Self-assembly Of Surfactants Research Articles

Unusual microwave heating of water in reverse micellar solution

Microwaves (MWs) are widely used for heating food, accelerating chemical reactions, drying materials, therapies, and so on. Water molecules absorb MWs and produce heat because of their substantial electric dipole moments. Recently, increasing attention has been paid to accelerating various catalytic reactions in water-containing porous materials using MW irradiation. Here, a critical question is whether water in nanoscale pores generates heat in the same way as liquid water. Is it valid that MW-heating behaviors of nanoconfined water are estimated solely by a dielectric constant of liquid water? There are almost no studies regarding this question. Here, we address it using reverse micellar (RM) solutions. Reverse micelles are water-containing nanoscale cages formed by self-assembled surfactant molecules in oil. We measured real-time temperature changes of liquid samples within a waveguide under MW irradiation at 2.45 GHz and at MW intensities of ~ 3 to ~ 12 W/cm2. We found that the heat production and its rate per unit volume of water in the RM solution are about one order of magnitude larger than those of liquid water at all the MW intensities examined. This indicates that water spots that are much hotter than liquid water under MW irradiation at the same intensity, are formed in the RM solution. Our findings will give fundamental information to develop effective and energy-saving chemical reactions in nanoscale reactors with water under MW irradiation, and to study MW effects on various aqueous mediums with nanoconfined water. Furthermore, the RM solution will serve as a platform to study the impact of nanoconfined water on MW-assisted reactions.

Electrostatic Epitaxy of Orientational Perovskites for Microlasers.

Orientational growth of single-crystalline structures is pivotal in the semiconductor industry, which is achievable by epitaxy for producing thin films, heterostructures, quantum wells, and superlattices. Beyond silicon and III-V semiconductors, solution-processible semiconductors, such as metal-halide perovskites, are emerging for scalable and cost-effective manufacture of optoelectronic devices, whereas the polycrystalline nature of fabricated structures restricts their application toward integrated devices. Here, electrostatic epitaxy, a process sustained by strong electrostatic interactions between self-assembled surfactants (octanoate anions) and Pb2+ , is developed to realize orientational growth of single-crystalline CsPbBr3 microwires. Strong electrostatic interactions localized at the air-liquid interface not only support preferential nucleation for single crystallinity, but also select the crystal facet with the highest Pb2+ areal density for pure crystallographic orientation. Due to the epitaxy at the air-liquid interface, direct growth of oriented single-crystalline microwires onto different substrates without the processes of lift-off and transfer is realized. Photonic lasing emission, waveguide coupling, and on-chip propagation of coherent light are demonstrated based on these single-crystalline microwires. These findings open an avenue for on-chip integration of single-crystalline materials.

How Does Nanostructure in Ionic Liquids and Hybrid Solvents Affect Surfactant Self-Assembly?

Ionic liquids (ILs) have recently emerged as novel classes of solvents that support surfactant self-assembly into micelles, liquid crystals, and microemulsions. Their low volatility and wide liquid stability ranges make them attractive for many diverse applications, especially in extreme environments. However, the number of possible ion combinations makes systematic investigations both challenging and rare; this is further amplified when mixtures are considered, whether with water or other H-bonding components such as those found in deep eutectics. In this Perspective we examine what factors determine amphiphilicity, solvophobicity and solvophilicity, in ILs and related exotic environments, in what ways these differ from water, and how the underlying nanostructure of the liquid itself affects the formation and structure of micelles and other self-assembled materials.

Effect of anions and cations on the self-assembly of ionic liquid surfactants in aqueous solution

Ionic liquid surfactants have shown increasing promise for substituting the traditional amphiphiles due to their flexible tunability and superior physicochemical properties. However, the effect of cationic structure and anion type on the surface properties of ionic liquid surfactants remains unclear. Herein, four ionic liquid surfactants [C12mim][BF4], [PyC12][Br], [C12mim][Br] and [PyC12][BF4] with the same alkyl side chain length were designed and synthesized. Their surface properties, such as micelle-free energy (ΔGmθ), surface tension reduction efficiency (ПCMC), and adsorption efficiency (pC20), and the influence of the type and structure of the anion and cation on their micellar physicochemical properties in aqueous solution were discussed according to the data. The proposed approach demonstrates that the critical micelle concentration (CMC) is determined by combining electrostatic and hydrophobic effects. When the anion is BF4−, the ionic liquid has a lower CMC, and BF4− has a superior hydrophobic effect, which allows the ionic liquid to form micelles more easily. In addition, the ionic liquid of tetrafluoroborate has higher interfacial activity (larger pC20) at the same temperature and its aqueous solution has lower surface tension, making it a more desirable surfactant. All four types of ionic liquids have negative values of ΔGmθ, implying that micelle formation is a spontaneous process. The surface activity of imidazolium- and pyridinium-based ionic liquids was slightly different from the critical micelle concentration under the same anion and carbon chain length. Imidazole and pyridine have highly similar hydrophobic and electrostatic effects, and the cation may not be the most critical factor affecting the surface properties.

