Lyotropic Liquid Crystalline Mesophases Research Articles

PH-Dependent Lyotropic Liquid Crystalline Mesophase and Ionization Behavior of Phytantriol-Based Ionizable Lipid Nanoparticles.

Self-assembled lipid nanoparticles (LNPs), serving as essential nanocarriers in recent COVID-19 mRNA vaccines, provide a stable and versatile platform for delivering a wide range of biological materials. Notably, LNPs with unique inverse mesostructures, such as cubosomes and hexosomes, are recognized as fusogenic nanocarriers in the drug delivery field. This study delves into the physicochemical properties, including size, lyotropic liquid crystalline mesophase, and apparent pKa of LNPs with various lipid components, consisting of two ionizable lipids (ALC-0315 and SM-102) used in commercial COVID-19 mRNA vaccines and a well-known inverse mesophase structure-forming helper lipid, phytantriol (PT). Two partial mesophase diagrams are generated for both ALC-0315/PT LNPs and SM-102/PT LNPs as a function of two factors, ionizable lipid ratio (α, 0-100 mol%) and pH condition (pH 3-11). Furthermore, the impact of different LNP stabilizers (Pluronic F127, Pluronic F108, and Tween 80) on their pH-dependent phase behavior is evaluated. The findings offer insights into the self-assembled mesostructure and ionization state of the studied LNPs with potentially enhanced endosomal escape ability. This research is relevant to developing innovative next-generation LNP systems for delivering various therapeutics.

Understanding the role of water in the lyotropic liquid crystalline mesophase of high-performance flexible supercapacitor electrolytes using a rheological approach

The effect of water on the structure, properties, and flexibility of lyotropic liquid crystalline (LLC) C12E23-LiCl-H2O gel electrolytes was explored. Structural techniques, such as X-ray Diffraction (XRD), Polarized Optical Microscopy (POM), and five dynamic measurements, were employed to examine the rheological properties of the LLC mesophase across various water contents. These analyses provided quantitative insights into the influence of water content and LiCl concentration on gel strength, gelation point, and structural recovery. The three-dimensional network of the gel encapsulates Li+ and Cl− ions within hydrophilic domains, showing significant performance in supercapacitor applications. The observed increase in storage modules with decreasing water content is attributed to variations in the quantity and average size of junction points owing to system entanglement. These research findings highlight that excess water molecules, which break down micellar connections, are responsible for the weakening of the gel. Conversely, at low water concentrations, the micellar domains entangle, displaying viscoelastic behavior akin to that of a transitory polymer network.

Inverse Cubic and Hexagonal Mesophase Evolution within Ionizable Lipid Nanoparticles Correlates with mRNA Transfection in Macrophages.

mRNA lipid nanoparticle (LNP) technology presents enormous opportunities to prevent and treat various diseases. Here, we developed a novel series of LNPs containing ionizable amino-lipids showing a remarkable array of tunable and pH-sensitive lyotropic liquid crystalline mesophases including the inverse bicontinuous cubic and hexagonal phases characterized by high-throughput synchrotron radiation X-ray scattering. Furthermore, with an interest in developing mRNA therapeutics for lung macrophage targeting, we discovered that there is a strong correlation between the mesophase transition of the LNPs during acidification and the macrophage association/transfection efficiency of mRNAs. The slight molecular structural differences between the SM-102 and ALC-0315 ionizable lipids are linked to the LNP's ability to transform their internal structures from an amorphous state to the inverse micellar, hexagonal, and finally cubic structures during endosomal maturation. SM-102 LNPs showed exceptionally improved transfection efficiency due to their ability to form a cubic structure at a lower pH than the ALC-0315 analogues, which remained within the hexagonal structure, previously attributed to promoting endosomal escape of the ionizable LNPs. Overall, the new knowledge draws our attention to the important role of mesophase transition in endosomal escape, and the novel LNP libraries reported herein have broad prospects for advancing mRNA therapeutics.

Self-assembly of cellulose nanocrystals confined to square capillaries.

