Phosphate Nanosheets Research Articles

Highly efficient removal of radioactive 90Sr based on sulfonic acid-functionalized α-zirconium phosphate nanosheets

Excellent column packing is a precondition for efficient separation of radioactive 90Sr from high level liquid waste (HLLW). α-ZrP particles are traditionally used as column packing for capturing radioactive nuclides from HLLW due to their excellent stability and adsorption ability. However, there remains room for improvement in terms of capacity and selectivity. Here, the traditional α-ZrP column packing was exfoliated and further modified by anchoring sulfonic groups on its surface to improve its adsorption capacity for 90Sr. The resulting ZrP-SO3H not only retained the excellent properties of α-ZrP but also possessed a larger surface area and much more adsorption sites. Adsorption experiments indicated that ZrP-SO3H exhibited excellent adsorption ability for separating of Sr2+ from acidic condition, and the maximum adsorption capacity of Sr2+ fitted by a Langmuir model is 183.21 mg g−1, which is higher than that of traditional α-ZrP and other similar column packings. In addition, kinetic studies indicated that Sr2+ adsorption on ZrP-SO3H is fast, and surface chemical adsorption is the main interaction between Sr2+ and ZrP-SO3H. Remarkably, radioactive experiment proved that ZrP-SO3H is an excellent adsorbent, and shows good stability for high efficiency for selective removal of 90Sr under complicate radioactive environment. Our present results implied that the novel ZrP-SO3H is potential column packing and could be suggested as promising column packing for separation of 90Sr from HLLW.

Amorphous Iron and Cobalt Based Phosphate Nanosheets Supported on Nickel Foam as Superior Catalysts for Hydrogen Evolution Reaction

Amorphous iron and cobalt based phosphate catalysts supported on nickel foam were developed using the colloidal chemical method and evaluated for the hydrogen evolution reaction (HER). By using a catalyst with a specific ratio of Fe0.72Co0.42PO4/Ni foam, an ultralow overpotential of 77 mV at a current density of 10 mA cm–2 was achieved, which is even comparable to the noble platinum (Pt) catalyst. The promotion was verified with electrochemical impedance spectroscopy (EIS) and mainly attributed to the activation effect of Fe, which accelerates the charge transfer efficiency of Co to the benefit of catalyzing the reduction reaction of the hydrogen ions.

Preparation of highly-stable and recyclable novel Au/ZrP composite catalyst for 4-nitrophenol reduction

Zirconium phosphate (ZrP) nanosheets were synthesized and modified with tetrabutylammonium hydroxide (TBA) to form ZrP nanosheets. The ZrP nanosheet surface was modified with organosilane N1-(3- trimethoxysilylpropyl) diethylene triamine molecules to generate an amine-terminated surface that prevents the aggregation of Au nanoparticles (Au NPs). These Au NPs anchor to ZrP in a single, highdensity layer through their affinity for the amino functional groups to produce a Au/ZrP composite catalyst. Structure confirmation and characterization were performed by field-emission scanning electron microscopy, field-emission transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, UV–visible spectroscopy, Fourier-transform infrared spectroscopy, and solid-state NMR spectroscopy. The Au/ZrP composites demonstrated excellent performance and stability as catalysts for the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) within 180 s. These composites have potential for industrial applications where separation and recycling are imperative.

Ultrathin LiFePO4/C cathode for high performance lithium-ion batteries: Synthesis via solvothermal transformation of iron hydroxyl phosphate Fe3(PO4)2(OH)2 nanosheet

A novel two-step solvothermal approach was firstly applied to acquire ultrathin lithium iron (II) phosphate (LiFePO4) nanosheet (with thickness about 28 nm) with exposed (010) surface facets. The iron hydroxyl phosphate Fe3(PO4)2(OH)2 nanosheet fabricated in the first solvothermal step was proved to be effective template for ultrathin LiFePO4 formation after solvothermal lithiation in the second solvothermal step. Importantly, the two-step solvothermal lithiation could produce ultrathin nanosheets while one-step solvothermal based on Fe(II) fabrication could only produce nanoplate-like particles. The as-synthesized nanosheets has shortened Li-ion diffusion path and high robustness in the structure during high C-rate electrochemical tests. Based on comparison with bulk LiFePO4 and nano-plate LiFePO4, the LiFePO4 nanosheet exhibits quite high specific discharge capacity of 169, 165, 159, 142, and 121 mAh g−1, at C-rate of 0.1, 0.2, 0.5, 1, and 5C, respectively, and excellent cycling performance with capacity kept at 121 mAh g−1 with no obvious fading under 500 times cycles. The newly developed method can provide useful references to other olivine type LiMPO4 cathodes and even have potential to find more applications in the synthesis of functional materials.

