Controllable Synthesis of 2D Nonlayered Cr2S3 Nanosheets and Their Electrocatalytic Activity Toward Oxygen Evolution Reaction

The design of oxygen evolution reaction (OER) electrocatalysts based on Earth-abundant materials holds great promise for realizing practically viable water-splitting systems. In this regard, two-dimensional (2D) nonlayered materials have received considerable attention in recent years owing to their intrinsic dangling bonds which give rise to the exposure of unsaturated active sites. In this work, we solved the synthesis challenge in the development of a 2D nonlayered Cr2S3 catalyst for OER application via introducing a controllable chemical vapor deposition scheme. The as-obtained catalyst exhibits a very good OER activity requiring overpotentials of only 230 mV and 300 mV to deliver current densities of 10 mA cm−2 and 30 mA cm−2 , respectively, with robust stability. This study provides a general approach to optimize the controllable growth of 2D nonlayered material and opens up a fertile ground for studying the various strategies to enhance the water splitting reaction

Fe–Al binary oxide nanosorbent: Synthesis, characterization and phosphate sorption property

Phosphorous removal using efficient treatment approach such as adsorption is vital for the control of eutrophication. In this study, nanosized Fe-Al binary oxide sorbent was synthesized through a modified gel evaporation method and employed for adsorption of phosphate from aqueous system. The nanosorbent was characterized by x-ray diffraction (XRD), scanning electron microscope coupled with energy dispersive x-ray spectroscopy (SEM/EDX), tunneling electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR) and flame atomic absorption spectroscopy (FAAS). Langmuir model showed the best fit to the experimental data with a maximum adsorption efficiency of 16.4 mg/g. Having all parameters optimized, it has been found that the nanosorbent exhibited 99.86% phosphate adsorption efficiency. The effect of co-existing anions on the adsorption of phosphate was also studied and no significant effect on the efficiency of the nanosorbent was observed due to competing ions such as fluoride. Desorbabilty of phosphate was investigated and found to be increased with increasing pH. The results of thermodynamic studies indicated that the process is spontaneous and endothermic. Both macroscopic and microscopic approaches were employed to predict the mechanism of phosphate adsorption on the Fe-Al binary oxide nanosorbent. Accordingly, the phosphate adsorption is presumed to occur via the replacement of surface hydroxyl groups by the phosphate species and formation of inner-sphere surface complexes at the water/oxide interfac

Hierarchical MnO2/activated carbon cloth electrode prepared by synchronized electrochemical activation and oxidation for flexible asymmetric supercapacitors

Despite appealing supercapacitive properties, the flexible asymmetric supercapacitor devices (FASCs) are still suffering from low mass loading and limited operating voltage, leading to unsatisfactory energy densities. Herein, we introduced a high-voltage anodic electro-deposition process (AED) which is a novel avenue enabling the synthesis of hierarchical MnO2 on activated carbon cloth (H-MnO2/ACC). Interestingly, the concomitant activation of carbon cloth substrate is found to be beneficial to improve the conductivity and hydrophilic nature of our novel electrode. A FASC based on H-MnO2/ACC-300 and reduced carbon cloth (RCC) was assembled using a mixed ionic liquid gel (ionogel) electrolyte. Benefiting from highly conductive paths derived from intimately attached fiber-MnO2 interfaces, hierarchically interpenetrated lamella MnO2 porosity and concentric MnO2 interlayer voids, as well as the merits of ionic liquid, the resultant FASC delivers an output voltage as high as 4 V and an impressive volumetric energy density of 3.82 mWh/cm3. Furthermore, the optimized H-MnO2/ACC-300 electrode with high mass loading can even retain 94.2% of initial capacitance upon 5000 cycles in 1 M Na2SO4. The unique H-MnO2/ACC can aid in the rational design towards flexible electronic devices with high mass loading and this synthetic strategy opens up enormous possibilities for the fabrication of electrodeposited materials