Biological systems exploit restricted degrees of freedom to drive self-assembly of nano- and microarchitectures. Simplified systems, such as colloidal nanoparticles that behave as lyotropic liquid crystalline mesophases in confined geometric spaces, may be used to mimic biological structures. Cellulose nanocrystals (CNCs) are colloidally stable nanoparticles that self-assemble into chiral nematic (ChN) liquid crystalline mesophases. To date, the self-assembly of ChN mesophases of CNCs has been studied under confinement conditions within curved surfaces or under drying conditions that impose curvatures that can be exploited to control ChN ordering; however, their self-assembly has not been investigated in geometries with square cross-sections under static conditions. Here, we show that because of surface anchoring on perpendicular surfaces, the ChN CNC phase is unable to bend with the 90° angle of the square capillary under increasing confinement. Instead, the ChN phase forms radial layers in the shape of concentric squircle shells. With increasing layer distance from the capillary wall, the squircles transition into concentric cylinder shells. In larger capillaries, the radial shell layers appear as a continuous spiral pattern that engulfs fragmented ChN pseudolayers, a defect to accommodate the cylindrical confinement of the mesophase. These results are useful for understanding the fundamentals of self-assembling systems and development of new technologies.

Lyotropic Liquid Crystalline Mesophases of Lithium Dihydrogen Phosphate and 10-Lauryl Ether Stabilized with Water or Phosphoric Acid.

The molten phase of transition metal and lithium salts self-assemble with non-ionic surfactants to form lyotropic liquid crystalline (LLC) mesophases, which are important in the development of gel-electrolytes and mesoporous materials. Here, we show that LiH2 PO4 forms a semi-stable LLC mesophase with 10-lauryl ether (C12 H25 (OCH2 CH2 )10 OH, C12 E10 ), decoded as Li-EO-X (X is LiH2 PO4 /C12 E10 mole ratio and between 2 and 200). The stability of the Li-EO-X phase is improved by increasing salt concentration (X>20) in the media. The semi-stable Li-EO-X mesophase is further stabilized by adding either water by controlling the humidity or H3 PO4 (PA) to the media. The phase behaviour of the above samples was investigated using POM, XRD, conductivity, and ATR-FTIR measurements. The addition of PA not only brings stability and higher conductivity (increase from 0.1 to 8.9 mS/cm) to the mesophase but also produce an LLC gel-electrolyte with a high buffer capacity that may be useful and important in various applications.

Boost Up the Mechanical and Electrical Property of CNT Fibers by Governing Lyotropic Liquid Crystalline Mesophases with Aramid Polymers for Robust Lightweight Wiring Applications

Monofilament type of polyaromatic amide (PA) and carbon nanotube (CNT) composite fibers is presented. A concept of a lyotropic liquid crystal (LLC) constructed via a spontaneous self-assembly is introduced to mitigate the extremely low compatibility between PA and CNT. These approaches provide an effective co-processing route of PA and CNT simultaneously to fabricate the uniform, continuous, and reliable composite fibers through a wet-spinning. Interestingly, the addition of a small amount PA into the dope solution of CNT governs the LLC mesophase not only in a spinneret stage but also in a coagulant region. Thus, the developed PA/CNT composite fibers have the high uniaxial orientational order and the close interfacial packing compared to the pure CNT fibers. The PA/CNT composite fibers achieve the outstanding tensile strength, electrical conductivity, and electrochemical response, while maintaining a lightweight. They also exhibit the chemical, mechanical, and thermal robustness. All of these advantages can make flexible, sewable, and washable PA/CNT composite fibers ideal nanocomposite materials for use in next-generation information and energy transporting system by replacing conventional metal electrical conductors.Graphical The lyotropic liquid crystal self-assembly governed by doping the aramid polymers shows the ability to construct mechanically strong and continuous carbon nanotube-based composite fibers that can be used in the lightweight and robust electrical wiring for extreme environmental applications.

Chitosan/Lactic Acid Systems: Liquid Crystalline Behavior, Rheological Properties, and Riboflavin Release In Vitro.

Chitosan or its derivatives exhibit lyotropic liquid crystalline mesophases under certain conditions due to its semi-rigid structures. This work describes the development of chitosan-based biocompatible systems that include new components: lactic acid and non-ionic surfactants. Polarized optical microscopy studies revealed that these systems are capable of forming gels or lyotropic liquid crystals (LLCs) in a certain range of chitosan and lactic acid concentrations. According to the viscosity studies, the rheological flow of the LLCs can be accurately described by the Casson flow model. The intermolecular interactions of the LLC components were studied by FTIR spectroscopy. According to the FTIR data, hydrogen bonding is supposed to be responsible for the formation of the LLCs. In the studied systems, this LLC complex exists as the [ChitH+·CH3-CH(OH)-COO-] ion pair. The studied gel and LLCs were shown to possess the most prolonged release capabilities for riboflavin among similar binary LLC systems. The supramolecular organization and rheological characteristics of the studied chitosan-based systems were found to affect the release of riboflavin.

