Evaporation-induced Self-assembly Research Articles

One‐pot synthesis of CuO/TiO2 nanocomposites for improved photocatalytic hydrogenation of 4‐nitrophenol to 4‐aminophenol under direct sunlight

AbstractThe excellent photocatalytic hydrogenation of 4‐nitrophenol (4‐NP) to 4‐aminophenol (4‐AP) with NaBH4 in the aqueous medium is still a big challenge. Herein, we report a facile one‐pot evaporation‐induced self‐assembly (EISA) method to synthesize a series of CuO/TiO2 nanocomposites. The as‐synthesized CuO/TiO2 photocatalysts exhibit remarkable catalytic activity under direct sunlight in selective hydrogenation of 4‐nitrophenol (4‐NP) to 4‐aminophenol (4‐AP) due to the synergistic interaction of guest copper nanoparticles with host titanium dioxide (TiO2) species. Especially, 5 wt% CuO/TiO2 nanocomposite revealed superior reaction rate constant (k) value (0.306 min−1) when compared to 3 wt% CuO/TiO2 (0.192 min−1) and 7 wt% CuO/TiO2 (0.240 min−1). Moreover, several characterization techniques (XRD, TEM, N2 adsorption–desorption isotherm, DRS, and XPS) were executed to deeply investigate the effect of copper content on the bulk and interfacial properties of the catalysts. The characterization results proved that the superior photocatalytic hydrogenation over 5 wt% CuO/TiO2 catalyst can be ascribed to moderate CuO loading as well as even dispersion of CuO species on the surface of active TiO2 host, which can largely improve the light absorption ability within visible light region. Besides, the 5 wt% CuO/TiO2 catalyst exhibits remarkable recyclability and durability, retaining its superior activity (above 95%) up to several repeating cycles, proving its practical applicability for hydrogenation reactions at domestic and industrial levels.

Mesostructured γ-Al2O3-Based Bifunctional Catalysts for Direct Synthesis of Dimethyl Ether from CO2

In this work, we propose two bifunctional nanocomposite catalysts based on acidic mesostructured γ-Al2O3 and a Cu/ZnO/ZrO2 redox phase. γ-Al2O3 was synthesized by an Evaporation-Induced Self-Assembly (EISA) method using two different templating agents (block copolymers Pluronic P123 and F127) and subsequently functionalized with the redox phase using an impregnation method modified with a self-combustion reaction. These nanocomposite catalysts and their corresponding mesostructured supports were characterized in terms of structural, textural, and morphological features as well as their acidic properties. The bifunctional catalysts were tested for the CO2-to-DME process, and their performances were compared with a physical mixture consisting of the most promising support as a dehydration catalyst together with the most common Cu-based commercial redox catalyst (CZA). The results highlight that the most appropriate Pluronic for the synthesis of γ-Al2O3 is P123; the use of this templating agent allows us to obtain a mesostructure with a smaller pore size and a higher number of acid sites. Furthermore, the corresponding composite catalyst shows a better dispersion of the redox phase and, consequently, a higher CO2 conversion. However, the incorporation of the redox phase into the porous structure of the acidic support (chemical mixing), favoring an intimate contact between the two phases, has detrimental effects on the dehydration performances due to the coverage of the acid sites with the redox nanophase. On the other hand, the strategy involving the physical mixing of the two phases, distinctly preserving the two catalytic functions, assures better performances.

Scalable Manufacturing of Mechanical Robust Bioinspired Ceramic-Resin Composites with Locally Tunable Heterogeneous Structures.

Lightweight structural materials with a unique combination of high stiffness, strength, toughness, and hardness, are highlydesired yet challenging to be artificially fabricated. Biological structural materials, on the other hand, ingeniously integrate multiple mutually exclusive mechanical properties together relying on their hierarchically heterogeneous structures bonded with gradient interfaces. Here, a scalable bottom-up approach combining continuous nanofiber-assisted evaporation-induced self-assembly with laminating, pressure-less sintering and resin infiltration is reported to fabricate bioinspired heterogeneous ceramic-resin composites with locallytunable microstructure to fulfill specific properties. A gradient interlayer isintroduced to provide a gradual transition between adjacent heterogeneous layers, effectively alleviating their property mismatch. The optimized heterogeneous nacre-like composite, as a demonstration, exhibits an attractive combination of low density (≈2.8gcm-3 ), high strength (≈292MPa), toughness (≈6.4MPam1/2 ), surface hardness (≈1144 kgfmm-2 ) and impact-resistance, surpassing the overall performance of engineering alumina. This material-independent approach paves the way for designing advanced bioinspired heterogeneous materials for diverse structural and functional applications.

