Real-time imaging of surface chemical reactions by electrochemical photothermal reflectance microscopy

Published on Feb 11, 2021in Chemical Science9.825
路 DOI :10.1039/D0SC05132B
Cheng Zong19
Estimated H-index: 19
(BU: Boston University),
Chi Zhang22
Estimated H-index: 22
(BU: Boston University)
+ 5 AuthorsJi-Xin Cheng84
Estimated H-index: 84
(BU: Boston University)
Sources
Abstract
Traditional electrochemical measurements based on either current or potential responses only present the average contribution of an entire electrode's surface. Here, we present an electrochemical photothermal reflectance microscope (EPRM) in which a potential-dependent nonlinear photothermal signal is exploited to map an electrochemical process with sub-micron spatial resolution. By using EPRM, we are able to monitor the photothermal signal of a Pt electrode during the electrochemical reaction at an imaging speed of 0.3 s per frame. The potential-dependent photothermal signal, which is sensitive to the free electron density, clearly revealed the evolution of surface species on the Pt surface. Our results agreed well with the reported spectroelectrochemical techniques under similar conditions but with a much faster imaging speed. We further mapped the potential oscillation during the oxidation of formic acid on the Pt surface. The photothermal images from the Pt electrode well matched the potential change. This technique opens new prospects for real-time imaging of surface chemical reaction to reveal the heterogeneity of electrochemical reactivity, which enables broad applications to the study of catalysis, energy storage, and light harvest systems.
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Great attention has been recently drawn to metal oxide electrocatalysts for electrocatalysis-based energy storage and conversion devices. To find the optimal electrocatalyst, a prerequisite is an activity metric that reasonably evaluates the intrinsic electrocatalytic activity of a particular catalyst. The intrinsic activity is commonly defined as the specific activity which is the current per unit catalyst surface area. Thus, the precise assessment of intrinsic activity highly depends on the re...
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Summary The oxidation of formic acid on single crystal platinum electrodes modified by a constant coverage of irreversibly adsorbed adatoms is described in this review. This subject has been studied for a wide period and the available information is huge. In consequence, we have selected the self-consistent set of results, which try to explain the nature of the electrocatalytic behavior of the adatoms and to point out the research details that should be addressed in the future. All the results h...
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Using a home-built reflectometer, we have investigated the changes in the optical reflectivity of a Pd(100) model catalyst during CO oxidation under high-pressure, high-temperature conditions. We observe changes in optical contrast when exposing the surface to CO oxidation conditions at 200 mbar from room temperature up to 400 掳C. These changes in reflectivity are a result both of the formation of a surface oxide layer and of a change in surface roughness because of gas exposure. However, the re...
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Chemical imaging with sufficient spatial resolution to resolve microparticles in tablets is essential to ensure high quality and efficacy in controlled release. The existing modalities have the following disadvantages: they are time-consuming or have poor spatial resolution or low chemical specificity. Here, we demonstrate an epi-detected mid-infrared photothermal (epi-MIP) microscope at a spatial resolution of 0.65 渭m. Providing identical spectral profiles as conventional infrared spectroscopy,...
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Despite its role in electrocatalysis and hydrogen generation, a complete understanding of the hydrogen evolution reaction on platinum remains elusive. Here, a detailed kinetic study of hydrogen adsorption and evolution on Pt(111) highlights the role of interfacial water reorganization in the hydrogen adsorption step.
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Scanning electrochemical microscopy (SECM) is an electroanalytical scanning probe technique capable of imaging substrate topography and local reactivity with high resolution. Since its inception in 1989, it has expanded into a wide variety of research areas including biology, corrosion, energy, kinetics, instrumental development, and surface modification. In the past 25 years, over 1800 peer-reviewed publications have focused on SECM, including several topical reviews. However, these reviews oft...
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A wide range of interfacial physicochemical processes, from electrochemistry to the functioning of living cells, involve spatially localized chemical fluxes that are associated with specific features of the interface. Scanning electrochemical probe microscopes (SEPMs) represent a powerful means of visualizing interfacial fluxes, and this Feature Article highlights recent developments that have radically advanced the speed, spatial resolution, functionality, and sensitivity of SEPMs. A major tren...
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Summary Photothermal microscopy enables detection of nanometer-sized objects solely based on their absorption. This technique allows efficient observation of various nano-objects in scattering media notably gold nanoparticles in cells. The extreme sensitivity of the method and the stability of the signals open numerous applications in spectroscopy, analytical chemistry and bioimaging. This review briefly describes the principle and the main characteristics of photothermal microscopy, with its ma...
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A theoretical model is herein proposed to account for changes in the normalized differential reflectance, 螖R/R, of well-defined single crystal Pt(111) surfaces|aqueous electrolyte interfaces. It assumes that 螖R/R is proportional to the area of the electrode either bare or covered by neutral and/or nominally charged species and, for a specific type of site, is modulated by the applied potential, E. Correlations between the coverage of the various species and E were obtained from data reported in ...
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#4Bo Zhang (UW: University of Washington)H-Index: 53
Abstract null null A dynamic partnership between optical imaging and electrochemistry has generated a myriad of new opportunities in which both fields are mutually beneficial for understanding the nanoscale electrochemical interfaces. An in-depth understanding of the heterogeneity of the interfaces is crucial for determining the performance of electrochemical devices, including energy-related systems. Based on classical optical microscopies, innovative methodologies and tools such as super resol...
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