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Quantification of the charge transport processes inside carbon nanopipettes† † Electronic supplementary information (ESI) available: TEM image of the prepared CNPs; calculation details of the solution resistance, and potential correction of the reference electrode. See DOI: 10.1039/d1sc04282c

ABSTRACT: Conductive nanopipettes have been extensively used as powerful multifunctional probes for electrochemical and ion transport measurements, while the involved charge transfer processes have not been fully explored. In this paper, we use both experimental and simulation methods to de-convolute and quantify the respective electron transfer (ET) and ion transport (IT) contributions to the resulting current signals in carbon nanopipettes (CNPs). The results present that the current signals in CNPs are determined by ET in the case of low solution depth and long timescales, while IT becomes dominant at short timescales or high solution depth. In addition, the electrochemically and chemically irreversible ET processes in CNPs were also quantified. The elucidated and quantified charge transport processes inside CNPs will help control and optimize the IT and ET processes at the nanoscale, promoting better and broad usage of conductive nanopipettes in single-entity sensing and imaging applications. The coupled electron transfer (ET) and ion transport (IT) processes in conductive nanopipettes, at both steady and transient states, are elucidated and quantified by experiments and simulation.

SUBMITTER: Liu R

PROVIDER: S-EPMC8597862 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Unveiling the contributions of electroosmotic flow (EOF) in the electrokinetic transport through structurally-defined nanoscale pores and channels is challenging but fundamentally significant because of the broad relevance of charge transport in energy conversion, desalination and analyte mixing, micro and nano-fluidics, single entity analysis, capillary electrophoresis etc. This report establishes a universal method to diagnose and deconvolute EOF in the nanoscale transport processes through current-potential measurements and analysis without simulation. By solving Poisson, Nernst-Planck (PNP) with and without Navier-Stokes (NS) equations, the impacts of EOF on the time-dependent ion transport through asymmetric nanopores are unequivocally revealed. A sigmoidal shape in the I-V curves indicate the EOF impacts which further deviate from the well-known non-linear rectified transport features. Two conductance signatures, an absolute change in conductance and a 'normalized' one relative to ion migration, are proposed as EOF impact (factor). The EOF impacts can be directly elucidated from current-potential experimental results from the two analytical parameters without simulation. The EOF impact is found more significant in intermediate ionic strength, and potential and pore size dependent. The less-intuitive ionic strength and size dependence is explained by the combined effects of electrostatic screening and non-homogeneous charge distribution/transport at nanoscale interface. The time-dependent conductivity and optical imaging experiments using single nanopipettes validate the proposed method which is applicable to other channel type nanodevices and membranes. The generalizable approach eliminates the need of simulation/fitting of specific experiments and offers previously inaccessible insights into the nanoscale EOF impacts under various experimental conditions for the improvement of separation, energy conversions, high spatial and temporal control in single entity sensing/manipulation, and other related applications.

Dataset Information

Quantification of the charge transport processes inside carbon nanopipettes† † Electronic supplementary information (ESI) available: TEM image of the prepared CNPs; calculation details of the solution resistance, and potential correction of the reference electrode. See DOI: 10.1039/d1sc04282c

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