Self-assembly Process Research Articles

Synergistic regulation of dual thresholds: Hydroxyl occupancy and carbon species in the targeted catalytic hydrocracking of lignite

The preparation of carbon-based catalyst supports from low-grade lignite, followed by its self-catalytic hydrocracking to produce lignite-derived aromatic compounds, is crucial for achieving efficient lignite utilization and expanding aromatic compound sources. During lignite catalytic hydrocracking, the uncontrolled diffusive migration of active hydrogen (H*) and insufficient protection of aromatic rings reduce the yield of aromatic compounds. Using Heishan lignite as the raw material, we employed a relay process of thermal-induced self-assembly and oxidation-mediated carbon distortion for fabricating the Co3O4/AC&GC-S-600 composite material, which features an optimal hydroxyl occupancy ratio and a balanced combination of amorphous carbon/graphite carbon (AC/GC) types. The optimal hydroxyl occupancy threshold balances Co3O4 dispersion and hydrophilicity, facilitating the efficient formation and directional migration of H* through synergistic interaction between Co3O4 and H2O. The adequate threshold of AC/GC ratio regulates substrate adsorption, activation, and inhibition of aromatic hydrogenation, enhancing selective C–O bridge bond cleavage and preserving the unsaturation of aromatic rings. The synergistic regulation of dual thresholds promotes the rapid formation and the directional migration of H*, enabling efficient conversion of Heishan lignite to aromatic compounds (45.8% conversion, 80.8% selectivity) under mild conditions. Characterization techniques, experimental analyses, kinetic studies, and density functional theory calculations confirm that thermally induced self-assembly and oxidation-mediated carbon distortion are crucial for redistributing the carbon framework of the Heishan lignite matrix and regulating the optimal dual thresholds of hydroxyl occupancy and AC/GC types, which are essential for the catalytic hydrocracking of Heishan lignite to aromatic compounds. This strategy provides a scientific basis for selective catalytic production of lignite-based aromatic compounds, thereby supporting its clean and efficient utilization.

Stimulated Pickering emulsion stabilized by binary particles with contrasting wettability and trace surfactant

The investigationof self-assembled particle structures at fluid interfaces has gained considerable interest across various fields. In particular, Pickering emulsions (PEs) stabilized by binary particles co-assembling at these interfaces have attracted even more attention. To explore the self-assembly process of superhydrophobic and superhydrophilic particles at oil–water (O/W) interfaces influenced by a trace amount of surfactant, a series of experiments were conducted. A small quantity (0.01 mmol·L−1) of dodecyltrimethylammonium bromide (DTAB) was introduced, establishing a variable stable emulsion system with high salt tolerance, capable of withstanding up to 6 mol·L−1 NaCl, in synergism with the particles. The DTAB concentration required to stabilize the O/W emulsion with particles was as low as 0.001 mmol·L−1. The stability and type of the resulting emulsion could be adjusted by varying the ratio of hydrophobic to hydrophilic particle (R) or by modifying acid/base conditions. The systems exhibited robust cyclic acid/base regulated demulsification and phase inversion behavior, maintaining stability over at least 10 cycles. Results indicated that the stability and nature of the emulsion were influenced by the curvature of the interface formed by the self-assembled interfacial particle structures, arising from the competitive adsorption of both types of particles and trace surfactant. Further analysis revealed a correlation between interfacial curvature and the surface charges of the particles, which could be modulated through DTAB adsorption. This study elucidated the behavior of hydrophilic and hydrophobic particle self-assembly at interfaces, provided a straightforward strategy for co-preparing switchable emulsions using superhydrophilic and superhydrophobic particles, and expanded the range of amphiphilic particles available for producing PEs. This approach presents significant potential for future research and applications in the field of PEs.