Two-dimensional mesoporous vanadium phosphate nanosheets through liquid crystal templating method toward supercapacitor application

Mesoporous vanadium phosphate (VOPO4) nanosheets have been successfully synthesized through an easy and reproducible lyotropic liquid crystals (LLC) templating approach for the first time. Using the triblock copolymer (P123) as a surfactant, VOPO4 precursor with a well-developed 2D hexagonal mesostructure can be obtained. Following complete removal of the template by calcination, crystallized VOPO4 frameworks with less-ordered mesostructure are achieved. The as-prepared mesoporous VOPO4 nanosheets exhibit superior pseudocapacitive performance (767 F g‒1 at 0.5A g‒1) by virtue of the favorable mesostructure that gives rise to abundant easily accessible redox active sites as well as reinforced charge transfer and ion diffusion properties. The charge storage mechanism of the mesoporous VOPO4 nanosheets has been experimentally demonstrated to be based on the reversible two-step redox reactions between V(V) and V(III) in acidic medium. This advantageous LLC templating strategy is expected to open up a new route for designing various mesoporous metal phosphates with superior electrochemical performance for utilization in energy storage devices.

Significant improvement of tribological performances of polyamide 46/polyphenylene oxide alloy by functionalized zirconium phosphate

Abstract A functionalized zirconium phosphate (FZrP) nanosheet was synthesized and introduced to PA46/PPO alloy as a solid lubricant. FZrP showed a high efficiency in improving the tribological performances, mechanical properties and moisture resistance of PA46/PPO. With the incorporation of 2.0% FZrP, the wear loss and friction coefficient of PA/PPO were decreased by 94.48% and 56.60%, respectively. Moreover, the friction and wear mechanism of FZrP was intensively studied and revealed: FZrP nanosheet retained and accumulated on the wear surface because of its strong interfacial binding force with the matrix, which resulted in the formation of a protective layer with good strength, tenacity and lubricity to resist severe wear damage.

Nickel phosphate as advanced promising electrochemical catalyst for the electro-oxidation of methanol

Mesoporous nickel phosphate nanotube (Meso NiPO NT) and mesoporous nickel phosphate nanosheet (Meso NiPO NS) are developed as catalysts for electrochemical methanol oxidation. Conventional mesoporous nickel phosphate which is composed of stacked nanocrystals (Meso NiPO), microporous VSB-5 and commercial nickel oxide (NiO) are used as control materials. Notably, both Meso NiPO NT (40.83 mA cm−2) and Meso NiPO NS (44.97 mA cm−2) exhibit much higher oxidation current density than VSB-5 (13.41 mA cm−2), Meso NiPO (19.85 mA cm−2) and commercial NiO (0.87 mA cm−2). As for the durability test on these materials modified fluorine-doped tin dioxide transparent conductive glass (FTO) electrodes, Meso NiPO NT displays the most stable performance and still retains 91.3% electrochemical activity, which perhaps benefit from its nanotube structure and large specific surface area (99.6 m2/g). Moreover, Meso NiPO NT has higher activity and more excellent stability than many of the previously reported nickel-based materials, suggesting a potential development for direct methanol fuel cells.

Humidity Sensors: Lithium Tin Sulfide—a High‐Refractive‐Index 2D Material for Humidity‐Responsive Photonic Crystals (Adv. Funct. Mater. 14/2018)

In article number 1705740, Bettina V. Lotsch and co-workers report a new generation of photonic humidity sensors based on ultrahigh refractive index lithium tin sulfide nanosheets and antimony phosphate nanosheets. Both materials intercalate water and show pronounced swelling under the influence of humidity. Once integrated as ultrathin 1D photonic crystals, pronounced sensitivity to ambient humidity, along with excellent optical quality is achieved. Cover Design: Katalin Szendrei-Temesi.

