Anion Transport through Lipids in a Hybrid Bilayer Membrane

Tse, Edmund C. M.; Barile, Christopher J.; Gewargis, John P.; Liu, Ying; Zimmerman, Steven C.; Gewirth, Andrew A.

doi:10.1021/ac5043544

Cited by 21 publications

(19 citation statements)

References 47 publications

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“…A less-explored alternative is to use a hybrid bilayer membrane (HBM), which consists of a self-assembled monolayer (SAM) covered by a monolayer of lipid (41). We previously utilized a HBM to assess anion permeability through lipids and to provide mechanistic insight into the unassisted anion transmembrane diffusion process (42). Using the HBM construct, we also demonstrated that O 2 reduction (O 2 þ 4H þ þ 4e -/ 2H 2 O) by CuBTT (CuBTT ¼ copper complex of 6-((3-(benzylamino)-1,2,4-triazol-5-yl)amino)hexane-1-thiol) is kinetically limited by proton transfer kinetics, suggesting that the rate-determining step (RDS) of O 2 reduction is the flip-flop diffusion of a proton carrier across the lipid membrane (43).…”

Section: Introductionmentioning

confidence: 99%

The Flip-Flop Diffusion Mechanism across Lipids in a Hybrid Bilayer Membrane

Barile

Tse

Liu

et al. 2016

Biophysical Journal

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In this study, we examine the mechanism of flip-flop diffusion of proton carriers across the lipid layer of a hybrid bilayer membrane (HBM). The HBM consists of a lipid monolayer appended on top of a self-assembled monolayer containing a Cu-based O2 reduction catalyst on a Au electrode. The flip-flop diffusion rates of the proton carriers dictate the kinetics of O2 reduction by the electrocatalyst. By varying both the tail lengths of the proton carriers and the lipids, we find the combinations of lengths that maximize the flip-flop diffusion rate. These experimental results combined with biophysical modeling studies allow us to propose a detailed mechanism for transmembrane flip-flop diffusion in HBM systems, which involves the bending of the alkyl tail of the proton carrier as the rate-determining step. Additional studies with an unbendable proton carrier further validate these mechanistic findings.

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Section: Introductionmentioning

confidence: 99%

The Flip-Flop Diffusion Mechanism across Lipids in a Hybrid Bilayer Membrane

Barile

Tse

Liu

et al. 2016

Biophysical Journal

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“…In this fashion, complex functions such as muscle contraction, neuronal signalling and metabolism are achieved. Membrane proteins are studied using patch clamps 8 , micropore arrays 9 and electrode-supported lipid bilayers 10 11 12 13 , and passive transmembrane ionic transport is controlled by local electrical and chemical potential gradients according to the Nernst–Planck equation 14 15 . While most common ions are Na + , K + and Cl − , proton (H + ) currents and concentration [ H + ] gradients play important physiological roles 16 .…”

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confidence: 99%

Electronic control of H+ current in a bioprotonic device with Gramicidin A and Alamethicin

et al. 2016

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In biological systems, intercellular communication is mediated by membrane proteins and ion channels that regulate traffic of ions and small molecules across cell membranes. A bioelectronic device with ion channels that control ionic flow across a supported lipid bilayer (SLB) should therefore be ideal for interfacing with biological systems. Here, we demonstrate a biotic–abiotic bioprotonic device with Pd contacts that regulates proton (H+) flow across an SLB incorporating the ion channels Gramicidin A (gA) and Alamethicin (ALM). We model the device characteristics using the Goldman–Hodgkin–Katz (GHK) solution to the Nernst–Planck equation for transport across the membrane. We derive the permeability for an SLB integrating gA and ALM and demonstrate pH control as a function of applied voltage and membrane permeability. This work opens the door to integrating more complex H+ channels at the Pd contact interface to produce responsive biotic–abiotic devices with increased functionality.

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“…This system was also found to be compatible with hexyl thioctate and thioctic acid tri(ethylene glycol) ester modified gold electrodes, which are capable of supporting HBMs and allow for more sensitive characterizations of pore forming toxins [72, 73]. Hydrophobic SAM modified electrodes covalently bound to a Cu(I)/Cu(II) redox center have recently been used to characterize anion transport through hybrid bilayer membranes, and show the transport to primarily follow a solubility-diffusion mechanism, rather than a pore mechanism [74]. In an alternative HBM approach, Ma et al developed a gold-attached SAM, terminated with an ubiquinone moiety, which was capable of tethering a lipid bilayer from the surface [75, 76].…”

Section: Lipid Membranes and Nanopore Signal Transductionmentioning

confidence: 99%

Bioinspired assemblies and plasmonic interfaces for electrochemical biosensing

Hinman

Cheng

2016

Journal of Electroanalytical Chemistry

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Electrochemical biosensing represents a collection of techniques that may be utilized for capture and detection of biomolecules in both simple and complex media. While the instrumentation and technological aspects play important roles in detection capabilities, the interfacial design aspects are of equal importance, and often, those inspired by nature produce the best results. This review highlights recent material designs, recognition schemes, and method developments as they relate to targeted electrochemical analysis for biological systems. This includes the design of electrodes functionalized with peptides, proteins, nucleic acids, and lipid membranes, along with nanoparticle mediated signal amplification mechanisms. The topic of hyphenated surface plasmon resonance assays is also discussed, as this technique may be performed concurrently with complementary and/or confirmatory measurements. Together, smart materials and experimental designs will continue to pave the way for complete biomolecular analyses of complex and technically challenging systems.

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Anion Transport through Lipids in a Hybrid Bilayer Membrane

Cited by 21 publications

References 47 publications

The Flip-Flop Diffusion Mechanism across Lipids in a Hybrid Bilayer Membrane

The Flip-Flop Diffusion Mechanism across Lipids in a Hybrid Bilayer Membrane

Electronic control of H+ current in a bioprotonic device with Gramicidin A and Alamethicin

Bioinspired assemblies and plasmonic interfaces for electrochemical biosensing

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