Optically active persistent luminescence in supramolecular nanoassemblies constructed from entirely achiral building blocks

Optically active persistent luminescent materials have attracted significant attention due to their distinctive luminescent characteristics and ability to exhibit rich circular polarization information. Despite extensive efforts to develop circularly polarized persistent luminescence (CPPL) materials using chiral molecules or polymers, fabricating CPPL materials from achiral units remains a big challenge. In this work, we introduce an efficient co-assembly strategy to create CPPL materials using entirely achiral organic molecules. The optical activities of co-assembled complexes are attributed to structural chirality, which arises from chiral nanohelices formed during symmetry breaking in the self-assembly process of C3-symmetric molecules. Achiral molecules with long-lasting phosphorescence can adhere to these chiral nanostructures via hydrogen bonding, and during the drying phase, form nanocrystals that align along helical fibers, resulting in circularly polarized, long-lasting phosphorescence. Enhanced CPPL efficiency, ranging from blue to yellow with a dissymmetry factor over 1.2 × 10−2 and lifetime of up to 0.6 s at room temperature, is achieved through hydrogen bonding driven co-assembly. Additionally, the CPPL spectra of these co-assemblies are captured using a homemade time-resolved circularly polarized long afterglow detection platform. This study not only presents a new approach for the high-efficiency design of CPPL materials from achiral building blocks but also significantly broadens the research possibilities in real-time CPPL analysis, offering a horizon in the exploration of CPPL materials.

Visualizing supramolecular assembly behavior, stimulus response, and solid state emission of higher-order Pt2+ aggregates.

Here, we present the first instance of a highly efficient red tetramer aggregate with tunable emission based on a cationic platinum(II) complex in conjunction with a silver cluster anion counterpart. This system exhibits multicolor emission response behaviors, which can be conveniently and directly detected through spectroscopic analysis, showcasing intriguing luminescence changes. The self-assembly of Pt⋯, π-π, and hydrogen bonding interactions not only enables an intriguing color adjustment from green to yellow emission, and eventually to red emission, but also demonstrates the co-existence of the monomer, excimer, and aggregation. These phenomena are further accompanied by well-defined nanostructures. The self-assembly process of these structures exhibits an isodesmic growth mechanism, which is dependent on temperature. In this regard, it exhibits potential applicability in multi-mode logic gates that rely on external stimuli such as concentration, solvent, and temperature. The sensitivity of the aggregates towards chemical stimuli combined with their exceptionally bright emission characteristics renders them suitable for diverse applications including solid-state lighting sensing mechanisms and anticounterfeiting measures. The multi-stimuli responsive phosphorescence and self-assembly behaviors of the cationic platinum(II) complex were substantiated by X-ray crystal structure determination, 1H NMR analysis spectroscopic investigations, computational calculations and scanning electron microscopy (SEM) studies.

Principles and Biomedical Applications of Self-Assembled Peptides: Potential Treatment of Type 2 Diabetes Mellitus

Type 2 diabetes mellitus (T2DM) is the most prevalent metabolic disorder worldwide. There have been tremendous efforts to find a safe and prolonged effective therapy for its treatment. Peptide hormones, from certain organisms in the human body, as the pharmaceutical agents, have shown outstanding profiles of efficacy and safety in plasma glucose regulation. Their therapeutic promises have undergone intensive investigations via examining their physicochemical and pharmacokinetic properties. Their major drawback is their short half-life in vivo. To address this challenge, researchers have recently started to apply the state-of-the-art molecular self-assembly on peptide hormones to form nanofibrillar structures, as a smart nanotherapeutic drug delivery technique, to tremendously enhance their prolonged bioactivity in vivo. This revolutionary therapeutic approach would significantly improve patient compliance. First, this review provides a comprehensive summary on the pathophysiology of T2DM, various efforts to treat this chronic disorder, and the limitations and drawbacks of these treatment approaches. Next, this review lays out detailed insights on various aspects of peptide self-assembly: adverse effects, potential applications in nanobiotechnology, thermodynamics and kinetics of the process, as well as the molecular structures of the self-assembled configurations. Furthermore, this review elucidates the recent efforts on applying reversible human-derived peptide self-assembly to generate highly organized smart nanostructured drug formulations known as nanofibrils to regulate and prolong the bioactivity of the human gut hormone peptides in vivo to treat T2DM. Finally, this review highlights the future research directions to advance the knowledge on the state-of-the-art peptide self-assembly process to apply the revolutionary smart nanotherapeutics for treatment of chronic disorders such as T2DM with highly improved patient compliance.