Reduced graphene oxide-modified Ni-Co phosphate nanosheet self-assembled microplates as high-performance electrode materials for supercapacitors

It is demonstrated that the incorporation of reduced graphene oxide (rGO) and pseudocapacitance materials often offer an effective strategy toward fast reversible redox reactions while remaining their high pseudocapacitance. In this work, a type of rGO-modified Ni-Co phosphates (Ni(Co)NH4PO4@rGO) microplates were fabricated for supercapacitors electrodes via a one-step hydrothermal method. SEM and TEM tests indicated that the obtained microplates are comprised of well-aligned crystalline Ni(Co)NH4PO4 nanosheets. Moreover, the rGO-modified microplates exhibit a high specific capacitance of 1020 F g−1 at 1 A g−1, which is 16.3% enhanced compared to that of the untreated Ni(Co)NH4PO4) ones (877 F g−1). While the rate capacitor can reach to 92%. Furthermore, it is observed that after 700-cycles, the specific capacitance can increase to their maximum value of 1451 F g−1 at current density of 10 A g−1, and can still remain 1275 F g−1 after 5000 cycles, showing a high cycling stability. The Ni(Co)NH4PO4 showed the same tendency but the low values. These excellent electrochemical performances could be due to rGO modification and self-assembled well-aligned nanosheets. This type of structures cannot only facilitate the transfer electrons, but also offer high electrochemical activity sites and short transport path length for electrolyte ions.

Facile Synthesis of Ultrathin Nickel-Cobalt Phosphate 2D Nanosheets with Enhanced Electrocatalytic Activity for Glucose Oxidation.

Two-dimensional (2D) ultrathin nickel-cobalt phosphate nanosheets were synthesized using a simple one-step hydrothermal method. The morphology and structure of nanomaterials synthesized under different Ni/Co ratios were investigated by transmission electron microscopy, scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. Moreover, the influence of nanomaterials' structure on the electrochemical performance for glucose oxidation was investigated. It is found that the thinnest nickel-cobalt phosphate nanosheets synthesized with a Ni/Co ratio of 2:5 showed the best electrocatalytic activity for glucose oxidation. Also, the ultrathin nickel-cobalt phosphate nanosheet was used as an electrode material to construct a nonenzymatic electrochemical glucose sensor. The sensor showed a wide linear range (2-4470 μM) and a low detection limit (0.4 μM) with a high sensitivity of 302.99 μA·mM-1·cm-2. Furthermore, the application of the as-prepared sensor in detection of glucose in human serum was successfully demonstrated. These superior performances prove that ultrathin 2D nickel-cobalt phosphate nanosheets are promising materials in the field of electrochemical sensing.

Microporous 2D NiCoFe phosphate nanosheets supported on Ni foam for efficient overall water splitting in alkaline media.

The development of high-performance non-precious electrocatalysts for both H2 and O2 evolution reactions (HER and OER activities) and overall water splitting is highly desirable but remains a grand challenge. Herein, we report a facile method to synthesize ultrathin, amorphous, porous, oxygen and defect enriched NiCoFe phosphate nanosheets (NSs). Owing to their microporous confinement in a 2D orientation, which can reduce the ion transport resistance during electrochemical processes, and defect enriched structure with higher electrochemically active surface area, these NiCoFe phosphate porous nanosheets supported on nickel foam (NiCoFe phosphate NSs/NF) facilitate the diffusion of gaseous products (H2 and O2) and exhibit remarkable catalytic performance and outstanding stability for both HER, OER and overall water splitting in an alkaline electrolyte (1.0 M KOH). For the OER electrocatalyst, 2D NiCoFe phosphate NSs/NF was oxidized to NiCoFe oxides/hydroxides on the catalyst surface and exhibited remarkable OER activity with a low overpotential of only 240 mV needed to reach a current density of 10 mA cm-2. For HER, 2D NiCoFe phosphate NSs/NF afforded a current density of 10 mA cm-2 at a low overpotential of only -231 mV. Furthermore, employing 2D NiCoFe phosphate NSs/NF as the electrocatalyst for both the anode and the cathode, a water splitting electrolyzer was able to reach 10 mA cm-2 at a cell voltage of 1.52 V with robust durability. Various characterization techniques indicated that the long term stability and the activity for overall water splitting are due to the porosity, the electrochemically active constituents, and synergistic effects. This work could be inspiring in the design of Earth abundant and highly efficient electrocatalysts for overall water splitting, especially for OER.