Hierarchical porous carbon foam supported on carbon cloth as high-performance anodes for aqueous supercapacitors

Carbon anodes have been widely utilized for the fabrication of high-performance asymmetric supercapacitors. However, they generally suffer from unsatisfactory energy density due to low specific capacitance arising from inferior conductivity and insufficient ionic diffusion rate. Here a surface modification method is conducted after the annealing of ZIF-67 precursor to produce hydrophilic, porous and heteroatom-doped carbon foam. On top of enhanced area capacitance, widened voltage window of −1.3–0 V (vs saturated calomel electrode) can be achieved through electrochemical reduction to suppress the hydrogen evolution reaction. The optimized reduced porous carbon foam on carbon cloth exhibits a maximum area capacitance of 1049 mF/cm2 at an applied current density of 12 mA/cm2 with excellent capacitance retention of 98.4% after 6000 charge-discharge cycles at 15 mA/cm2. By well pairing with hierarchical MnO2/CC cathode, a 2.3 V asymmetric supercapacitor in neutral aqueous Na2SO4 electrolyte is assembled, which delivers an exceptional energy density of up to 10.07 mWh/cm3. The procedure in this paper for carbonaceous material to simultaneously achieve considerable capacitance and enlarged voltage window can open up a wider prospect toward design of anodes for high-performance aqueous supercapacitor

Insight into the role of interfacial reconstruction of manganese oxides toward enhanced electrochemical capacitors

The pursuit of facile synthetic methods for systematic control over the morphology and crystal phase of nanostructures has attracted a tremendous amount of interest. By utilizing the acid-induced layer-to-tunnel transition method of MnO2, we here for the first time report multi-layered sawtooth-shape MnO2 with relatively high mass loading. The optimized electrode exhibits durable activity with enhanced surface area, electrical conductivity and ionic diffusion. A high areal capacitance of 1781.8 mF/cm2 is obtained and excellent rate performance can be corroborated from capacitance retention of 64.1% when the current density is increased by 45-fold. Our uniquely assembled heterostructure endows a large number of active sites and acts as electron superhighways to facilitate efficient charge transportation. Further coupling with activated graphene/CC anode, a flexible device with a maximum operating voltage of 2.2 V is assembled, delivering a high volumetric energy density of 4.3 mWh/cm3 at a power density of 27.6 mW/cm3 with outstanding cycling performance. The finding promotes the development of highly efficient faradaic electrode materials toward closing the gap between achieved and theoretical capacitance without limiting the mass loading

Multifunctional tunneling devices based on graphene/h-BN/MoSe2 van der Waals heterostructures

The vertically stacked devices based on van der Waals heterostructures (vdWHs) of two-dimensional layered materials (2DLMs) have attracted considerable attention due to their superb properties. As a typical structure, graphene/hexagonal boron nitride (h-BN)/graphene vdWH has been proved possible to make tunneling devices. Compared with graphene, transition metal dichalcogenides possess intrinsic bandgap, leading to high performance of electronic devices. Here, tunneling devices based on graphene/h-BN/MoSe2 vdWHs are designed for multiple functions. On the one hand, the device shows a typical tunneling field-effect transistor behavior. A high on/off ratio of tunneling current (5 × 103) and an ultrahigh current rectification ratio (7 × 105) are achieved, which are attributed to relatively small electronic affinity of MoSe2 and optimized thickness of h-BN. On the other hand, the same structure also realizes 2D non-volatile memory with a high program/erase current ratio (>105), large memory window (∼150 V from ±90 V), and good retention characteristic. These results could enhance the fundamental understanding of tunneling behavior in vdWHs and contribute to the design of ultrathin rectifiers and memory based on 2DLMs

Facile Electron Transfer in Atomically Coupled Heterointerface for Accelerated Oxygen Evolution