Host-Guest Adduct as a Stimuli-Responsive Prodrug: Enzyme-Triggered Self-Assembly Process of a Short Peptide Within Mitochondria to Induce Cell Apoptosis.

To address the issue of nonspecific biodistribution of a chemotherapeutic drug, stable [2]pseudorotaxane complexes (PK@CAOPP and PR@CAOPP) are used to demonstrate a proof of concept. Cationic -PPh3 + moiety in CAOPP allows specific localization of the PK@CAOPP/ PR@CAOPP in the mitochondrial membrane (MM). Electrostatic interaction between the cationic LysinePK or ArgininePR moiety and the negatively charged phosphoesterCAOPP functionality in CAOPP favours strong adduct formation. The ALP-induced hydrolytic cleavage of the phosphoester moiety in cancer cells triggers dephosphorylation and releases PK/ PR moiety from PK@CAOPP/PR@CAOPP. PK or PR, derived from the Phe-Phe dipeptide, formed fibril-like molecular aggregates in the MM to induce dysfunction, depolarization, ROS generation and apoptotic MCF7 cell death. Such phenomena were not observed in ALP-negative HEK293 normal cells. These propositions were confirmed through control studies using NBDK and PE, other guest molecules. Smaller size and inclusion of the short peptides (PK or PR) within the hydrophobic interior of CAOPP, were attributed to their stability in blood serum. Thus, we have demonstrated the use of supramolecular adducts as a potential therapeutic option for treating cancer cells without affecting healthy cells. The efficacy was also established with an in-vivo MCF7 tumour xenograft model using Balb/c nude mice.

Molecularly imprinted electrochemical sensor based on APTES-functionalized indium tin oxide electrode for the determination of sulfadiazine.

Anelectrochemical sensor was developedfor the sensitive and selective detection of sulfadiazine(SDZ), based on a molecularly imprinted polymer (MIP) film formed on an indium tin oxide (ITO) electrode through a self-assembly process. The SDZ-imprinted ITO electrode (SDZ-MIP/APTES-ITO) was prepared through in situ polymerization using sulfadiazine, methacrylic acid (MAA), ethylene glycol dimethacrylate (EGDMA), and 2,2'-azobisisobutyronitrile (AIBN) as the template, functional monomer, cross-linker, and initiator respectively. Before polymerization, the ITO electrode was functionalized with 3-aminopropyltriethoxysilane (APTES) to promote covalent attachment of the polymer to the electrode. After polymerization, the template molecule SDZ was removed to create selective recognition sites, forming the molecularly imprinted polymer electrode (MIP/APTES-ITO), which facilitates sulfadiazine detection. The sensor's performance was evaluated using cyclic and differential pulse voltammetry, demonstrating a linear response in the sulfadiazine concentration range 0.1 to 300μM, with a detection limit of 0.11μM. The MIP-based sensor exhibited goodreproducibility, repeatability, selectivity, and stability in sulfadiazine detection. Its practical applicability was confirmed by the successful quantification of sulfadiazine in spiked milk samples.