Boosting solar-driven N2 to NH3 conversion using defect-engineered TiO2/CuO heterojunction photocatalyst

Ammonia (NH3) is one of the important energy sources for sustainable chemical products and carbon-free energy carriers. Artificial N2 photofixation is one of the promising approaches for the clean production of NH3 using photocatalysts in N2-dissolved water as a hydrogen source. We prepared defect-engineered TiO2/CuO heterojunction photocatalysts by the simple evaporation-induced self-assembly (EISA) method followed by post-thermal annealing under inert gas flow. The formation of a type-Ⅱ using TiO2 and CuO facilitated light absorption in near IR to UV light and the separation of photoexcited electron-hole pairs. In addition, the further post-thermal annealing under N2 gas flow resulted not only in an increase in crystallinity for the photoactive Anatase TiO2 and Tenorite CuO in the bulk but also in the in-situ formation of Ti3+ defect sites on the TiO2 surface. The increased crystallinity enhanced the photoexcited charge transport, while the defect sites improved N2 adsorption and activation, promoting the photocatalytic conversion of N2 to NH3. The defect-engineered TiO2/CuO photocatalysts exhibited a high NH3 production rate (1.575 μ mol g−1h−1) under visible light irradiation (λ≥ 420 nm) without any sacrificial agent, this value is 9.4 times and 2.5 times higher than those obtained with pristine TiO2 and TiO2/CuO photocatalysts, respectively. This work clearly demonstrates the synergistic effect of heterojunction and defect-engineering and provides insights into how each strategy can affect solar-driven NH3 production.

Solvent-Free Catalytic Hydrotreatment of Alcell Lignin Using Mono- and Bimetallic Ni(Mo) Catalysts Supported on Mesoporous Alumina

Technical lignins are an attractive and renewable source for the production of aromatic chemicals. However, efficient depolymerization of technical lignins to valuable low-molecular-weight chemicals is challenging due to its recalcitrant nature. Here, we report the use of nonprecious metal-based, monometallic Ni (prereduced) and bimetallic NiMo (in situ sulfided) catalysts supported on mesoporous alumina, either as such or doped with Si, Mg, or Ti, for a solvent-free catalytic hydrotreatment (batch, 400 °C, 4 h reaction time, 100 bar initial H2 pressure) of Alcell lignin to obtain oils enriched in biobased chemicals like alkylphenols and the parent phenol. These are important building blocks in the chemical industry and are currently obtained from fossil resources. The catalysts were prepared by a one-pot evaporation-induced self-assembly (EISA) method and characterized by various techniques [N2 physisorption, X-ray diffraction (XRD), temperature-programmed desorption (TPD), temperature-programmed reduction (TPR), and transmission electron microscopy (TEM)]. The best result was obtained using a monometallic Ni catalyst with an ordered mesoporous alumina support doped with Ti, giving an oil yield of 57 wt % with 10 wt % alkylphenols on lignin intake. By comparison, it was shown that the mesoporous structure of alumina is crucial for enhanced lignin oil yields.

Effect of amorphous ordered mesoporous carrier on adsorption and desorption of Hg0 over CeOx-amTiO2

Improper disposal of deactivated mercury (Hg) adsorbents will cause secondary contamination which is still hazardous to human beings. Wet desorption is a green and environmentally friendly method, but there is a lack of sufficient study. In this work, a cerium oxide loaded ordered mesoporous amorphous titanium dioxide (CeOx-amTiO2) composite is obtained based on the evaporation-induced self-assembly (EISA) process. It possesses a high specific surface area (∼198 m2/g), uniform pore diameters (∼14.7 nm), and large pore volume (∼0.49 cm3/g). The CeOx-amTiO2 demonstrates high adsorption capacity in various atmospheres (63.3 % in pure N2, 95.0 % in N2 + 400 ppm H2S), and achieves a desorption efficiency of 93.2 % in 0.2 mol/L sodium thiosulfate (Na2S2O3) solution. The large specific surface area and ordered mesostructure significantly facilitate the mass transfer process, reasonably explaining the strong adsorption capacity and fast desorption kinetics. X-ray photoelectron spectroscopy (XPS) characterization and thermodynamic calculations reveal that the reduction of Ce3+ plays a key role in the desorption of Hg. In addition, the amorphous carrier structure reduces the binding strength between the adsorption product and the adsorbent, further accelerating the desorption process. This study provides a pathway for the efficient desorption of Hg0 removal adsorbents.

