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Journal ArticleDOI

Highly spatial imaging of electrochemical activity on the wrinkles of graphene using all-solid scanning electrochemical cell microscopy

19 Aug 2021-
TL;DR: In this article, a solid PAM nanoball at the tip of a nanocapillary contacts graphene and behaves as an electrochemical cell for simultaneously measuring the morphology and electrochemical activity.
Abstract: Here, all-solid scanning electrochemical cell microscopy (SECCM) is first established by filling polyacrylamide (PAM) into nanocapillaries as a solid electrolyte. A solid PAM nanoball at the tip of a nanocapillary contacts graphene and behaves as an electrochemical cell for simultaneously measuring the morphology and electrochemical activity. Compared with liquid droplet-based SECCM, this solid nanoball is stable and does not leave any electrolyte at the contact regions, which permits accurate and continuous scanning of the surface without any intervals. Accordingly, the resolutions in the lateral (x-y) and vertical (z) directions are improved to ∼10 nm. The complete scanning of the wrinkles on graphene records low currents at the two sidewalls of the wrinkles and a relatively high current at the center of the wrinkles. The heterogeneity in the electrochemical activity of the wrinkle illustrates different electron transfer features on surfaces with varied curvatures, which is hardly observed by the current electrochemical or optical methods. The successful establishment of this high spatial electrochemical microscopy overcomes the current challenges in investigating the electrochemical activity of materials at the nanoscale, which is significant for a better understanding of electron transfer in materials.
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TL;DR: In this article , the authors present a high-throughput imaging technique for single-cell manipulation and measurement using SICM as an Electrochemical probe and demonstrate that it is a complementary technique to single-object electrochemistry.
Abstract: ACCESS Metrics & More Article Recommendations ■ CONTENTS High-Throughput Nanopores 320 Nanopore Working Principle 320 Arrayed Nanopore Configurations 321 Machine-Learning Assisted Nanopore Readout 321 Integration Modalities for Nanopores 321 Nanopore-Confined Electrochemistry 322 High-Throughput Scanning Ion Conductance Microscopy 324 From Nanopore to Nanoprobe 324 High-Throughput SICM 324 High-Throughput Imaging 325 High-Throughput Single-Cell Manipulation and Measurements 326 SICM as an Electrochemical Probe 326 Applications in Material Sciences 327 Applications in Life Sciences 328 High-Throughput Scanning Electrochemical Cell Microscopy 329 Technical and Theoretical Developments 329 Electrochemical Measurements and Characterization 331 Popular Redox Reactions and Electrode Materials 331 Corrosion 332 Phase Formation 332 Two-Dimensional Materials 333 Photoelectrochemistry 335 Electrocatalysis: Single Particles and PseudoSingle-Crystal Screening of Structure−Activity 336 Battery Electrode Materials 339 Optical Microscopies in Electrochemistry 339 Overview of Operational Principles 339 Operational Principles 339 Methodologies for Quantitative Image Analysis 340 Converting Local Optical Information into an Electrochemically Relevant Signal 340 Computing and Automatized Image Analysis 340 Imaging Single Events 340 A Complement to Single Nanoobject Electrochemistry 340 Electron Transfer 341 Probing Concentration Profiles 341 Conversion 341 Growth and Dissolution 342 Catalysis and Motion 342 Competing Processes 343 Electrochemistry versus Physical Transformation 343 Competing Electrochemical Reactions 344 One versus Many 344 Seeing Collective Behaviors 344 How to Access Missing Pieces of Information 344 Hyphenation with Local Complementary Information 345 Other Electrochemical and Electronic HighThroughput Imaging Techniques 345 Conclusion 346 Author Information 347 Corresponding Authors 347 Authors 347 Author Contributions 347 Notes 347 Biographies 347 Acknowledgments 348 List of Abbreviations Used 348 References 349

15 citations

Journal ArticleDOI
TL;DR: In this article , a single-cell scanning electrochemical cell microscopy (SECCM) strategy was proposed to improve the spatial resolution and utilize the potential-resolved current from the antibody-antigen complex to increase electrochemical imaging accuracy.
Abstract: The electrochemical visualization of proteins in the plasma membrane of single fixed cells was achieved with a spatial resolution of 160 nm using scanning electrochemical cell microscopy. The model protein, the carcinoembryonic antigen (CEA), is linked with a ruthenium complex (Ru(bpy)32+)-tagged antibody, which exhibits redox peaks in its cyclic voltammetry curves after a nanopipette tip contacts the cellular membrane. Based on the potential-resolved oxidation or reduction currents, an uneven distribution of membrane CEAs on the cells is electrochemically visualized, which could only be achieved previously using super-resolution optical microscopy. Compared with current electrochemical microscopy, the single-cell scanning electrochemical cell microscopy (SECCM) strategy not only improves the spatial resolution but also utilizes the potential-resolved current from the antibody-antigen complex to increase electrochemical imaging accuracy. Eventually, the electrochemical visualization of cellular proteins at the nanoscale enables the super-resolution study of cells to provide more biological information.
References
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Book
01 Jan 1980
TL;DR: In this paper, the authors present a comprehensive overview of electrode processes and their application in the field of chemical simulation, including potential sweep and potential sweep methods, coupled homogeneous chemical reactions, double-layer structure and adsorption.
Abstract: Major Symbols. Standard Abbreviations. Introduction and Overview of Electrode Processes. Potentials and Thermodynamics of Cells. Kinetics of Electrode Reactions. Mass Transfer by Migration and Diffusion. Basic Potential Step Methods. Potential Sweep Methods. Polarography and Pulse Voltammetry. Controlled--Current Techniques. Method Involving Forced Convention--Hydrodynamic Methods. Techniques Based on Concepts of Impedance. Bulk Electrolysis Methods. Electrode Reactions with Coupled Homogeneous Chemical Reactions. Double--Layer Structure and Adsorption. Electroactive Layers and Modified Electrodes. Electrochemical Instrumentation. Scanning Probe Techniques. Spectroelectrochemistry and Other Coupled Characterization Methods. Photoelectrochemistry and Electrogenerated Chemiluminescence. Appendix A: Mathematical Methods. Appendix B: Digital Simulations of Electrochemical Problems. Appendix C: Reference Tables. Index.