An efficient and cost-effective approach for the development of advanced catalysts has been regarded as a sustainable way for green energy utilization. The general guideline to design active and efficient catalysts for oxygen evolution reaction (OER) is to achieve high intrinsic activity and the exposure of more density of the interfacial active sites. The heterointerface is one of the most attractive ways that plays a key role in electrochemical water oxidation. Herein, atomically cluster-based heterointerface catalysts with strong metal support interaction (SMSI) between WMn2O4 and TiO2 are designed. In this case, the WMn2O4 nanoflakes are uniformly decorated by TiO2 particles to create electronic effect on WMn2O4 nanoflakes as confirmed by X-ray absorption near edge fine structure. As a result, the engineered heterointerface requires an OER onset overpotential as low as 200 mV versus reversible hydrogen electrode, which is stable for up to 30 h of test. The outstanding performance and longterm durability are due to SMSI, the exposure of interfacial active sites, and accelerated reaction kinetics. To confirm the synergistic interaction between WMn2O4 and TiO2, and the modification of the electronic structure, highresolution transmission electron microscopy (HR-TEM), X-ray photoemission spectroscopy (XPS), and X-ray absorption spectroscopy (XAS) are used

Facile Electron Transfer in Atomically Coupled Heterointerface for Accelerated Oxygen Evolution

An efficient and cost-effective approach for the development of advanced catalysts has been regarded as a sustainable way for green energy utilization. The general guideline to design active and efficient catalysts for oxygen evolution reaction (OER) is to achieve high intrinsic activity and the exposure of more density of the interfacial active sites. The heterointerface is one of the most attractive ways that plays a key role in electrochemical water oxidation. Herein, atomically cluster-based heterointerface catalysts with strong metal support interaction (SMSI) between WMn2O4 and TiO2 are designed. In this case, the WMn2O4 nanoflakes are uniformly decorated by TiO2 particles to create electronic effect on WMn2O4 nanoflakes as confirmed by X-ray absorption near edge fine structure. As a result, the engineered heterointerface requires an OER onset overpotential as low as 200 mV versus reversible hydrogen electrode, which is stable for up to 30 h of test. The outstanding performance and long-term durability are due to SMSI, the exposure of interfacial active sites, and accelerated reaction kinetics. To confirm the synergistic interaction between WMn2O4 and TiO2, and the modification of the electronic structure, high-resolution transmission electron microscopy (HR-TEM), X-ray photoemission spectroscopy (XPS), and X-ray absorption spectroscopy (XAS) are used.Validerad;2023;Nivå 2;2023-03-08 (joosat);Licens fulltext: CC BY License</p

Hierarchical MnO2/activated carbon cloth electrode prepared by synchronized electrochemical activation and oxidation for flexible asymmetric supercapacitors

Despite appealing supercapacitive properties, the flexible asymmetric supercapacitor devices (FASCs) are still suffering from low mass loading and limited operating voltage, leading to unsatisfactory energy densities. Herein, we introduced a high-voltage anodic electro-deposition process (AED) which is a novel avenue enabling the synthesis of hierarchical MnO2 on activated carbon cloth (H-MnO2/ACC). Interestingly, the concomitant activation of carbon cloth substrate is found to be beneficial to improve the conductivity and hydrophilic nature of our novel electrode. A FASC based on H-MnO2/ACC-300 and reduced carbon cloth (RCC) was assembled using a mixed ionic liquid gel (ionogel) electrolyte. Benefiting from highly conductive paths derived from intimately attached fiber-MnO2 interfaces, hierarchically interpenetrated lamella MnO2 porosity and concentric MnO2 interlayer voids, as well as the merits of ionic liquid, the resultant FASC delivers an output voltage as high as 4 V and an impressive volumetric energy density of 3.82 mWh/cm(3). Furthermore, the optimized H-MnO2/ACC-300 electrode with high mass loading can even retain 94.2% of initial capacitance upon 5000 cycles in 1 M Na2SO4. The unique H-MnO2/ACC can aid in the rational design towards flexible electronic devices with high mass loading and this synthetic strategy opens up enormous possibilities for the fabrication of electrodeposited materials