Ordered Hierarchical Porous Structure of PtSn/3DOMM-Al2O3 Catalyst for Promoting Propane Non-Oxidative Dehydrogenation.

Herein, the hierarchical porous catalyst of 3-dimensional ordered macro-mesoporous (3DOMM) Al2O3 supported active PtSn nanoparticles (NPs) was prepared by the combined synthesized path of evaporation-induced self-assembly with colloid crystal template (EISA-CCT) methods. The hierarchical macro-mesoporous composite structure can markedly increase the specific surface area, accommodate the diffusion of propene, and decrease the number of surface acid sites. In addition, the special surface property and pore structure of 3DOMM-Al2O3 can modify the interaction between metals and substrates, as well as stabilize the metal nanoparticle, which promotes the formation of a highly active and stable PtSn phase. The PtSn/3DOMM-Al2O3 catalyst exhibits higher productivity and stability than PtSn/Al2O3 catalysts with macropore and mesopore structures. The PtSn/3DOMM-Al2O3 catalyst displays the best catalytic performance with propylene selectivity over 95% at a propane conversion of 33.9%. The study of the ordered hierarchical porous structure of PtSn/3DOMM-Al2O3 catalysts can contribute to obtaining improved catalysts in industrial processes.

Bimetallic ordered mesoporous carbon from lignin for catalytic selective hydrogenation of levulinic acid to γ-valerolactone

Herein, a Ni/Ru bimetallic ordered mesoporous carbon (Ni/Ru@WOMC) was prepared through solvent evaporation induced self-assembly (EISA) method with walnut shell organosolv lignin as carbon precursor and Ni2+ as crosslinking agent followed by impregnating small amount of Ru, where the mass ratio of Ni/Ru was about 10:1. The resulting material showed superior catalytic activity on hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). A nearly 100 % GVL yield could be obtained in 2-propanol solvent under mild conditions at a low reaction temperature of 80 °C in 4 h reaction time. The Ni/Ru@WOMC catalyst could be used at least 5 times without obvious loss of its catalytic performance, which can be ascribed to the confinement effect provided by their ordered mesoporous structure. This successful development of Ni/Ru@WOMC in the hydrogenation of LA to GVL opens up new opportunities for the catalytic application of lignin derived functionalized ordered mesoporous carbon in biomass transformation reactions.

Cellulose nanocrystals-based bio-composite optical materials for reversible colorimetric responsive films and coatings

Photonic materials with a tunable chiral nematic structure that can selectively reflect light dynamically are valuable for applications in smart responsive materials. Here, we prepared potential photonic composites with a chiral nematic structure by forming cellulose nanocrystals (CNCs) and waterborne polyurethane (WPU) composites with different compositions on different substrates by evaporation-induced self-assembly. With increasing WPU content, the reflected wavelength increased from 400 to 680 nm, which was mainly caused by the increase of the chiral nematic pitch. In addition, the mechanical properties were better for higher WPU content. WPU was sensitive to small amounts of moisture in ethanol owing to the swollen WPU after absorbing water will increase the helical pitch. The reversible red shift induced by moisture was approximately 100 nm. When wood was used as the substrate, the CNCs still self-assembled to form chiral nematic structures and the adhesion forces of the composites to the wood substrate were strong. By using MgCl2 solution as an ink, invisible patterns can be written on the coating, which can be revealed temporarily by ethanol. In addition, the invisible pattern of photonic coating is rewritable. The easily prepared environmentally friendly photonic composite has great potential in sensors, anti-counterfeiting labels and smart decorative coatings.

