Voltammetric demonstration of thermally induced natural convection in aqueous solution

Literature Information

Publication Date 2019-04-25
DOI 10.1039/C9CP01913H
Impact Factor 3.676
Authors

Danlei Li, Christopher Batchelor-McAuley, Lifu Chen, Richard G. Compton


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Abstract

In electrochemical systems imperfect thermostating inevitably leads to the presence of bulk convective flows. As recognised by Nernst [Z. Phys. Chem., 1904, 52] damping of these bulk convective flows next to a solid surface, or at the electrode, leads to diffusional mass transport predominating locally. This work questions the exclusivity of diffusional transport and provides hitherto unexplored physical insights into how thermally induced flows in bulk solution can, on both macro- and microelectrodes, influence a voltammetric measurement. Imperfect thermostating results in flows in the bulk solution which are predicted and here expeimentally shown to be of the order of 100 μm s−1. Here we show that even in the absence of natural convective flows induced by the electrochemical reaction itself, this thermally induced bulk convection can significantly affect the voltammetric response. First, evaporative losses from an open electrochemical cell can be sufficient to produce convective flows that can alter the electrochemical response. Second, electrodes with various sizes and geometries have been investigated and experimental results evidence that the sensitivity of an electrode to these flows in bulk solution is to a large extent controlled by the size of the surrounding non-conductive supporting substrate used to insulate parts of the electrode.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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