Interfacial Engineering of Particulate & Surfactant Systems for Enhanced Performance in Industrial Applications

Particulate and surfactant systems are an integral part either in processing or product lines in essentially every major industry, including Energy and Minerals, Pharmaceutical, Agriculture & Food, Microelectronics, Healthcare, Cosmetics, Consumer Products, and Analytical Instrumentation & Services. In most applications, product and process specifications depend on the synergistic or competitive interactions between the particles and reagent schemes. The primary goal of our research efforts has been to generate the structure-property-performance correlations-based knowledge and technology platforms for industry to develop more sustainable products and processes. Engineering the physicochemical/mechanical properties of surfaces, particles, and self-assembling surfactant systems enables their enhanced performance in industrial applications. Specifically, understanding and control of the nano and atomic-scale forces between particles and synthesis of functionalized particles form the foundation for targeted contributions in biomedical, advanced materials and minerals, sensor, and coating technologies. A synoptic overview of selected projects is presented in this review. Additional details can be found in the topic-specific references listed at the end of this manuscript.

The role of surface topography in the self-assembly of polymeric surfactants.

We propose a classical density functional theory model to study the self-assembly of polymeric surfactants on curved surfaces. We use this model to investigate the thermodynamics of phase separation of a binary mixture of size asymmetric miscible surfactants on cylindrical and spherical surfaces, and observe that phase separation driven by size alone is thermodynamically unfavorable on both cylindrical and spherical surfaces. We use the theory, supplemented by dissipative particle dynamics (DPD) simulations, to predict pattern formation on a non-uniform surface with regions of positive and negative curvature. Our results suggest potential ways to couple surface topography and polymeric surfactants to design surfaces coated with non-uniform patterns.

Study of the self-assembly of a gemini surfactant induced by anionic QDs in aqueous solution.

The interaction of anionic quantum dots (QDs) with a gemini surfactant (1,1'-(propane-1,3-diyl-2-ol)bis(3-hexadecyl-1H-imidazol-3-ium)) bromide [C16Im-3OH-ImC16]Br2 in water has been investigated, yielding a unique class of luminescent self-assemblies. Instead of engaging with the QDs directly, the dimeric surfactant self-associates into micelles first. After adding [C16Im-3OH-ImC16]Br2 to aqueous solutions containing QDs, two types of structural formations, supramolecular and vesicles, were confirmed. A variety of intermediary structures, including cylindrical and oligomers of vesicles are found to be present. Field-emission scanning electron microscopy (FESEM) and confocal laser scanning microscopy (CLSM) were used to investigate the luminescent and morphological properties of the self-assembled nanostructures in the first turbid (Ti) and second turbid (Tf) regions. FESEM images show discrete spherical vesicles in the mixture's Ti and Tf regions. The presence of self-assembled QDs in these spherical vesicles makes them naturally luminescent, according to CLSM data. Because the QDs are equally distributed in the micelles, their self-quenching is greatly reduced and their luminescence is effectively sustained. We have also demonstrated the successful encapsulation of dye rhodamine B (RhB) into these self-assembled vesicles using CLSM without any structural disturbance. The discovery of luminescent self-assembled vesicles from a QD-[C16Im-3OH-ImC16]Br2 combination might lead to new potential in controlled release drug delivery and sensing.

HRMAS-NMR and simulation study of the self-assembly of surfactants on carbon nanotubes.