Tailoring the self-assembly of lipid-based lyotropic liquid crystalline mesophases with biocompatible ionic liquid aqueous solutions

Interest in lipid-based lyotropic liquid crystalline nanoparticles (LCNPs) as drug delivery vehicles continues to grow, owing to their unique structural features. The structure of these particles can be controlled to suit specific applications, through tailoring the lipid composition and solvent conditions. Ionic liquids (ILs) are liquid salts comprising tailorable cations and anions, of which some are known to support the self-assembly of amphiphiles, and hence can be used as designer solvents for LCNPs. We employed dynamic light scattering, small angle X-ray scattering, and cryogenic transmission electron microscopy to examine the particle size and lyotropic liquid crystalline mesophase behavior of monoolein (MO)-based LCNPs in aqueous solutions containing 13 choline ILs with a selection of amino acid and carboxylate anions at 6 concentrations 20, 10, 5, 1, 0.33, and 0.16 wt%. Our results show the formation of LCNPs with various liquid crystalline nanostructures, including the inverse bicontinuous primitive cubic (Q2) phase with the Im3m crystallographic space group, the inverse hexagonal (H2), and the inverse discontinuous micellar cubic (I2) phases. The internal nanostructures of the MO nanoparticles depended on three main factors, the anion of the ILs, the IL concentration, and the pH of the solution. This study elucidates the potential application of IL solvents as a powerful tool to tailor the internal nanostructure of MO-based LCNPs, and advances the exploration of IL-enabled responsive LCNPs systems as prospective nanocarriers.

Chiral emergence in multistep hierarchical assembly of achiral conjugated polymers

Intimately connected to the rule of life, chirality remains a long-time fascination in biology, chemistry, physics and materials science. Chiral structures, e.g., nucleic acid and cholesteric phase developed from chiral molecules are common in nature and synthetic soft materials. While it was recently discovered that achiral but bent-core mesogens can also form chiral helices, the assembly of chiral microstructures from achiral polymers has rarely been explored. Here, we reveal chiral emergence from achiral conjugated polymers, in which hierarchical helical structures are developed through a multistep assembly pathway. Upon increasing concentration beyond a threshold volume fraction, dispersed polymer nanofibers form lyotropic liquid crystalline (LC) mesophases with complex, chiral morphologies. Combining imaging, X-ray and spectroscopy techniques with molecular simulations, we demonstrate that this structural evolution arises from torsional polymer molecules which induce multiscale helical assembly, progressing from nano- to micron scale helical structures as the solution concentration increases. This study unveils a previously unknown complex state of matter for conjugated polymers that can pave way to a field of chiral (opto)electronics. We anticipate that hierarchical chiral helical structures can profoundly impact how conjugated polymers interact with light, transport charges, and transduce signals from biomolecular interactions and even give rise to properties unimagined before.

Role of Water in the Lyotropic Liquid Crystalline Mesophase of Lithium Salts and Non-ionic Surfactants.

The lyotropic liquid crystalline (LLC) mesophase forms upon evaporation of water from aqueous solutions of LiX salts (X is Cl-, Br-, NO3-, or SCN-) and a surfactant [C12H25(OCH2CH2)10OH, abbreviated as C12E10]. The LiX/C12E10/H2O aqueous solutions have been monitored (during evaporation of their excess water to obtain stable LLC mesophases) by gravimetric, spectroscopic, and conductivity measurements to elucidate the role of water in these mesophases. The water/salt molar ratio in stable mesophases changes from 1.5 to 8.0, depending on the counteranion of the salt and the ambient humidity of the laboratory. The LiX/C12E10/H2O LLC mesophases lose water at lower humidity levels and absorb water at higher humidity levels. The LiCl-containing mesophase holds as few as four structural water molecules per LiCl, whereas the LiNO3 mesophase holds 1.5 waters per salt (least among those assessed). This ratio strongly depends on the atmospheric humidity level; the water/LiX mole ratio increases by 0.08 ± 0.01 H2O in the LLC mesophases per percent humidity unit. Surprisingly, the LLC mesophases are stable (no salt leaching) in broad humidity (10-85%) and salt/surfactant mole ratio (2-10 LiX/C12E10) ranges. Attenuated total reflectance Fourier transform infrared spectroscopic data show that the water molecules in the mesophase interact with salt species more strongly in the LiCl mesophase and more weakly in the case of the nitrate ion, which is evident by the shift of the O-H stretching band of water. The O-H stretching peak position in the mesophases decreases in the order νLiCl > νLiBr > νLiSCN > νLiNO3 and accords well with the H2O/LiX mole ratio. The conductivity of the LLC mesophase also responds to the amount of water as well as the nature of the counteranion (X-). The conductivity decreases in the order σLiCl > σLiBr > σLiNO3 > σLiSCN at low salt mole ratios and in the order σLiBr > σLiCl > σLiNO3 > σLiSCN at higher ratios due to structural changes in the mesophase.