20,533 citations

Journal ArticleDOI
TL;DR: In this paper, the authors present a survey of electrochemical methods and their applications, focusing on the following categories: electrochemical water treatment methods, electrochemical method fundamentals and applications, and student solutions manual.
Abstract: Electroanalytical methods colorado state university. electrochemical methods fundamentals and applications. electrochemical methods fundamentals and applications. electrochemical methods fundamentals and applications. electrochemical methods student solutions manual. electrochemical methods fundamentals and applications. electrochemical methods fundamentals and applications. electrochemical methods student solutions manual. electrochemical methods fundamentals and applications. electrochemical methods fundamentals and applications. electrochemical methods fundamentals and applications. customer reviews electrochemical methods. electrochemical water treatment methods sciencedirect. electrochemical methods fundamentals and applications. electrochemical methods student solutions manual. electrochemical methods fundamentals and applications. electrochemical methods 2nd edition textbook solutions. electrochemical methods fundamentals and applications. electrochemical methods fundamentals and applications. electrochemical methods fundamentals and applications

5,804 citations

Journal ArticleDOI
TL;DR: In this paper, a review outlines the different mechanisms of wrinkle, ripple and crumple formation, and the interplay between wrinkles and ripples' attributes (wavelength/width, amplitude/height, length/size, and bending radius) and graphene's electronic properties and other mechanical, optical, surface, and chemical properties.

780 citations

Journal ArticleDOI
TL;DR: In situ/operando characterization techniques provide information on the structure evolution, redox mechanism, solid-electrolyte interphase (SEI) formation, side reactions, and Li-ion transport properties under operating conditions under realistic operation conditions.
Abstract: The increasing demands of energy storage require the significant improvement of current Li-ion battery electrode materials and the development of advanced electrode materials. Thus, it is necessary to gain an in-depth understanding of the reaction processes, degradation mechanism, and thermal decomposition mechanisms under realistic operation conditions. This understanding can be obtained by in situ/operando characterization techniques, which provide information on the structure evolution, redox mechanism, solid-electrolyte interphase (SEI) formation, side reactions, and Li-ion transport properties under operating conditions. Here, the recent developments in the in situ/operando techniques employed for the investigation of the structural stability, dynamic properties, chemical environment changes, and morphological evolution are described and summarized. The experimental approaches reviewed here include X-ray, electron, neutron, optical, and scanning probes. The experimental methods and operating principles, especially the in situ cell designs, are described in detail. Representative studies of the in situ/operando techniques are summarized, and finally the major current challenges and future opportunities are discussed. Several important battery challenges are likely to benefit from these in situ/operando techniques, including the inhomogeneous reactions of high-energy-density cathodes, the development of safe and reversible Li metal plating, and the development of stable SEI.

345 citations

Journal ArticleDOI
14 Dec 2020-Nature
TL;DR: In this paper, a local spectroscopic technique using a scanning tunnelling microscope was used to detect a sequence of topological insulators in magic-angle twisted bilayer graphene (MATBG) with Chern numbers C = ǫ±1, ±2 and ±3.
Abstract: Interactions between electrons and the topology of their energy bands can create unusual quantum phases of matter. Most topological electronic phases appear in systems with weak electron–electron interactions. The instances in which topological phases emerge only as a result of strong interactions are rare and mostly limited to those realized in intense magnetic fields1. The discovery of flat electronic bands with topological character in magic-angle twisted bilayer graphene (MATBG) has created a unique opportunity to search for strongly correlated topological phases2–9. Here we introduce a local spectroscopic technique using a scanning tunnelling microscope to detect a sequence of topological insulators in MATBG with Chern numbers C = ±1, ±2 and ±3, which form near filling factors of ±3, ±2 and ±1 electrons per moire unit cell, respectively, and are stabilized by modest magnetic fields. One of the phases detected here (C = +1) was previously observed when the sublattice symmetry of MATBG was intentionally broken by a hexagonal boron nitride substrate, with interactions having a secondary role9. We demonstrate that strong electron–electron interactions alone can produce not only the previously observed phase, but also other unexpected Chern insulating phases in MATBG. The full sequence of phases that we observe can be understood by postulating that strong correlations favour breaking time-reversal symmetry to form Chern insulators that are stabilized by weak magnetic fields. Our findings illustrate that many-body correlations can create topological phases in moire systems beyond those anticipated from weakly interacting models. Strong electron–electron interactions in magic-angle twisted bilayer graphene can fundamentally change the topology of the system’s flat bands, producing a hierarchy of strongly correlated topological insulators in modest magnetic fields.

237 citations