Alteration of Membrane Compositional Asymmetry by LiCoO<sub>2</sub> Nanosheets

Doğangün, Merve; Hang, Mimi N.; Troiano, Julianne M.; McGeachy, Alicia C.; Melby, Eric S.; Pedersen, Joel A.; Hamers, Robert J.; Geiger, Franz M.

doi:10.1021/acsnano.5b01440

Cited by 42 publications

(38 citation statements)

References 81 publications

(135 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In the C-H stretching region, Figure 2A shows what we had reported earlier for the C−H stretching region, namely peaks at ~2880 cm -1 , ~2900 cm -1 , and ~2950 cm -1 characteristic of lipids in a well-formed bilayer. 8,9,34 The peak at ~2880 cm -1 is attributable to the symmetric CH 3 stretches of the lipid alkyl tails while the SFG intensity of the other two peaks is due to spectral interference from the water molecules, as demonstrated recently using D 2 O 34 and Page 7 spectral lineshape modeling. 26 Adding PAH to the bilayer leads to SFG intensity decreases, indicating a clear perturbation in the lipid structure with the addition of the polycations.…”

Section: Iid Pah-membrane Interaction Experiments Following Bilayermentioning

confidence: 78%

Perturbation of Hydrogen Bonding Networks over Supported Lipid Bilayers by Poly (Allylamine Hydrochloride)

Dalchand

Doğangün

Ohno

et al. 2019

Preprint

View full text Add to dashboard Cite

<div><div><div><p>Water is vital to many biochemical processes and is necessary for driving many fundamental interactions of cell membranes with their external environments, yet it is difficult to probe the membrane/water interface directly and without the use of external labels. Here, we employ vibrational sum frequency generation (SFG) spectroscopy to understand the role of interfacial water molecules above bilayers formed from zwitterionic (phosphatidylcholine, PC) and anionic (phosphatidylglycerol, PG, and phosphatidylserine, PS) lipids as they are exposed to the common polycation poly (allylamine hydrochloride) (PAH) in 100 mM NaCl. We show that as the concentration of PAH is increased, the interfacial water molecules are irreversibly displaced and find that it requires 10 times more PAH to displace interfacial water molecules from membranes formed from purely zwitterionic lipids when compared to membranes that contain the anionic PG and PS lipids. This outcome is likely due to difference in (1) the energy with which water molecules are bound to the lipid headgroups, (2) the number of water molecules bound to the headgroups, which is related to the headgroup area, and (3) the electrostatic interactions between the PAH molecules and the negatively charged lipids that are favored when compared to the zwitterionic lipid headgroups. The findings presented here contribute to establishing causal relationships in nanotoxicology and to understanding, controlling, and predicting the initial steps that lead to the lysis of cells exposed to membrane disrupting polycations, or to transfection.</p></div></div></div>

show abstract

Section: Iid Pah-membrane Interaction Experiments Following Bilayermentioning

confidence: 78%

Perturbation of Hydrogen Bonding Networks over Supported Lipid Bilayers by Poly (Allylamine Hydrochloride)

Dalchand

Doğangün

Ohno

et al. 2019

Preprint

View full text Add to dashboard Cite

show abstract

“…Nanosheets of NMC and LCO were synthesized by adapting a previously reported method . Briefly, to make NMC, a LiNi 1/3 Mn 1/3 Co 1/3 (OH) 2 precursor was synthesized by adding an aqueous transition salt mixture containing 0.2 M Co(II) acetate, 0.2 M Ni(II) acetate, and 0.2 M Mn(II) acetate dropwise into 0.1 M aqueous LiOH under magnetic stirring.…”

Section: Methodsmentioning

confidence: 99%

“…Samples for SEM images were prepared by spin‐coating (1000 rpm) a dilute methanolic solution of either NMC or LiCoO 2 onto a pristine boron‐doped SiO 2 wafer. For transmission electron microscopy images of NMC and LCO, see Dogangun et al and Hang et al , respectively.…”

Section: Methodsmentioning

confidence: 99%

“…Only a few studies have highlighted the toxicological implications and mode of action of these nanoscale complex metal oxides. A prior study of LCO nanosheets and supported lipid bilayers showed that this material had the ability to alter synthetic bilayer compositional symmetry ; in bacteria, toxicity was the result of dissolution of Ni and Co ions . The impact of nanoscale LCO and NMC on multicellular organisms is largely unknown.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Core chemistry influences the toxicity of multicomponent metal oxide nanomaterials, lithium nickel manganese cobalt oxide, and lithium cobalt oxide to Daphnia magna

Bozich

Hang

Hamers

et al. 2017

Enviro Toxic and Chemistry

View full text Add to dashboard Cite

Lithium intercalation compounds such as lithium nickel manganese cobalt oxide (NMC) and lithium cobalt oxide (LCO) are used extensively in lithium batteries. Because there is currently little economic incentive for recycling, chances are greater that batteries will end up in landfills or waste in the environment. In addition, the toxicity of these battery materials traditionally has not been part of the design process. Therefore, to determine the environmental impact and the possibility of alternative battery materials, representative complex battery nanomaterials, LCO and NMC, were synthesized, and toxicity was assessed in Daphnia magna. Toxicity was determined by assessing LCO and NMC at concentrations in the range of 0.1 to 25 mg/L. Acute studies (48 h) showed no effect to daphnid survival at 25 mg/L, whereas chronic studies (21 d) show significant impacts to daphnid reproduction and survival at concentrations of 0.25 mg/L for LCO and 1.0 mg/L for NMC. Dissolved metal exposures showed no effect at the amounts measured in suspension, and supernatant controls could not reproduce the effects of the particles, indicating a nanomaterial-specific impact. Genes explored in the present study were actin, glutathione-s-transferase, catalase, 18s, metallothionein, heat shock protein, and vitellogenin. Down-regulation of genes important in metal detoxification, metabolism, and cell maintenance was observed in a dose-dependent manner. The results show that battery material chemical composition can be altered to minimize environmental impacts. Environ Toxicol Chem 2017;36:2493-2502. © 2017 SETAC.