Synthesis and Application of Mesoporous Materials: Process Status, Technical Problems, and Development Prospects: A Mini-Review

The world today is witnessing a new technological revolution, particularly in the area of new materials. Different types of materials often have different characteristics and uses. Mesoporous materials have a large specific surface area, easily modifiable inner and outer surfaces, tunable pore size and pore channels, and good biocompatibility and thermodynamic stability, thus emerging as a new candidate material in the chemical research community. The presence of mesopores facilitates the rapid diffusion of macromolecules, reduces resistance to mass transfer, and provides different properties depending on the pore size, making mesoporous materials a potential candidate for a wide range of applications. This paper reviews the recent methods used to synthesize mesoporous materials, including hydrothermal synthesis, microwave synthesis, the sol–gel method, the phase conversion method, and the templating method. The soft templating method is introduced in detail, including bulk self-assembly, solvent evaporation-induced self-assembly, solution-based nanoprecipitation, interfacial self-assembly in a solution, and emulsion template self-assembly. The current status of the processes related to mesoporous materials in the fields of biomedicine, environmental and energy, electrochemical energy storage, and gas separation is elaborated. Finally, the technical issues and future directions in the synthesis and application of mesoporous materials are briefly discussed.

Ordered mesoporous Ni-La2O3/Al2O3 catalysts towards efficient plasma-assisted dry reforming of methane

Plasma-assisted dry reforming of methane reaction provides a promising way to produce syngas with unity H2/CO ratio as one important chemical feedstock. Aiming to establish a match between CH4 and CO2 activation rates to suppress carbon deposition under combining plasma and catalyst, the design of reasonable and efficient catalytic materials is great of importance. Herein, we reported that the addition of La enhanced the reducibility of Ni2+ species and promoted Ni dispersion over the highly ordered mesoporous 10Ni5LaAl-one pot catalyst. In comparison to 10Ni5La/Al prepared by the incipient wetness impregnation (IWI) method and 10NiAl-one pot prepared by one pot solvent evaporation-induced self-assembly (EISA) method, the 10Ni5LaAl-one pot catalyst exhibited the highest catalytic activity for syngas production (H2/CO ratio of 0.98) and the strongest coke-resistance ability in the plasma-assisted DRM reaction. Meanwhile, excellent stability performance was obtained within 90 h for the catalyst owing to the higher discharge power, efficient capacitance and lower apparent activation energy of CO2 under plasma condition. And possible reaction mechanism of the10Ni5LaAl-one pot was proposed during plasma-catalytic DRM process.

Efficient Calcium Looping-Integrated Methane Dry Reforming by Dual Functional Aerosol Ca–Ni–Ce Nanoparticle Clusters

Calcium looping (CaL) integrated with methane dry reforming (DRM) shows promise for carbon capture and utilization. To enhance the CaL–DRM tandem processes, a raspberry-structured aerosol dual-functional material composed of CaO (CO2 adsorbent), Ni (DRM catalyst), and CeO2 (promoter) was fabricated via gas-phase evaporation-induced self-assembly. The utilization of Ca–Ni–Ce is highly beneficial by the creation of metal–support–promoter interaction for promoting an effective carbon capture followed by interfacial catalysis, providing an alternative pathway with enhanced redox ability and reduction of activation energy. The Ca–Ni–Ce composite materials with clustered particle characteristics showed great improvement in the performance of cyclic CaL–DRM in comparison to the reported values: low required carbonation/decarbonation temperatures (400/600 °C), high CO2 uptake efficiency (12.1 mmolCO2/gCaO), ultrahigh CO2 conversion (97.2%) under relatively low-temperature operation (600 °C), and sufficiently high operational stability. Overall, the proposed Ca–Ni–Ce hybrid material fabricated via the aerosol synthetic method demonstrates significant advances in the low-temperature CaL–DRM processes, showing promise as a sustainable chemical engineering route for industrial applications.

Evaporation-induced self-assembly of gold nanorods on a hydrophobic substrate for surface enhanced Raman spectroscopy applications

The controllable assembly of plasmonic nanoparticles has developed as one of the most significant approaches for surface enhanced Raman spectroscopy (SERS) applications. This study developed a simple approach to improve a large-scale ordered assembly of gold nanorods (GNRs) by controlling the droplet evaporation mode on hydrophobic substrates. The hydrophobic substrate was efficiently produced by spin coating the silicone oil onto the glass slides and annealing them. The analyte molecule rhodamine (R6G) was employed as a surface-enhanced Raman scattering probe to demonstrate the potential effects of the synthesized arrays. This hydrophobic platform enables the concentration and delivery of analyte molecules into the surface enhanced Raman spectroscopy sensitive site while suppressing the coffee ring effect generated by the smooth contraction motion of the base contact radius of the droplet without any pinning. Thus, the limit of detection (LOD) of the R6G analyte was lowered to 10−10 M and the homogenous dispersion of surface enhanced Raman spectroscopy hotspots within the self-assembly reproducible surface enhanced Raman spectroscopy signal. This new method enables a broad range of packing patterns and mechanisms by changing the host nanoparticles in the dispersion.