Fabrication of ZrP nanosheet decorated macromolecular charring agent and its efficient synergism with ammonium polyphosphate in flame-retarding polypropylene

Poor efficiency is one of the biggest challenges for halogen-free flame retardant polymer. Catalyzing the carbonization of polymer itself during combustion is proposed to be a promising way to address this issue. In this work, a novel macromolecular charring agent (MCA) decorated by zirconium phosphate nanosheet named ZrP-d-MCA was synthesized and characterized. Subsequently, it was combined with ammonium polyphosphate (APP) to reduce the flammability of polypropylene (PP). When the contents of ZrP-d-MCA and APP were 5 wt% and 15 wt%, respectively, PP/Zr-d-MCA/APP could reach a limiting oxygen index of 32.5% and achieve UL-94 V-0 rating. Moreover, the bench-scale combustion performance determined by the cone calorimeter was significantly improved. The flame-retardant mechanism of ZrP-d-MCA/APP was revealed: during combustion, ZrP nanosheet could efficiently catalyze the charring reactions of MCA to form closed micro-nano char-cages, in which the degradation products of PP would be trapped and catalyzed into thermostable graphitization char.

Label-Free Photoelectrochemical "Off-On" Platform Coupled with G-Wire-Enhanced Strategy for Highly Sensitive MicroRNA Sensing in Cancer Cells.

MicroRNA (miRNAs) quantification, especially at low abundance, is vital for disease diagnosis, prognosis, and therapy. Herein we develop a distinctive label-free "off-on" configuration for photoelectrochemical (PEC) sensing platform fabrication, coupled with DNA four-way junction (4J) architecture as well as G-wire superstructure for signal amplification. In addition, ultrathin copper phosphate nanosheets (CuPi NSs) coating Au nanoparticles (Au-CuPi NSs) serve as a highly efficient photocathode substrate. To improve the sensitivity, and avoid the false positive signals, the quencher, gold nanoparticles (GNPs), is utilized to switch off the PEC signal because of the commendable surface plasmon resonance (SPR) absorption. Subsequently, ingenious DNA 4J architecture is applied to export proportional c-myc regions for target quantification. Assisted with the G-wire superstructure formation, the enhancer 5,10,15,20-tetra(4-sulfophenyl)-21H,23H-porphyrin (TSPP) is coupled on the substrate to switch on the PEC signal, thus realizing the miRNA assay with persuasive accuracy, high sensitivity, and low detection limit. In addition, we execute the miRNA detection in prostate carcinoma cell line 22Rv1, and acquire desirable quantitative capability. Remarkably, the prepared PEC sensing platform not only realizes the highly efficient miRNAs quantification, but also uncovers a marvelous horizon for sensing platform fabrication.

Fluorescent Humidity Sensors Based on Photonic Resonators

AbstractAmong the different approaches to humidity sensing available, those based on fluorescent signals are gathering a great deal of attention due to their fast response and versatility of detection and design. So far, all proposals have focused on the use of luminescent probes whose emission is either triggered or inhibited by the presence of water that reacts or alters their chemical environment, hence inducing the signal change. Here, a novel concept in fluorescent humidity sensing based on combining stimuli‐responsive photonic resonators with molecular fluorescent probes is introduced. The resonator is assembled from humidity‐swellable antimony phosphate nanosheets embedding a planar light‐emitting probe, whose emission is dramatically modified by the changes that ambient humidity causes in its photonic environment. Guided by “in silico” optical design of the resonator architecture and subsequent experimental realization, two embodiments of fluorescent photonic humidity sensors featuring turn‐on and turn‐off detection schemes are presented. The interplay between the luminescent properties of an emitter and its photonic environment implies a fundamental advantage as the emitters are not chemically altered during the detection process. At the same time, it paves the way toward a new generation of photonic humidity sensors which can conveniently be interfaced with common fluorescence detection schemes.

Effective Interlayer Engineering of Two-Dimensional VOPO4 Nanosheets via Controlled Organic Intercalation for Improving Alkali Ion Storage.