Bio-sourced flexible supramolecular glasses for dynamic and full-color phosphorescence

Glass, a diverse family of amorphous materials, has significantly advanced human society across various fields. The demand for flexible ultrathin glass, driven by modern optical displays and portable optoelectronics, presents challenges in energy consumption, fabrication complexity, and recycling. Here, we demonstrate flexibility and full-color luminescence in large-scale ultrathin glasses derived from readily available natural resources, specifically egg albumen (EA) and gelatin (GEL), via an evaporation-driven self-assembly process. The dynamic crosslinked networks formed through hydrogen bonding between EA and GEL impart both high hardness and flexibility to the glasses, with hardness and flexural strength values comparable to state-of-the-art inorganic and organic glasses. Additionally, the EA–GEL-based glasses exhibit excitation-dependent and time-gated chiral ultralong phosphorescence with color from blue and red, and a lifetime of up to 180.4 ms. With their easy processability and full-color emission, these biogenic glasses can be fabricated into anti-counterfeiting patterns and optical information codes.

Pioneering SubPc-Br/CdS S-scheme heterojunctions: Achieving superior photocatalytic oxidation through enhanced radical synergy and photocorrosion mitigation

For the efficient harnessing of solar energy and mitigation of environmental pollution, the development and application of semiconductor photocatalysis technology is paramount. Herein, a novel SubPc-Br/CdS supramolecular array with an S-scheme heterojunction was synthesized through the intermolecular π-stacked self-assembly of subphthalocyanine (SubPc-Br) and nanometer cadmium sulfide (CdS). This self-assembly system features a highly structured architecture and excellent stability. Experiments and ground-state differential charge calculations demonstrate that SubPc-Br and CdS form a built-in electric field during the self-assembly process, a critical factor in promoting the dissociation of electrons and holes. Additionally, this study utilized time-dependent density functional theory (TDDFT) to simulate the dynamic adsorption behavior of excited oxygen molecules on the SubPc-Br/CdS interface for the first time. The analysis of molecular charge differential density under different excited states proved that the addition of SubPc-Br molecules not only improves the photocorrosion resistance of CdS in an O2 adsorption environment but also enhances the production of advanced reactive oxygen species under the synergistic action of h+ and ·O2–. When subjected to visible light, the degradation efficiency of minocycline (MC) achieved 96.8% within 60 min and maintained 80.3% after 5 cycles. In summary, this study highlights the feasibility of creating advanced S-scheme heterojunction photocatalysts through the strategic incorporation of organic supramolecules with semiconductor catalysts.

Induction of multicomponent peptide assembly via solvent exchange strategy for enhanced structure and bioactivities

Multicomponent peptides, composed of numerous peptides with various binding sites and functionalities, are increasingly exploited in nanotechnology, biomedicine and functional food applications. This article reported that nucleation and growth of Zein (Z) during solvent exchange could form a confined space to drive spontaneous self-assembly of multicomponent peptides. The self-assembly process began with a concentration gradient generated by the exchange of water and ethanol driving the nucleation of Z to form small aggregates, while multicomponent peptides selectively or anisotropically adsorbed on the Z surface via electrostatic interactions and hydrophobic interactions, participating in and controlling the assembly kinetics, ultimately leading to the formation of well-defined nanoparticles (NPs). The multicomponent peptides-based assemblies could effectively encapsulate the hydrophobic functional agent quercetin (Que), presenting good biocompatibility, antioxidant activity, and preventing DSS-induced colitis. This study elucidated the self-assembly mechanism of multicomponent peptides and demonstrated their synergistic effects with hydrophobic compounds for disease prevention, offering valuable insights into the development of novel functional materials to regulate human health.