show abstract

“…All SLBs were formed at 0.01 M Tris buffer and 0.1 M NaCl in the presence of 0.005 M CaCl 2 ·2H 2 O at pH 7.40 ± 0.03. 29 Following bilayer formation, SLBs were rinsed with Ca-free buffer to remove excess vesicles.…”

Section: Pagementioning

confidence: 99%

Hydrogen Bond Networks Near Supported Lipid Bilayers from Vibrational Sum Frequency Generation Experiments and Atomistic Simulations

Doğangün¹,

Ohno²,

Liang³

et al. 2018

Preprint

Self Cite

View full text Add to dashboard Cite

We report vibrational sum frequency generation (SFG) spectra in which the C-H stretches of lipid alkyl tails in fully hydrogenated single-and dual-component supported lipid bilayers are detected along with the O-H stretching continuum above the bilayer. As the salt concentration is increased from ~10 µM to 0.1 M, the SFG intensities in the O-H stretching region decrease by a factor of 2, consistent with significant absorptive-dispersive mixing between χ (2) and χ (3) contributions to the SFG signal generation process from charged interfaces.A method for estimating the surface potential from the second-order spectral lineshapes (in the OH stretching region) is presented and discussed in the context of choosing truly zero-potential reference states. Aided by atomistic simulations, we find that the strength and orientation distribution of the hydrogen bonds over the purely zwitterionic bilayers are largely invariant between sub-micromolar and hundreds of millimolar concentrations. However, specific Dogangun et al.Page 2 interactions between water molecules and lipid headgroups are observed upon replacing phosphocholine (PC) lipids with negatively charged phosphoglycerol (PG) lipids, which coincides with SFG signal intensity reductions in the 3100 cm -1 to 3200 cm -1 frequency region.The atomistic simulations show that this outcome is consistent with a small, albeit statistically significant, decrease in the number of water molecules adjacent to both the lipid phosphate and choline moieties per unit area, supporting the SFG observations. Ultimately, the ability to probe hydrogen-bond networks over lipid bilayers holds the promise of opening paths for understanding, controlling, and predicting specific and non-specific interactions between membranes and ions, small molecules, peptides, polycations, proteins, and coated and uncoated nanomaterials.I. Introduction. The structure of water over lipid membranes is of interest for a variety of reasons that are rooted in fundamental scientific interest and connect all the way to biological function and technological applications. 1-6 Specific questions pertain to whether there exist populations of interfacial water molecules that can undergo hydrogen-bond (H-bond) interactions with certain membrane constituents that can be strengthened or weakened with variations in ionic strength, or, as indicated by molecular dynamics simulations, 2 whether some population of water molecules exists that may interact specifically with certain lipid headgroups over others.While interface-specific vibrational spectroscopic approaches, particularly those that are based on sum frequency generation (SFG), are in principle well suited for probing water near membranes, this method has been largely limited to probing lipid monolayers 1, 7-16 chemically asymmetric bilayers, [17][18][19] or the use of D 2 O as opposed to H 2 O. 20-21 Indeed, the use of SFG spectroscopy for probing fully hydrogenated lipid bilayers is now just emerging. Part of the Dogangun et al. Page 3 reason for this relatively new ...

show abstract

Alteration of Membrane Compositional Asymmetry by LiCoO₂ Nanosheets

Cited by 42 publications

References 81 publications

Perturbation of Hydrogen Bonding Networks over Supported Lipid Bilayers by Poly (Allylamine Hydrochloride)

Perturbation of Hydrogen Bonding Networks over Supported Lipid Bilayers by Poly (Allylamine Hydrochloride)

Core chemistry influences the toxicity of multicomponent metal oxide nanomaterials, lithium nickel manganese cobalt oxide, and lithium cobalt oxide to Daphnia magna

Hydrogen Bond Networks Near Supported Lipid Bilayers from Vibrational Sum Frequency Generation Experiments and Atomistic Simulations

Contact Info

Product

Resources

About

Alteration of Membrane Compositional Asymmetry by LiCoO2 Nanosheets

Cited by 42 publications

References 81 publications

Perturbation of Hydrogen Bonding Networks over Supported Lipid Bilayers by Poly (Allylamine Hydrochloride)

Perturbation of Hydrogen Bonding Networks over Supported Lipid Bilayers by Poly (Allylamine Hydrochloride)

Core chemistry influences the toxicity of multicomponent metal oxide nanomaterials, lithium nickel manganese cobalt oxide, and lithium cobalt oxide to Daphnia magna

Hydrogen Bond Networks Near Supported Lipid Bilayers from Vibrational Sum Frequency Generation Experiments and Atomistic Simulations

Contact Info

Product

Resources

About

Alteration of Membrane Compositional Asymmetry by LiCoO₂ Nanosheets