Synthesis of ultra-thin graphene-like nanosheets from lignin based on evaporation induced self-assembly for supercapacitors

Graphene-like carbon materials are widely used in power devices due to their excellent structural characteristics. In this study, ultra-thin graphene-like nanosheets (LGLNs) with rich surface wrinkles were prepared by classical evaporation induced self-assembly (EISA) using lignin biomass as carbon precursor, followed by chemical activation with KHCO3. The obtained LGLN900 material calcined at 900 °C had a thickness of ca. 3 nm, a large specific surface area of 2886 m2 g−1 with a high specific pore volume of 2.10 cm3 g−1. In addition, a large number of wrinkles on the surface of LGLN900 endows its effective compression resistance. When the LGLN900 material was used as electrode material of supercapacitor, a high specific capacitance of 388 F g−1 was obtained at 0.2 A g−1 current density in 6 M KOH aqueous solution, and 269 F g−1 specific capacitance could be at remained at 40 A g−1. The supercapacitor assembled with LGLN900 afforded a specific energy density of (11.0–13.7) Wh kg−1 at a power density of (128.8–6465) W kg−1. This work provides a facile and green strategy for the synthesis of highly wrinkled ultra-thin graphene-like nanosheets from sustainable biomass resources, which should have wide applications in adsorption, catalysis and energy storage.

Self-Assembly Strategies for Graphene Oxide/Silica Nanostructures: Synthesis and Structural Analysis

Abstract Nanostructured 3D silica-based materials can be designed using a low-dimensional template. Various composites composed of graphene oxide (GO) and silica have been investigated. However, to improve the performance of GO/silica nanostructure (GSN), the exploitation of the assembly method and the effect of combining GO and silica on the hybrid structure need to be elucidated. In this study, novel mesoporous GSNs were developed using two self-assembly methods: particle attaching-induced self-assembly (PAISA) and polymerization- and evaporation-induced self-assembly (PEISA). The synthesized GSNs obtained using each method were analyzed to determine the effect of combining silica with GO in each method on the porosity of GSNs. The former method introduced silica nanoparticles into GO, and aligned pores similar to the particle size were formed. In the latter method, synthesized GSN had broad mesopores, and a higher surface area derived from the silica particles randomly formed inside/outside GO layers. Both GSNs have specific surface areas close to that of the introduced silica, suggesting that the porosity of GSNs can be controlled by selecting the appropriate silica structure and its synthesis. Furthermore, GSN had a higher pore volume than silica itself, suggesting the formation of a hierarchical structure by introducing GO.

Ultra-thin highly-wrinkled graphene-like nanosheets for supercapacitor electrodes via 4-nitrocatechol and solvent-induced self-assembly

Graphene-like carbon materials are in high demand due to their potential applications in power devices. However, conventional synthesis of graphene-like materials causes repacking to occur during high-pressure compression steps resulting in low surface areas and unfavorable structures for mass transfer. Herein, ultra-thin wrinkled graphene-like nanosheets (GNs) were prepared simply via classical evaporation induced self-assembly (EISA) of 4-nitrocatechol as carbon precursor. Combination of EISA and subsequent KHCO3 activation and calcination at 900 °C (GN-900) afforded materials with thicknesses of (2–3) nm, specific surface areas of 3300 m2 g−1 with specific pore volumes of 2.34 cm3 g−1 under optimum conditions. When GN-900 was evaluated as an electrode material, a specific capacitance of 367 F g−1 was achieved at 0.2 A g−1 current density in 6 M KOH aqueous solution with a rate capability of 228 F g−1 at 40 A g−1. Supercapacitors assembled with GN-900 had specific energy densities of 11.5 Wh kg−1 at power densities of 89.8 W kg−1. Moreover, capacitance retention was greater than 98% after 3000 cycles at 10A g−1. Materials prepared with the proposed methods in this study were determined to be structurally stable and to exhibit favorable electrochemical performance for present and near-future supercapacitor applications.