Insight into interfacial dynamics of photogenerated carriers in Cs3Bi2I9/Au heterostructure nanocomposites for high-sensitivity broadband photodetection with negative photoconductivity

The negative photoconductivity (NPC) effect is becoming an increasingly significant factor in the development of next-generation optoelectronics. However, research in the field of NPC-dominated optoelectronics remains in its infancy and frequently encounters challenges related to fabrication complexity, slow photoresponse speed, instability, and a limited spectral response range. Herein, a Cs3Bi2I9/Au heterostructure nanocomposite was prepared via a simple self-assembly process utilizing electrostatic interactions with Au nanoparticles (NPs) and lead-free Cs3Bi2I9 nanoplates. The Cs3Bi2I9/Au nanocomposite-based photodetectors (PDs) demonstrate a broadband photoresponse (405–1550 nm), enhanced rise/fall times (27.2/40.0 µs), and reduced noise density (4.7 × 10−13 A/Hz1/2 at 1 Hz). In contrast to the positive photoconductivity (PPC) effect observed in colloidally synthesized Cs3Bi2I9 nanoplate-based PDs, the NPC can be attributed to the decrease in photocurrent under light illumination during the processes of recombination and trapping of photogenerated carriers induced by the incorporation of Au NPs. These findings are expected to provide valuable insights into achieving high-performance NPC-dominated PDs by regulating the dynamics of photogenerated carriers in perovskite heterostructures.

Route to Measure Exact Parameters of Bio-Nanostructures Self-Assembly

Artificial bio-nanocoatings, primarily composed of proteins, offer a broad range of applications across various fields thanks to their unique properties. Proteins, as major components of these structures, enable a high degree of customization, such as mutations, conjugation with other molecules or nanoparticles, or the inclusion of an enzymatic activity. Their ability to self-assembly simplifies the production of bio-nanocoatings, making this process efficient and environment-friendly. Despite these advantages, a comprehensive understanding of the underlying self-assembly mechanism is lacking, and the reaction rates governing this process have not been characterized. In this article, we introduce a novel method to determine the key parameters describing the self-assembly mechanism of bio-nanostructures. For the first time, this approach enables an accurate calculation of the autocatalytic and self-inhibitory parameters controlling the process. Through mathematical modeling, our method enhances the understanding of how the protein-based nanocoatings form and opens new avenues for their application in nanotechnology and synthetic biology. Improved control over the self-assembly processes may enable the development of nanomaterials optimized for specific functions, such as drug delivery, biosensing, and bioactive surface fabrication.

Substrate as the primer of relay-race spin-driven self-assembly of chiral molecules

The molecules of chiral N-trifluoroacetylated α-aminoalcohols can self-assemble and form long and thin fiber-like supramolecular structures (strings). The strings effectively grow on the surface of the substrate and the amount of them, as well as their morphology, depend on the properties of the substrate. In particular, self-assembly was not observed on the electroconductive substrates, such as some metals (copper and aluminum) and graphite. The strings were found on the surface of titanium due to the peculiarities of the titanium oxide’s properties. The strings usually emanate from some nucleation zones, where the growth was initiated and then proceeded spontaneously outside these areas. We supposed the relay-race scheme of the transfer of spin polarization, which describes the mechanics and thermodynamics of the observed self-assembly process. The scheme implies the preliminary orientation of two molecules, their mutual polarization accompanied by spin-polarization, and finally the binding of the molecules. We also suppose this mechanism can play a significant role in various self-assembly processes in living cells.

Polymerization-induced Chiral Self-assembly for the In situ Construction, Modulation, Amplification and Applications of Asymmetric Suprastructures.

In the polymerization-induced chiral self-assembly (PICSA) process, chiral functional monomers undergo spontaneous supramolecular self-assembly and asymmetric stacking during living polymerization, leading to the in situ generation of chiroptical polymer assemblies characterized by diverse morphologies. The PICSA strategy facilitates precise control and manipulation of both non-covalent supramolecular helices and covalent macromolecular helices within aggregated cores, thereby driving significant advancements in fields such as chiral recognition materials, asymmetric catalysts, nonlinear optical materials, and ferroelectric liquid crystals (LC). This minireview summarizes recent developments in the in situ chiroptical construction and modulation associated with the PICSA methodology. Furthermore, it seeks to elucidate emerging PICSA systems founded on various living polymerization mechanisms, exploring hierarchical chirality transfer processes and the pathway complexities in both equilibrium and non-equilibrium conditions. This minireview also presents several illustrative examples that demonstrate the practical applications of chiral polymer materials synthesized through the PICSA approach, thereby illuminating future opportunities in this innovative field.