Polyethoxylated surfactants, such as those of the Tween and Pluronic series, are commonly used to disperse carbon nanotubes (CNTs) and other nanoparticles. However, the current understanding of the nature of interactions between these surfactants and CNTs is limited. The nature of the interactions between surfactants (Tween-80 [T80] and Pluronic F68 [PF68]) and CNTs was investigated using high-resolution magic angle spinning nuclear magnetic resonance (HRMAS-NMR) and coarse-grained molecular dynamics (MD) simulations. HRMAS-NMR revealed that T80 molecules interact with single-walled CNTs (SWCNTs) and multi-walled CNTs (MWCNTs) via the oleyl chain, whereas PF68 molecules interact with the surface of SWCNTs and MWCNTs via the polypropylene oxide residues. The polyethylene oxide chains were oriented towards the external aqueous environment. The HRMAS-NMR results were supported by MD simulations, and the latter provided further insights into the nature of the interactions.

The effects of the nature of the sterol on the properties and stability of niosome bilayer vesicles

Niosome vesicles as potential nanocarriers for drug delivery systems have been in development since the mid-1980s. These vesicles form by self-assembly of cholesterol and nonionic surfactants in an aqueous phase. The aim of the present molecular dynamics (MD) simulation study is to determine how changes in the sterol side chain and ring affect the structure and stability of sorbitan monostearate (Span60) niosome bilayers. Five sterols are examined: cholesterol (CHL), β-sitosterol (BST), ergosterol (ERG), stigmasterol (STS), and lanosterol (LST). Different sets of simulations were performed by varying the number of molecules (30, 40, and 50 % sterol concentration). The interactions between Span60 and the different sterols are found to be strongly dependent on the sterol’s side chain and head group. BST is found to markedly reduce the effectiveness of the sterol on the ordering of the bilayers, a result that persists over the whole range of concentrations examined in this work.

CO2-Responsive Wormlike Micelles Based on Pseudo-Tetrameric Surfactant.

Wormlike micelles, which are linear aggregates created by the self-assembly of surfactants, may entangle to form dynamic three-dimensional network-like structures, endowing solutions with considerable macroscopic viscoelasticity. Recently, a pressing need has arisen to research a novel stimuli-responsive worm-like micelle that is efficient and environmentally friendly. CO2 is an inexpensive, abundant, non-toxic, biocompatible, and non-combustible gas, and it is anticipated that CO2 may serve as the trigger for stimuli-responsive worm-like micelles. In this paper, the formation of CO2-switchable pseudo-tetrameric surfactants, which subsequently self-assemble into CO2-switched wormlike micelles, is accomplished using a simple mixing of two commercial reagents, such as stearic acids and cyclen. The rheological characteristics switched by the use of CO2 are cycled between that of a low-viscosity (1.2 mPa·s) fluid and a viscoelastic fluid (worm-like micelles, 3000 mPa·s). This article expands the field of study on stimuli-responsive worm-like micelles.

Self-assembly of anionic surfactant and its effect on oil–water interface: Implications for enhanced oil recovery

Surfactant micellization is a self-assembly process governed by complex interplay of solvent-mediated interactions. However, quantitative modeling of micelle formation and its effect on oil–water interface are not yet completely understood. In this work, dissipative particle dynamics simulations were used to investigate the self-assembly behavior of anionic surfactants of alcohol alkoxy sulfate (AAS) and its structural influence on the interfacial properties of oil–water at the mesoscopic scale. Our results indicate that with the increase of surfactant concentration, the morphology of surfactant aggregates varied from spherical micelles to rod-shaped micelles, and finally formed worm-like micelles. The larger the number of propylene oxide (PO) groups, the easier the formation of large micelles and the more tightness of formed micelles. On the oil–water interface, the interfacial tension of solutions decreased with increasing surfactant concentration below the critical micelle concentration, whereas a positive correlation was found for the tightness of surfactant arrangement. When surfactants formed micelles, the overall coverage area of AAS decreased and a lower root mean square end distance of individual PO group directly affected interfacial properties of AAS. The obtained results could provide a solid theoretical basis for the rational design of efficient surfactants in oil recovery and soft matter applications.

Self-Assembled Structure of α-Isostearyl Glyceryl Ether Affects Skin Permeability-a Lamellar with 70-nm Spaces and L3 Phase Enhanced the Transdermal Delivery of a Hydrophilic Model Drug.