Improving the decorative performance of UV-curable coatings with iridescent cellulose nanocrystal film.

Cellulose nanocrystals (CNC) possess remarkable mechanical properties, a high aspect ratio, a large specific surface area, and a unique nanostructure, making them a popular choice in various fields. In this study, a CNC suspension was prepared through acid hydrolysis, and subsequently, a film exhibiting iridescence and chiral nematic structure was formed on the cured UV-WA surface via evaporation-induced self-assembly. The mean diameter and length of CNC were determined to be 25.1-33.3 nm and 281.3-404.2 nm, respectively, through transmission electron microscope analysis. The experimental results revealed that the color of the film significantly changes with variations in the CNC suspension concentration. Notably, the formation of the iridescent film is dependent on the concentration of CNC, with concentrations between 1.2% and 2.9% being optimal, and the aspect ratio of the CNC nanoparticles being around 11.3. X-ray diffraction analysis confirmed that the CNC nanoparticles possess the same crystal structure as microcrystalline cellulose (cellulose I). Fourier transform infrared spectroscopy revealed that the C[double bond, length as m-dash]C bond present in the liquid UV-curable coating disappeared upon UV irradiation. The performance of the CNC iridescent film, with varying thickness, was evaluated using UV-vis spectroscopy. The thermogravimetric analysis results indicate that the addition of CNC enhances the membrane's thermal stability and heat resistance. The results indicate that as the thickness of the CNC iridescent film increases, the corresponding UV-vis spectra display a redshift. The UV-WA/CNC shows potential in the field of decoration and establishing a straightforward, cost-effective, and efficient method for producing photonic materials with structural colors.

Colloidal crystals of monodisperse fluoro-nanoparticles by aqueous polymerization-induced self-assembly.

Here, we prepared monodisperse fluorinated nanospheres with the diameter regulated from 100 to 200 nm and PDI of the diameter lower than 0.05 via polymerization-induced self-assembly (PISA). Mono/multilayered 2D and large-scale ordered 3D lattices were formed by solvent evaporation-induced colloidal self-assembly. This work shows the promising application of PISA in colloidal self-assembly.

Methanol-water mixture evaporation-induced self-assembly of ZIF-8 particles.

We report a strategy for the self-assembly of zeolitic imidazolate framework-8 (ZIF-8) particles induced by the evaporation of a methanol-water mixture. This strategy effectively suppresses the coffee ring effect, facilitates the rapid assembly of ZIF-8 particles, and improves the orientation and optical properties of self-assembled superstructures.

Phase Behavior, Self-Assembly, and Adhesive Potential of Cellulose Nanocrystal-Bovine Serum Albumin Amyloid Composites.

Structural organization is ubiquitous throughout nature and contributes to the outstanding mechanical/adhesive performance of organisms including geckoes, barnacles, and crustaceans. Typically, these types of structures are composed of polysaccharide and protein-based building blocks, and therefore, there is significant research interest in using similar building blocks in the fabrication of high-performance synthetic materials. Via evaporation-induced self-assembly, the organization of cellulose nanocrystals (CNCs) into a chiral nematic regime results in the formation of structured CNC films with prominent mechanical, optical, and photonic properties. However, there remains an important knowledge gap in relating equilibrium suspension behavior to dry film structuring and other functional properties of CNC-based composite materials. Herein, we systematically investigate the phase behavior of composite suspensions of rigid CNCs and flexible bovine serum albumin (BSA) amyloids in relation to their self-assembly into ordered films and structural adhesives. Increasing the concentration of BSA amyloids in the CNC suspensions results in a clear decrease in the anisotropic fraction volume percent via the preferential accumulation of BSA amyloids in the isotropic regime (as a result of depletion interactions). This translates to a blue shift or compression of the chiral nematic pitch in dried films. Finally, we also demonstrate the synergistic adhesive potential of CNC-BSA amyloid composites, with ultimate lap shear strengths in excess of 500 N/mg. We anticipate that understanding the systematic relationships between material interactions and self-assembly in suspension such as those investigated here will pave the way for a new generation of structured composite materials with a variety of enhanced functionalities.