Suppressing Static and Dynamic Disorder for High-Efficiency and Stable Thick-Film Organic Solar Cells via Synergistic Dilution Strategy.

Developing stable and highly efficient thick-film organic solar cells (OSCs) is crucial for the large-scale commercial application of organic photovoltaics. A novel synergistic dilution strategy to address this issue, using Polymethyl Methacrylate (PMMA) -modified zinc oxide (ZnO) as the interfacial layer, is introduced. This strategy effectively mitigates oxygen defects in ZnO while also regulating the self-assembly process of the active layer to achieve an ordered distribution of donors and acceptors. In synergistic diluted devices, the dynamic disorder is reduced owing to the suppression of electron-phonon coupling, while the static disorder is suppressed by improved molecular stacking and enhanced intermolecular interactions. Consequently, the 300nm PM6:L8-BO device post-synergistic dilution manifests a marked enhancement in device performance, achieving a photovoltaic power conversion efficiency (PCE) >17% with excellent thermal stability. A typical ternary system is selected to explore the general applicability of synergistic dilution strategy, the PCE has been enhanced significantly from 17.89% to 18.72%, which falls within the range of the highest values among inverted single junction OSCs. As a practical application that depends on the pivotal synergy between high efficiency and stability, this approach paves the way for large-scale implementation of OSCs and ensures cost-effectiveness.

Preferential Binding of Cations Modulates Electrostatically Driven Protein Aggregation and Disaggregation.

Protein aggregation resulting in either ordered amyloids or amorphous aggregates is not only restricted to deadly human diseases but also associated with biotechnological challenges encountered in the therapeutic and food industries. Elucidating the key structural determinants of protein aggregation is important to devise targeted inhibitory strategies, but it still remains a formidable task owing to the underlying hierarchy, stochasticity, and complexity associated with the self-assembly processes. Additionally, alterations in solution pH, salt types, and ionic strength modulate various noncovalent interactions, thus affecting the protein aggregation propensity and the aggregation kinetics. However, the molecular origin and a detailed understanding of the effects of weakly and strongly hydrated salts on protein aggregation and their plausible roles in the dissolution of aggregates remain elusive. In this study, using fluorescence and circular dichroism spectroscopy in combination with electron microscopy and light scattering techniques, we show that the ionic size, valency, and extent of hydration of cations play a crucial role in regulating the protein aggregation and disaggregation processes, which may elicit unique methods for governing the balance between protein self-assembly and disassembly.

Multifunctional composite phase change material with electrostatic self-assembly structure based on carboxylated multi-walled carbon nanotubes

The need for improved thermal regulation in electronic devices and solar thermal energy storage, prompted by the energy crisis, has expedited the advancement of phase change materials (PCMs). Carboxylated multi-walled carbon nanotubes (MWCNT-COOH) were produced by introducing carboxyl functional groups onto MWCNTs utilizing a concentrated acid treatment. The novel composite was engineered through an electrostatic self-assembly process between the negatively charged MWCNT-COOH and the positively charged Poly dimethyl diallyl ammonium chloride (PDDA) solution, filling the structure with the PCM polyethylene glycol (PEG) and incorporating the (magnesium hydrate) Mg(OH)2 to enhance the material's flame resistance at high temperatures. The thermal conductivity of the obtained composites improved significantly from 0.25 W/m·K to 1.183 W/m·K, while maintaining an enthalpy of phase transition of phase change of 135.1 J/g. Owing to the capillary effect of the closely packed MWCNT-COOH tubular structure, the composite material exhibited excellent high-temperature shape retention ability. Additionally, the composite demonstrated high absorption with an absorbance reaching 1.18 L/(g·cm) and composite materials can convert up to 86.8 % of light energy into heat energy.