Self-assembled surfactant structures, such as liquid crystals, have the potential to enhance transdermal drug delivery. In the present study, the pseudo-ternary system of GET (composed of α-Isostearyl glyceryl ether (GEIS) and polysorbate 60)/1,3 butanediol (BG)/water) was shown to exhibit a complex phase diagram. Small- and wide-angle X-ray scattering (SWAXS) and freeze-fracture transmission electron microscopy (FF-TEM) revealed that GET6BG60 (6%GET/60%BG/34%Water) formed a lamellar phase with a repeated distance of approximately 72nm. Such a long-repeated distance of the lamellar phase was unique in the surfactant system. Moreover, the various structures, such as multilamellar vesicles and branched-like layers, were observed, which suggested that they might be deformable. On the other hand, only core-shell particles were observed in GET6BG20, the core of which was an L3 phase. GET6BG20 and GET6BG60 significantly enhanced the skin permeation of the hydrophilic model drug, antipyrine (ANP) (log Ko/w, - 1.51). However, their permeation profiles were distinct. Liquid chromatography-tandem mass spectrometry revealed that epidermal accumulation of GEIS was significantly higher with GET6BG60 than GET6BG20 after 1.5h of permeation, which might be attributed to differences in their deformable properties. Furthermore, GEIS was reported to affect intercellular lipids. Accumulated GEIS in the epidermis may have interacted with intercellular lipids and enhanced the transdermal delivery of ANP. The difference in the permeation profiles of ANP may be attributed to the penetration process of GEIS in the epidermis. This study suggests that GET6BG20 and GET6BG60 are unique carriers to enhance the permeation of hydrophilic drugs, such as ANP.

Editorial: theme issue on complex rheology in biological systems

Editorial: theme issue on complex rheology in biological systems

Self-Assembly of a C16M[Mn] Magnetic Surfactant in Water.

A magnetic surfactant, which combines the properties of a surfactant with magnetic responsiveness, shows great potential in biotechnology, separation, adsorption, and catalysis, especially in non-invasive manipulation through a magnetic field. However, a molecularly magnetic surfactant is usually paramagnetic for the amorphous and less ordered structures. In this work, magnetic surfactant 1-methyl-3-hexadecane-imidazolium [MnCl2Br] (C16M[Mn]) is reported to self-assemble in water. The C16M[Mn] magnetic surfactant self-assembles in water to form a lamellar hydrogel from 10 to 50 wt % at and below room temperature. The hydrogel changes from a gel to a sol at 30 °C, and the hexadecane chains in the hydrogel change from noncrystalline to crystalline at 0 °C. In the hydrogel state, the lamellar domain spacing is varied from 36 to 45 nm depending on the concentration and self-assembly temperature. After self-assembly, the magnetic susceptibility of the freeze-dried magnetic surfactant is increased. Most important is the fact that the freeze-dried sample at a high concentration (40-50 wt %) shows the highest magnetic susceptibility, which is related to the closer molecular packing and the more ordered structures. The self-assembly-induced increase in magnetic susceptibility provides a method for improving the magnetic properties of a magnetic surfactant.

Stable nanoreactors for material fabrication using the aggregation of fluorinated ionic liquid surfactants in ionic liquid solvents

The design of thermostable and efficient self-assembly nanoreactors is highly desirable for the fabrication of nanomaterials. Benefiting from the tunable properties and nonvolatility of ionic liquids (IL), IL-in-IL self-assembly systems show a flexible structure and thermostability under extreme conditions. Inspired by this hypothesis, stronger hydrophobic fluorinated ILs are expected to fabricate nonvolatile IL-in-IL self-assembly systems. In this work, two series of fluorinated ILs were synthesized and characterized by NMR, FTIR, DSC, and TGA. Then, the aggregation of these fluorinated ILs in protic and aprotic IL solvents was studied by surface tension and 19F NMR methods. The microstructure of these IL-in-IL aggregation systems was characterized by DLS and SAXS. The fluorinated ILs exhibit excellent surface activity even in aprotic ILs. Furthermore, protic ILs display superior ability to promote the self-assembly of ILs surfactants. These IL-in-IL aggregation systems display the typical morphology of ellipsoidal or multilayer spherical micelles with diameters of approximately 10 nm ∼ 60 nm. A typical IL-in-IL aggregation system was proposed as an efficient nanoreactor to prepare nanoscale MOFs without using any volatile organic solvents or autoclaving. The synthesized HKUST-1 exhibits larger surface areas and nanoscale morphology by XRD, SEM, TEM, BET, and XPS characterization. The results presented in this study offer key information to design new thermostable IL-based colloidal systems and their applications.

