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Cation Dependent Surface Charge Regulation in Gated Nanofluidic Devices.

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  • 1Department of Mechanical and Aerospace Engineering, The Ohio State University , Columbus, Ohio 43210, United States.

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Surface charge significantly impacts nanoscale electrolyte transport. Divalent ions like Ca2+ and Mg2+ strongly interact with surfaces, reducing charge and influencing ion flow in nanofluidic devices.

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Area of Science:

  • Nanoscale science
  • Physical chemistry
  • Surface science

Background:

  • Surface charge is a critical factor in aqueous electrolyte transport at the nanoscale.
  • This phenomenon is relevant in both engineered systems and biological processes like ion transport.

Purpose of the Study:

  • To investigate how surface charge density affects electrolyte transport in a gated nanofluidic channel.
  • To compare the transport behavior of monovalent and divalent electrolytes, as well as mixtures.

Main Methods:

  • Utilized a gated nanofluidic device with embedded electrodes to tune surface charge density.
  • Systematically studied the transport of potassium chloride (KCl), sodium chloride (NaCl), magnesium chloride (MgCl2), calcium chloride (CaCl2), and KCl + CaCl2 mixtures.
  • Employed nanochannel conductance measurements and numerical modeling.

Main Results:

  • Divalent cations (Ca2+, Mg2+) significantly reduced native surface charge density (up to 4-5 times) compared to monovalent cations.
  • In electrolyte mixtures, Ca2+ dominated, making nanochannel conductance independent of KCl concentration.
  • Divalent ion-surface interactions limited the gate electrode's ability to modulate surface potential.

Conclusions:

  • Cation-dependent interactions dictate nanoscale ion transport in nanofluidic devices.
  • Surface charge modulation by external gates is influenced by specific ion-surface chemistries.
  • Understanding these interactions is crucial for controlling ion transport in nanochannels.