Two-dimensional (2D) energy materials have shown the promising electrochemical characteristics for lithium ion storage. However, the decreased active surfaces and the sluggish charge/mass transport for beyond-lithium ion storage that has potential for large-scale energy storage systems, such as sodium or potassium ion storage, caused by the irreversible restacking of 2D materials during electrode processing remain a major challenge. Here we develop a general interlayer engineering strategy to address the above-mentioned challenges by using 2D ultrathin vanadyl phosphate (VOPO4) nanosheets as a model material for challenging sodium ion storage. Via controlled intercalation of organic molecules, such as triethylene glycol and tetrahydrofuran, the sodium ion transport in VOPO4 nanosheets has been significantly improved. In addition to advanced characterization including X-ray diffraction, high-resolution transmission electron microscopy, and X-ray absorption fine structure to characterize the interlayer and the chemical bonding/configuration between the organic intercalants and the VOPO4 host layers, density functional theory calculations are also performed to understand the diffusion behavior of sodium ions in the pure and TEG intercalated VOPO4 nanosheets. Because of the expanded interlayer spacing in combination with the decreased energy barriers for sodium ion diffusion, intercalated VOPO4 nanosheets show much improved sodium ion transport kinetics and greatly enhanced rate capability and cycling stability for sodium ion storage. Our results afford deeper understanding of the interlayer-engineering strategy to improve the sodium ion storage performance of the VOPO4 nanosheets. Our results may also shed light on possible multivalent-ion based energy storage such as Mg2+ and Al3+.

Facile Synthesis of β-SrHPO4 with Wide Applications in the Effective Removal of Pb2+ and Methyl Blue

A facile synthesis routine of β-type strontium hydrogen phosphate (β-SrHPO4) nanosheets was provided by the method of solution growing at temperatures below 80 °C. β-SrHPO4 was utilized for removing lead ions (Pb2+) and adsorbing methyl blue. Within the pH values from 2.0 to 6.0 of lead solutions, the adsorption capacity of β-SrHPO4 could reach above 1000 mg·g–1. The maximum removal capacity was 1409 mg·g–1 for Pb2+ within 15 min at pH = 4.5 and remained stable with the increase of temperatures. Different cations (Zn2+, Cr3+, Cd2+, and Co2+) affected slightly on the adsorption of Pb2+. It is revealed that the adsorption mechanism of Pb2+ was based on dissolution–precipitation theory. The maximum adsorption capacity was 335.68 mg·g–1 for methyl blue. The adsorption data of methyl blue accorded with the Langmuir isotherm model with R2 = 0.994 and the pseudo-second-order kinetic model with R2 = 0.99996, showing that the removal of methyl blue was dominated by a chemical sorption process. The thermodynamic st...

Design and fabrication of highly sensitive and stable biochip for glucose biosensing

Common producing steps for test strips is complex and fussy. In this work, we proposed a feasible binder-free test strips fabrication method to directly grow enzyme/manganese phosphate nanosheets hybrids on the screen-print electrodes (SPE). Combined with microfluidic packaging technology, the ready-made portable electrochemical biochip shows a wider linear range (1–40mM, R2=0.9998) and excellent stability (maintained 98% response current after 20days store and retained 75% response current after continuous 30days determination) for the detection of glucose. Compared with commercial test strips, the biochip exhibits excellent sensitivity, stability and accuracy, which is indicative of its potential application in real samples.

Thermal Stability of Optically Transparent Alpha-Zirconium Phosphate/Poly(methyl methacrylate) Nanocomposites with High Particle Loading

Polymeric nanocomposites have gained attention over the past few decades for their enhanced thermal stability and degradation. However, the reactions involved in a polymer nanocomposite can vary significantly from system to system, making it necessary to investigate novel nanofillers in search for more effective materials. Nanocomposites comprised of alpha-zirconium phosphate (ZrP) nanosheets in poly (methyl methacrylate) (PMMA) were prepared with a wide range of nanoparticle loadings (0, 5, 10, and 30 wt.% ZrP in PMMA). The ZrP nanocomposites were characterized using UV-visible spectroscopy (UV-vis), x-ray diffraction (XRD), thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). Nanocomposites were well dispersed and optically transparent as shown by XRD and UV-vis. However in the UV region, transparent ZrP nanocomposites possessed excellent UV scattering properties, significantly reducing the transmittance of UV-light, while remaining transparent to the visual spectrum. Thermal stability studies using TGA and DTG showed the peak mass loss rate (PMLR) was reduced by 10% and simultaneously shifted to higher temperatures by 41 °C. Since the nanocomposites in this work cover such a large range of ZrP loadings, large amounts of high-temperature residuals were encountered after TGA studies, indicating that the high loading ZrP nanocomposites are largely noncombustible. In addition, DSC studies showed that ZrP content does affect the glass transition temperature, but not enough to limit the application in which ZrP nanocomposites could be used. These results point to ZrP nanocomposites being useful as polymer replacements, behaving like polymers until the event of a fire, in which case they are largely noncombustible.