PH-Induced hydrogels and viscoelastic solutions constructed by a Rosin-Based Pseudo-Gemini surfactant

• A novel pseudo-Gemini surfactant was constructed by mixing a rosin-based surfactant (C 10 MPAN) with maleic acid (MA). • Hydrogels at pH 5.35–5.00, 2.00 ∼ 1.00 and viscoelastic solutions at pH 5.00–2.00 are formed in the C 10 MPAN/MA system. • Vesicles, wormlike and enormous lamellar micelles were sequentially formed by decreasing the pH of C 10 MPAN/MA system. • In C 10 MPAN/MA system, maltese crosses lamellar liquid crystal was formed in the hydrogels at pH 1.00. Rosin-based surfactants exhibit unique superiority in self-assembly; however, pseudo-Gemini surfactants derived from rosin are rare. Herein, A new pH-responsive surfactant, N-decyl-maleimidepimaric acid N, N-dimethylenediamide (C 10 MPAN) was synthesized from rosin, and its structure was characterized by NMR and MS. Additionally, a novel pseudo-Gemini surfactant was prepared by mixing C 10 MPAN and maleic acid (MA) at a molar ratio of 2:1. Hydrogels at pH 5.35–5.00, viscoelastic solutions at pH 5.00–2.00, and hydrogels at pH ≤ 2.00 formed sequentially in the C 10 MPAN/MA aqueous solutions. The properties of these hydrogels and viscoelastic solutions were investigated using rheology, cryogenic transmission electron microscopy (cryo-TEM), differential scanning calorimetry (DSC), polarized optical microscopy (POM), and small-angle x-ray scattering (SAXS). The aggregates in the C 10 MPAN/MA aqueous solution underwent a transition from unilamellar vesicles to multilamellar vesicles, to wormlike micelles, and finally to enormous lamellar micelles as the pH was decreased from 5.35 to 1.00. The exponent between the zero-shear viscosity of the wormlike micelles and concentration reached 23.1. The sizes of the unilamellar vesicles at pH 5.35 varied from 10 to 100 nm, while those of the multilamellar vesicles at pH 5.00 reached 500 nm. Moreover, a Maltese crosses liquid crystal phase was formed by the lamellar micelles. 1 H NMR and surface tension methods were further used to investigate the aggregation mechanism induced by the pH. The large rigid skeleton of rosin acts as the backbone for the formation of diverse aggregates. This study shows the superior properties of rigid groups in the self-assembly of surfactants and provides a new insight for the applications of rosin.

Spontaneous formation of a self-healing carbon nanoskin at the liquid–liquid interface

Biological membranes exhibit the ability to self-repair and dynamically change their shape while remaining impermeable. Yet, these defining features are difficult to reconcile with mechanical robustness. Here, we report on the spontaneous formation of a carbon nanoskin at the oil–water interface that uniquely combines self-healing attributes with high stiffness. Upon the diffusion-controlled self-assembly of a reactive molecular surfactant at the interface, a solid elastic membrane forms within seconds and evolves into a continuous carbon monolayer with a thickness of a few nanometers. This nanoskin has a stiffness typical for a 2D carbon material with an elastic modulus in bending of more than 40–100 GPa; while brittle, it shows the ability to self-heal upon rupture, can be reversibly reshaped, and sustains complex shapes. We anticipate such an unusual 2D carbon nanomaterial to inspire novel approaches towards the formation of synthetic cells with rigid shells, additive manufacturing of composites, and compartmentalization in industrial catalysis.

Hierarchically Porous MOFs Synthesized by Soft-Template Strategies.

