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Precise Electrochemical Sizing of Individual Electro-Inactive Particles

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Field-effect based attomole titrations in nanoconfinement.

Rogier B H Veenhuis¹, Egbert J van der Wouden, Jan W van Nieuwkasteele

¹MESA+ Institute for Nanotechnology, Universiteit Twente, The Netherlands.

|December 22, 2009

Summary

This study introduces a new capacitive method for precise pH control in microfluidic and nanofluidic channels. The technique uses applied voltage to shift pH, enabling sensitive titrations in tiny volumes for bioassays.

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Area of Science:

Electrochemistry
Microfluidics
Nanofluidics

Background:

Controlling pH in micro- and nanofluidic systems is crucial for various applications, including bioassays and cell-based research.
Existing methods for pH manipulation in confined volumes can be limited by factors such as electrolysis and ionic strength compatibility.

Purpose of the Study:

To develop and demonstrate a novel capacitive method for actuating pH changes in micro- and nanofluidic channels.
To quantify the induced pH shifts and assess the method's linearity and applicability for titrations.

Main Methods:

A device utilizing two external metal gate electrodes separated by an insulating channel wall was employed.
Gate potentials were applied to induce proton release or uptake from silicon nitride surface groups, causing pH shifts.
Fluorescein was used as a fluorescent pH indicator to measure pH changes, with a maximum shift of 1.6 pH units observed.

Main Results:

A purely capacitive pH actuation mechanism was achieved, neglecting electrolysis due to a high-quality silicon nitride insulating layer.
A linear relationship was established between the applied gate potential and the change in fluorescein intensity, indicating voltage-controlled proton modulation.
The method successfully demonstrated the titration of 100 attomoles of TRIS in a 7 pL volume.

Conclusions:

This capacitive pH actuation method offers a "soft" and effective way to precisely control pH in small volumes, suitable for bioassays and cell-based research.
The technique operates effectively at physiological ionic strengths and in channels up to 1 micrometer in height, overcoming limitations of double-layer overlap-dependent methods.
The sensitivity of optical detection is the primary limitation for detecting smaller volumes or substances.