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Steric effects on AC electroosmosis in dilute electrolytes Brian D. Storey1, Lee R. Edwards1, Mustafa Sabri Kilic2, Martin Z. Bazant2 1Olin College of Engineering 2MIT Storey, Edwards, Kilic, Bazant PRE 2008 Bazant, Kilic, Storey, Ajdari, arXiv, 2007 Motivation – ICEO microfluidics • For engineers, ICEO operates at low voltage (portable microfluidics). • For electrokinetic theorists, ICEO operates at high voltage ~100 kT/e. • Current simulations of ICEO microfluidic devices rely on classical electrokinetic theory. • What’s complicated about ICEO? Large voltage, dynamics, long range flow patterns, complex geometry. • Can we develop a simple theory that can be implemented as boundary conditions in commercial finite element codes for predicting macro-scale flows? Bazant & Squires PRL & JFM2004 AC Electroosmosis Ramos, Morgan, Green, Castellenos 1998 Ajdari, PRE 2000 ACEO Pump Exp. data from Urbanski et al, MIT Classical electrokinetics i kT ln ci zi eci Chemical potential of dilute point ions: ci e Near a wall, steady state, 1D: Applied voltage =.025 V 3 z i e kT Applied voltage =0.75 V 20 10 2.5 10 10 1.5 C C 2 0 10 1 -10 10 0.5 0 0 Would need ions to be 0.01 angstrom -20 1 2 3 X 4 5 10 0 1 2 3 X 4 5 Bikerman (1942) ci i kT ln zi eci 1 ze @ equilibrium c e kT 1 c C, dimensionless, ν, volume fraction in bulk Kilic, Bazant, Ajdari – PRE 2007 Model applied to ACEO Linearized, DH Non-linear, GCS Bikerman model Flow contours – different ion size Theory and experiment Ion is 4 nm to best fit data. Exp. from Studer, Pepin, Chen, Ajdari Analyst 2004 Better steric models Carnahan Starling (2 nm) “volume effects can be underestimated significantly” using Bikerman model. (Biesheuvel & van Soestbergen, JCIS 2007). We can reduce to ~1 nm if we assume ε changes in double layer Concentration effects-ACEO experiments Urbanski et al. 2007 Studer et al, 2004 Concentration effects - simple model Electroosmotic mobility U s bE t Valid for any continuum model D b b d b 0 Simplest model of a viscoelectric effect b 1 c b (Bazant, Kilic, Storey, Ajdari 2007 arXiv) Viscoelectric model applied to ACEO x 10 -3 Velocity 2 1 0 Increasing concentration -1 -1 10 10 0 10 Frequency 1 10 2 Need an ion size of ~4 nm to fit forward flow data Lose the flow reversal when we combine models What’s missing? • Correlations effects. • Faradaic reactions (recall talk of Ramos et al on TWEO). • ….. What’s needed? • Experiments designed to study these effects. • Multi-scale modeling Conclusions • ICEO applications has opened new avenues for study in theoretical EK. • Crowding of ions, increased viscosity, and decreased permittivity are not new ideas (Bikerman, 1970). • Accounting for steric effects can effect qualitative and quantitative predictions in ACEO. • Still more work is needed for a truly useful theory based on first principles. Induced charge electroosmosis (ICEO) Bazant & Squires PRL & JFM2004 Theory & experiment Exp. from Studer, Pepin, Chen, Ajdari Analyst 2004 AC Electroosmosis *simulations account for EK through BC. Ramos, Morgan, Green, Castellenos 1998