Role of Water in the Lyotropic Liquid Crystalline Lithium Iodide-Iodine-Water-C12E10 Mesophase as a Gel Electrolyte in a Dye-Sensitized Solar Cell.

By replacing volatile and flammable organic-based electrolytes with gel electrolytes, dye-sensitized solar cells (DSSCs) may be a viable and more practical alternative to other clean energy sources. Although they present a promising alternative, gel electrolytes still have some drawbacks for practical applications, such as low ionic conductivity and infusion difficulties into the pores of the working electrode. Here, we introduce a new one-step fabrication method that uses a lyotropic liquid crystalline (LLC) gel electrolyte (LiI:I2:H2O:C12H25(OCH2CH2)10OH) and a dye (N719) to construct a DSSC that performs (7.32%) 2.2 times better compared with a traditional two-step production. Water plays a key role in the gel electrolyte, where the H2O/LiI mole ratio is around 2.57 under ambient laboratory conditions (ALCs); however, this ratio linearly increases to 4.00 and then to 5.85 at 40 and 75% humidities, respectively, without affecting the two-dimensional (2D) hexagonal structure of the mesophase. The ionic conductivity of the gel electrolyte linearly increases accordingly, by 2.2 (4.8 × 10-5 to 10.6 × 10-5) and 13.1 times (63.0 × 10-5 S/cm) from ALC to 40 and ALC to 75% humidity, respectively. Increasing water in the gel phase improves the conductivity of the LLC mesophase and the short-circuit current (Isc) of the DSSC, but negatively influences the open-circuit voltage (Voc) of the cell, equilibrium reaction between the LiI and I2, and the anchoring of the dye molecules over the titania surface.

Novel Amphiphilic Block Copolymers for the Formation of Stimuli-Responsive Non-Lamellar Lipid Nanoparticles.

Non-lamellar lyotropic liquid crystalline (LLC) lipid nanoparticles contain internal multidimensional nanostructures such as the inverse bicontinuous cubic and the inverse hexagonal mesophases, which can respond to external stimuli and have the potential of controlling drug release. To date, the internal LLC mesophase responsiveness of these lipid nanoparticles is largely achieved by adding ionizable small molecules to the parent lipid such as monoolein (MO), the mixture of which is then dispersed into nanoparticle suspensions by commercially available poly(ethylene oxide)–poly(propylene oxide) block copolymers. In this study, the Reversible Addition-Fragmentation chain Transfer (RAFT) technique was used to synthesize a series of novel amphiphilic block copolymers (ABCs) containing a hydrophilic poly(ethylene glycol) (PEG) block, a hydrophobic block and one or two responsive blocks, i.e., poly(4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)benzyl acrylate) (PTBA) and/or poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA). High throughput small angle X-ray scattering studies demonstrated that the synthesized ABCs could simultaneously stabilize a range of LLC MO nanoparticles (vesicles, cubosomes, hexosomes, inverse micelles) and provide internal particle nanostructure responsiveness to changes of hydrogen peroxide (H2O2) concentrations, pH and temperature. It was found that the novel functional ABCs can substitute for the commercial polymer stabilizer and the ionizable additive in the formation of next generation non-lamellar lipid nanoparticles. These novel formulations have the potential to control drug release in the tumor microenvironment with endogenous H2O2 and acidic pH conditions.

Robust Angular Anisotropy of Circularly Polarized Luminescence from a Single Twisted-Bipolar Polymeric Microsphere.

