, Alexander Kuhn, Serena Arnaboldi
Summary: In this study, a simple and original self-propelled bimetallic Janus rotor was designed. The rotor is powered by the combination of a spontaneous electric and ionic current, generated by two coupled redox reactions, and a magnetic field placed orthogonal to the device surface. This design produces a magnetohydrodynamic vortex at each extremity of the rotor arm, generating an overall driving force for propulsion. The direction of the self-polarized object can be controlled by the direction of the electric current or the orientation of the external magnetic field, resulting in predictable motion.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Electrochemistry
Gerardo Salinas, Laurent Bouffier, Neso Sojic, Alexander Kuhn
Summary: Thermodynamics is an intriguing aspect of physical chemistry that is involved in various natural phenomena. The spontaneity of a chemical reaction is directly related to fundamental thermodynamic parameters such as the Gibbs free energy change. The visualization of electromotive force allows students to understand the underlying concepts of spontaneity in coupled reactions. This study introduces the thermodynamic concept of spontaneity to undergraduate students using the concepts of endogenous and exogenous bipolar electrochemistry. By encoding the chemical information of two coupled reactions through the light emission of a light-emitting diode used as a bipolar electrode, the thermodynamic information of the involved redox reactions can be directly read out.
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Ruchao Gao, S. Mohsen Beladi-Mousavi, Gerardo Salinas, Patrick Garrigue, Lin Zhang, Alexander Kuhn
Summary: Graphene monolayers can be postmodified with high precision by highly site-selective functionalization with platinum (Pt) clusters, resulting in catalytically active two-dimensional nanomaterials. The type and speed of motion of these materials can be controlled by controlling the deposition time and location of the Pt clusters.
Article
Multidisciplinary Sciences
Serena Arnaboldi, Gerardo Salinas, Sabrina Bichon, Sebastien Gounel, Nicolas Mano, Alexander Kuhn
Summary: This study introduces an autonomous bi-enzymatic system that utilizes the spontaneous oxidation and reduction of glucose and oxygen to trigger reversible motion. The system operates without the need for any external trigger, relying on the asymmetric uptake and release of ions on a conducting polymer strip that houses glucose oxidase and bilirubin oxidase enzymes. The time-asymmetric consumption of both fuels by the enzymatic reactions leads to the autonomous actuation of the device.
NATURE COMMUNICATIONS
(2023)
Article
Electrochemistry
Tommaso Nicolini, Bernardo A. Frontana-Uribe, Alexander Kuhn, Gerardo Salinas
Summary: Conducting polymers with tunable properties were synthesized by copolymerizing different aromatic monomers. The electrochemical, spectroscopic, and electrical properties of the copolymers were characterized, showing promising results for the development of stable, reversible, and fast-operating electrochromic devices.
Article
Materials Science, Multidisciplinary
Marcin Dabrowski, Stephane Reculusa, Damien Thuau, Cedric Ayela, Alexander Kuhn
Summary: This article presents a novel and cost-effective strategy for enhancing the sensing performance of cantilever-shaped, mass-sensitive sensors. The strategy involves introducing macroporosity in the recognition unit. The sensors developed using this strategy are successfully used for air humidity monitoring and chemical sensing.
ADVANCED MATERIALS TECHNOLOGIES
(2023)
Article
Chemistry, Physical
Gerardo Salinas, Serena Arnaboldi, Patrick Garrigue, Giorgia Bonetti, Roberto Cirilli, Tiziana Benincori, Alexander Kuhn
Summary: Chemistry on-the-fly is a concept that has been extensively studied in recent years for its potential in recognizing, quantifying, and converting chemical species in solution. This study proposes a promising approach for asymmetric synthesis using a combination of a magnetic field-enhanced self-electrophoretic propulsion mechanism and enantioselective redox chemistry. By employing Janus swimmers as redox-active elements, the conversion of a prochiral molecule into a specific enantiomer with high enantiomeric excess can be achieved spontaneously while the swimmers move. The magnetic field-enhanced self-mixing of the swimmers improves the reaction yield and conversion rate through the formation of local magnetohydrodynamic vortices.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Multidisciplinary
Thitapond Nulek, Serena Arnaboldi, Gerardo Salinas, Giorgia Bonetti, Roberto Cirilli, Tiziana Benincori, Chularat Wattanakit, Adrian E. E. Flood, Alexander Kuhn
Summary: Preferential crystallization induced by chiral surfaces is used to isolate enantiopure antipodes. In this study, inherently chiral oligomers are used for enantioselective crystallization of asparagine and glutamic acid, which have no structural correlation with the template. This approach shows versatility and has potential applications in the resolution of pharmaceutical compounds.
CHEMICAL COMMUNICATIONS
(2023)