The past few decades have been witnessing the rapid research boom of metal-organic frameworks (MOFs), which are assembled from metal nodes and multitopic organic linkers. In virtue of their modular assembly mode, they can be tailored according to desired functions to satisfy numerous potential applications. However, most initially reported MOFs were restricted to the microporous regime, limiting their practical applications with bulk molecules involved. Therefore, the research attention was immediately directed toward enlarging the intrinsic pore size of frameworks by extending the secondary building units or organic ligands. Unfortunately, the synthesis of more extended ligands is frequently tedious, and the most resultant MOFs are not sufficiently stable, restricting their popularization. The soft-template strategy is recognized as a promising avenue to produce hierarchically porous MOFs (HPMOFs), although early attempts generally failed due to the incompatibility between the surfactant self-assembly and guided crystallization process of MOF precursors in the organic phase. Therefore, developing a rational soft-template strategy to achieve the precise control of morphology and porosity of HPMOFs is of great significance.In this Account, we present our recent progress on the development and applications of HPMOFs prepared by soft-template strategies. We highlight the key issues upon using the soft-template strategy to synthesize HPMOFs. To enhance the interaction between the template and MOF precursor, a long-chain monocarboxylic acid strategy is introduced to synthesize HPMOFs with irregular mesopores in the organic phase. Then, to improve the order of mesopores, an aqueous-phase synthesis method using amphoteric surfactants as templates is developed to prepare ordered HPMOFs. To further enlarge the pore size and make the synthesis conditions of MOFs compatible with the self-assembly of surfactants, a salting-in species-induced self-assembly strategy is proposed and coupled with the structure-directing properties of copolymer templates to synthesize a series of HPMOFs with large mesopores and even macropores. This salting-in ion-mediated self-assembly (SIMS) strategy paves the way to modify the pore size, pore structure, morphology, and chemical composition of HPMOFs. The separated but intimately interconnected hierarchical pores in the resultant HPMOFs can not only realize rapid mass transport but also isolate different-size guest molecules so that they are competent for a broad range of applications including protein digestion, cascade catalysis, enzyme-assisted substrate sensing, and DNA cleavage. Finally, the limitations, challenges, and future developments of this rapidly evolving field are described. This Account with a highlight to the soft-template strategies not only provides interesting insights to understand the assembly process between templates and MOFs but also inspires an optimization of the properties of HPMOFs from diverse aspects for desired applications.

Alkane-tolerant worm-like micelles based on assembled surfactants

Self-assembly of surfactants in aqueous solution can form a variety of aggregate structures, among which worm-like micelles (WLMs) have attracted much attention due to their excellent viscoelasticity. The addition of oil often leads to a decrease in the viscosity of WLMs, which is closely related to the location of oil dissolution within the WLMs. Whether oil could induce a viscosity increase in WLMs caught our attention. In order to explore the effect of alkanes on the microstructure of different WLMs systems, three WLMs systems were prepared using three surfactants: oleic acid-N,N-dimethylcyclohexylamine (OA-DMCHA), sodium oleate-chlorinated sodium (NaOA-NaCl) and cetyltrimethylammonium bromide-sodium salicylate (CTAB-NaSA). The changes of parameters such as viscosity, microstructure of these systems before and after the introduction of alkanes were analyzed. The relationship between the alkane concentration and the interlayer spacing of the lamellar phase was investigated by small angle X scattering (SAXS). Except for OA-DMCHA, the structures of the other two systems were destroyed after the addition of alkanes. Considering the solubility of surfactants in organic alkanes, it was found that alkanes can enter the hydrophobic barrier layer of OA-DMCHA. The initial WLMs transformed into a lamellar phase, and the interlayer spacing of the lamellar phase increased with increasing alkane concentration.

Mesomorphic Polymer Hydrogel Stabilizing Ionic Surfactant Self-Assembly for Fuel Cells

Lyotropic self-assembly of ionic surfactants benefits the construction of ion-conductive pathways but suffers from poor mechanical stability owing to the intrinsic fluidity. Here, a novel mesomorphic polymer hydrogel, featuring a porous network of the cross-linked polymer trapping lyotropic self-assembly of ionic surfactants, is presented for fuel cells. The mesomorphic hydrogel, which is facilely derived from radical polymerization of an acrylamide monomer and a cross-linker in an aqueous solution of 1-tetradecyl-3-methylimidazolium hydrogen sulfate, exhibits not only a lamellar lyotropic liquid crystal phase but also reversible tensile, compressive, and shear deformations. Macroscopic alignment of the mesomorphic hydrogel is achieved by low-frequency shear, and ionic conductivity is promoted to 166 mS cm–1 by virtue of the aligned ion-conductive channels. A hydrogen fuel cell is fabricated from the mesomorphic polymer hydrogel, and a peak power density of 48 mW cm–2 is achieved. Overall, this work provides a strategy to endow functional lyotropic self-assembly with mechanical strengths for diverse electrochemical applications.