It has long been surmised that the circular polarization of luminescence (CPL) emitted by a chiral molecule or a molecular assembly should vary with the direction in which the photon is emitted. Despite its potential utility, this anisotropic CPL has not yet been demonstrated at the level of single molecules or supramolecular assemblies. Here we show that conjugated polymers bearing chiral side chains self-assemble into solid microspheres with a twisted bipolar interior, which are formed via liquid-liquid phase separation and subsequent condensation into a cholesteric lyotropic liquid crystalline mesophase. The resultant microspheres, when dispersed in methanol, exhibit CPL with a glum value as high as 0.23. The microspheres are mechanically robust enough to be handled with a microneedle under ambient conditions, allowing comprehensive examination of the angular anisotropy of CPL. The single microsphere is found to exhibit distinct angularly anisotropic birefringence and CPL with glum up to ∼0.5 in the equatorial plane, which is 2.5-fold greater than that along the polar axis. Such optically anisotropic solid materials are important for the application to next-generation microlight-emitting and visualizing devices as well as for fundamental optics studies of chiral light-matter interaction.

Tuning Nanostructured Lyotropic Liquid Crystalline Mesophases in Lipid Nanoparticles with Protic Ionic Liquids.

We herein report 13 protic ionic liquids (PILs) as tunable solvation media to regulate the internal lyotropic liquid crystalline mesophase of monoolein-based nanoparticles. A range of nanostructures, including inverse bicontinuous cubic, inverse hexagonal, and sponge/lamellar mesophases, were produced and verified by synchrotron small-angle X-ray scattering. Notably, manipulating the cation/anion structures of the PILs can alter the monoolein packing behavior and cause a sequential phase transition (hexagonal → cubic → lamellar) in the nanoparticles. The solvent channels inside the nanoparticles were enlarged up to 40% under certain PIL-water conditions, making these materials prospective for encapsulation of large molecules. Finally, a freeze-drying study demonstrated the ability of PILs to preserve nanostructure upon reconstitution of the nanoparticles compared to that in pure water. This study opens a new route for fine-tuning lyotropic liquid crystalline structures using PILs, which circumvents issues encountered using conventional salts.

The Evaluations of Menthol and Propylene Glycol on the Transdermal Delivery System of Dual Drug-Loaded Lyotropic Liquid Crystalline Gels.

This study aimed to evaluate the effects of two different structural alcohol permeation enhancers (menthol and propylene glycol) on the internal structure and in vitro properties of the dual drug-loaded lyotropic liquid crystalline (LLC) gels. The LLC gels were prepared and characterized by polarized light microscopy, small-angle X-ray scattering, differential scanning calorimetry, attenuated total reflectance-Fourier transform infrared spectrum, and rheology. Based on the results, the inner structure of the gels was QII mesophase and exhibited a pseudoplastic fluid behavior. The level of internal order in the LLC mesophase would be affected by introduced 2wt% menthol (MEN) and propylene glycol (PG). The in vitro release experiment showed that the release behavior of sinomenine hydrochloride (SH) and cinnamaldehyde (CA) from the LLC system was dominated by Fickian diffusion (n < 0.43). MEN and PG had the opposite effects on the release of hydrophilic SH, while the MEN and PG both increased the release of lipophilic drug CA. Furthermore, in vitro permeation studies indicated that MEN and PG could both improve the skin permeability of SH and CA, and MEN displayed more pronounced enhancement. All the samples showed no skin irritation on the normal rat skin. Collectively, in our research, monoterpenoid MEN exhibited a better penetration-promoting effect than straight-chain fatty alcohol PG on the dual drug-loaded LLC system.

Lyotropic Liquid Crystalline Mesophase Governs Interfacial Molecular Orientation of Conjugated Polymer Thin Films

Interfacial out-of-plane molecular orientation critically influences the electronic performance of organic semiconductor thin films. The appearance of a lyotropic liquid crystalline (LC) mesophase ...

Aqueous Lyotropic Mesophase Behavior of Gemini Dicarboxylate Surfactants Swollen with n-Decane.