Megamolecule Self-Assembly Networks: A Combined Computational and Experimental Design Strategy.

This work describes the use of computational strategies to design megamolecule building blocks for the self-assembly of lattice networks. The megamolecules are prepared by attaching four Cutinase-SnapTag fusion proteins (CS fusions) to a four-armed linker, followed by functionalizing each fusion with a terpyridine linker. This functionality is designed to participate in a metal-mediated self-assembly process to give networks. This article describes a simulation-guided strategy for the design of megamolecules to optimize the peptide linker in the fusion protein to give conformations that are best suited for self-assembly and therefore streamlines the typically time-consuming and labor-intensive experimental process. We designed 11 candidate megamolecules and identified the most promising linker, (EAAAK)2, along with the optimal experimental conditions through a combination of all-atom molecular dynamics, enhanced sampling, and larger-scale coarse-grained molecular dynamics simulations. Our simulation findings were validated and found to be consistent with the experimental results. Significantly, this study offers valuable insight into the self-assembly of megamolecule networks and provides a novel and general strategy for large biomolecular material designs by using systematic bottom-up coarse-grained simulations.

Quantifying Interface-Performance Relationships in Electrochemical CO2 Reduction through Mixed-Dimensional Assembly of Nanocrystal-on-Nanowire Superstructures.

Fine-tuning the interfacial sites within heterogeneous catalysts is pivotal for unravelling the intricate structure-property relationship and optimizing their catalytic performance. Herein, a simple and versatile mixed-dimensional assembly approach is proposed to create nanocrystal-on-nanowire superstructures with precisely adjustable numbers of biphasic interfaces. This method leverages an efficient self-assembly process in which colloidal nanocrystals spontaneously organize onto Ag nanowires, driven by the solvophobic effect. Importantly, varying the ratio of the two components during assembly allows for accurate control over both the quantity and contact perimeter of biphasic interfaces. As a proof-of-concept demonstration, a series of Au-on-Ag superstructures with varying numbers of Au/Ag interfaces are constructed and employed as electrocatalysts for electrochemical CO2-to-CO conversion. Experimental results reveal a logarithmic linear relationship between catalytic activity and the number of Au/Ag interfaces per unit mass of Au-on-Ag superstructures. This work presents a straightforward approach for precise interface engineering, paving the way for systematic exploration of interface-dependent catalytic behaviors in heterogeneous catalysts.

Scalable fabrication of flexible 3D PEDOT/rGO Scaffold for high-performance supercapacitors via a self-assembly method

Conducting polymers hold great prospects in energy storage, especially in the field of flexible energy storage, however, their broad applications are limited due to the poor processability, difficulty in structural design diversity and unsatisfactory performance when used alone. Herein, the processability of PEDOT in organic phase is significantly enhanced by surfactant modification via a self-assembly process, contributing to the convenient and low-cost construction of 3D PEDOT architecture. Importantly, the PEDOT and rGO can be introduced into the same porous structure synchronously and conveniently. Superior capacitive performance is shown for the porous PEDOT/rGO film benefits from the combination of PEDOT with excellent electrochemical stability, rGO with high conductivity and porous structure with abundant active sites and chambers for electrolyte storage. The porous PEDOT/rGO film can be used as a scaffold for the deposition of conductive polymers. For example, once PPy is deposited, a high specific capacitance of 407.8 F g-1 at a current density of 0.5 A g-1, accompanied by a prominent capacitance retention of 90% after 5000 cycles are achieved. When it is used to construct the symmetric supercapacitor (SSC), a high energy density of 52.9 Wh kg-1 at the power density of 200.2 W kg-1 is delivered, with a high capacitance retention of 85%. Moreover, it shows excellent mechanical flexibility upon multiple bending cycles, rendering great potential in portable or wearable energy storage devices.