Effectively suppressing vanadium permeation in vanadium redox flow battery application with modified Nafion membrane with nacre-like nanoarchitectures

Abstract A novel self-assembled composite membrane, Nafion-[PDDA/ZrP]n with nacre-like nanostructures was successfully fabricated by a layer-by-layer (LbL) method and used as proton exchange membrane for vanadium redox flow battery applications. Poly(diallyldimethylammonium chloride) (PDDA) with positive charges and zirconium phosphate (ZrP) nanosheets with negative charges can form ultra-thin nacre-like nanostructure on the surface of Nafion membrane via the ionic crosslinking of tightly folded macromolecules. The lamellar structure of ZrP nanosheets and Donnan exclusion effect of PDDA can greatly decrease the vanadium ion permeability and improve the selectivity of proton conductivity. The fabricated Nafion-[PDDA/ZrP]4 membrane shows two orders of magnitude lower vanadium ion permeability (1.05 × 10−6 cm2 min−1) and 12 times higher ion selectivity than those of pristine Nafion membrane at room temperature. Consequently, the performance of vanadium redox flow batteries (VRFBs) assembled with Nafion-[PDDA/ZrP]3 membrane achieved a highly coulombic efficiency (CE) and energy efficiency (EE) together with a very slow self-discharge rate. When comparing with pristine Nafion VRFB, the CE and EE values of Nafion-[PDDA/ZrP]3 VRFB are 10% and 7% higher at 30 mA cm−2, respectively.

(Invited) Nanostructured Graphene Electrodes for High Performance and Stretchability

Chemically derived graphene oxide (GO) and its derivatives are promising candidates for a variety of carbon-based functional nanostructures and hybrid architectures, because of their unique characteristics that include high theoretical surface area, tunable electrical conductivity, excellent solution processability, and high mass producibility at low cost. However, the irreversible stacking due to the strong π–π interactions between graphene nanosheets during drying or reduction processes significantly decreases the solution processability as well as accessible surface area. In this talk, I firstly present a sea-urchin-shaped template approach for fabricating highly crumpled graphene balls in bulk quantities with a simple process. Simultaneous chemical etching and reduction process of graphene oxide (GO)-encapsulated iron oxide particles results in dissolution of the core template with spiky morphology and conversion of the outer GO layers into reduced GO layers with increased hydrophobicity which remain in contact with the spiky surface of the template. After completely etching, the outer graphene layers are fully compressed into the crumpled form along with decrease in total volume by etching. The crumpled balls exhibit significantly larger surface area and good water-dispersion stability than those of stacked reduced GO or other crumple approaches, even though they also show comparable electrical conductivity. Furthermore, they are easily assembled into 3D macroporous networks without any binders through typical processes such as solvent casting or compression molding. The graphene networks with less pore volume still have the crumpled morphology without sacrificing the properties regardless of the assembly processes, producing a promising active electrode material with high gravimetric and volumetric energy density for capacitive energy storage. For the second part, using a facile ice-templated self-assembly process with reduced graphene sheets and vanadium phosphate (VOPO4) nanosheets, we realize a vertically porous nanocomposite of layered VOPO4 and graphene nanosheets with high surface area and high electrical conductivity. The resulting 3D VOPO4–graphene nanocomposite has a much higher capacitance of 527.9 F g–1 at a current density of 0.5 A g–1, compared with ~247 F g–1 of simple 3D VOPO4, with solid cycling stability. The enhanced pseudocapacitive behavior mainly originates from vertically porous structures from directionally grown ice crystals and simultaneously inducing radial segregation and forming inter-stacked structures of VOPO4–graphene nanosheets. This VOPO4–graphene nanocomposite electrode exhibits high surface area, vertically porous structure to the separator, structural stability from interstacked structure and high electrical conductivity, which would provide the short diffusion paths of electrolyte ions and fast transportation of charges within the conductive frameworks. In addition, an asymmetric supercapacitor (ASC) is fabricated by using vertically porous VOPO4–graphene as the positive electrode and vertically porous 3D graphene as the negative electrode; it exhibits a wide cell voltage of 1.6 V and a largely enhanced energy density of 108 Wh kg–1. In the last part, we also used the ice-templated vertically porous graphene nanostructures as a stretchable supercapacitor electrode. Radially compressed honeycomb structures exhibited nearly-zero poission ratio structures and maintained their structure and electrical conductivity even at 50 % of starched states. The capacitive performance of these compressed honeycomb structures also shows fairly high over 130 F g-1 and these high performance still be maintained at highly stretched condition.