We report detailed small-angle X-ray scattering (SAXS) studies of the impact of variable n-decane loadings on the lyotropic liquid crystalline (LLC) phase behaviors of homologous bis(tetramethylammonium) gemini didecanoate surfactants TMA-7x, which derive from dimerizing decanoic acid through its α-carbon with hydrocarbyl linkers -(CH2)x- where x = 3, 4, 5, and 6. TMA-7x amphiphiles with x = 3 or 5 exhibit a strong propensity to form normal double gyroid (G) LLC network mesophases over wide surfactant hydration ranges, as compared to homologues with x = 4 or 6. On swelling aqueous TMA-7x LLC mesophases with up to 35 wt % n-decane, we demonstrate that odd-carbon linked surfactants (x = 3 or 5) form G and normal double diamond (D) phases over wide water concentration windows with T = 22-100 °C. Complementary studies of decane-swollen TMA-7x (x = 4 or 6) aqueous LLCs instead demonstrate significantly diminished network phase stability, in favor of hexagonally-packed cylinder phases and a zoo of complex quasispherical micelle packings, which include micellar C14 and C15 Laves phases (P63/mmc and Fd3(-)m symmetries, respectively) and high-symmetry hexagonally close packed (HCP) and body-centered cubic (BCC) arrangements. These rich phase behaviors are rationalized in terms of linker length parity-dependent surfactant conformations and the delicate free energy balance that guides the packing of these geometrically anisotropic amphiphiles by minimizing unfavorable water-hydrophobic contacts, maximizing ionic surfactant-headgroup counterion solvation with minimal local variations, and maximizing electrostatic cohesion within these supramolecular assemblies.

Lyotropic Lamellar Mesophase. Magneto-Morphologic Transforma tions and Optical Refracting Properties: Effect of Optically Active Dopants

Abstract Effect of optically active dopants on the morphologic and optical refracting properties of the lyotropic liquid crystalline mesophase with anisometric micelles has been investigated. Lyotropic lamellar mesophases, which are formed by the plate-like micelles of quasi-indef inite diameter, were objects of the investigations. Wine acid (WA) and tartaric acid (TA) were used as the optically active dopants. Texture transformations under influence of an external magnetic field and time and temperature changes of these textures for quaternary mixtures with various concentrations of the optically active dopants have been studied. Unusual textures with the spherical microdroplet formations have been found and studied. The optical refracting properties of ternary and quaternar y lyotropic systems vs. temperature and concentration were investigated.

Lyotropic liquid crystalline hexagonal mesophase. Thermo-morphologic and magneto-morphologic transformations, electrical conductivity and optical refractive properties: Effect of optically active compounds

Mesophase chirality in lyotropic liquid crystalline hexagonal E mesophase, which is formed by the anisometric micelles with quasi-infinite length, was studied. Effect of the optically active dopants {tartaric acid (TA) and wine acid (WA)} on the thermo-morphologic, magneto-morphologic, electrical conductivity and optical refractive properties of E mesophase has been investigated. Chiral structures of E mesophase with the spaghetti-like texture have been found in the quaternary amphiphile+water+aliphatic alcol+chiral dopant lyotropic systems and the pitch of such structures vs. concentration of optically active dopants has been estimated. Texture transformations vs. temperatures and external magnetic fields for mixtures with various concentrations of the optically active dopants have been studied. Effect of TA and WA dopants on texture types, specific electrical conductivity and refractive index is analyzed and discussed.

Lyotropic Liquid Crystalline Mesophases Made of Salt-Acid-Surfactant Systems for the Synthesis of Novel Mesoporous Lithium Metal Phosphates.

Mesoporous lithium metal phosphates are an important class of materials for the development of lithium ion batteries. However, there is a limited success in producing mesoporous lithium metal phosphates in the literature. Here, a lyotropic liquid crystalline (LLC) templating method was employed to synthesize the first examples of LiMPO4 (LMP) of Mn(II), Co(II), and Ni(II). A homogeneous aqueous solution of lithium and transition metal nitrate salts, phosphoric acid (PA), and surfactant (P123) can be spin coated or drop-cast coated over glass slides to form the LLC mesophases which can be calcined into mesoporous amorphous LMPs (MA-LMPs). The metal salts of Mn(II), Co(II) and Ni(II) produce MA-LMPs that crystallize into olivine structures by heat treatment of the LLC mesophase. The Fe(II) compound undergoes air oxidation. Therefore, both Fe(II) and Fe(III) precursors produce a crystalline Li3 Fe2 (PO4 )3 phase at over 400 °C. The MA-LMPs show no reactivity towards lithium, however the crystalline iron compound exhibits electrochemical reactivity with lithium and a good electrochemical energy storage ability using a lithium-ion battery test.