Design and Advanced Manufacturing of NU-1000 Metal-Organic Frameworks with Future Perspectives for Environmental and Renewable Energy Applications.

Metal-organic frameworks (MOFs) represent a relatively new family of materials that attract lots of attention thanks to their unique features such as hierarchical porosity, active metal centers, versatility of linkers/metal nodes, and large surface area. Among the extended list of MOFs, Zr-based-MOFs demonstrate comparably superior chemical and thermal stabilities, making them ideal candidates for energy and environmental applications. As a Zr-MOF, NU-1000 is first synthesized at Northwestern University. A comprehensive review of various approaches to the synthesis of NU-1000 MOFs for obtaining unique surface properties (e.g., diverse surface morphologies, large surface area, and particular pore size distribution) and their applications in the catalysis (electro-, and photo-catalysis), CO2 reduction, batteries, hydrogen storage, gas storage/separation, and other environmental fields are presented. The review further outlines the current challenges in the development of NU-1000 MOFs and their derivatives in practical applications, revealing areas for future investigation.

Water-Stable Fluorous Metal-Organic Frameworks with Open Metal Sites and Amine Groups for Efficient Urea Electrocatalytic Oxidation.

Urea oxidation reaction (UOR) is one of the promising alternative anodic reactions to water oxidation that has attracted extensive attention in green hydrogen production. The application of specifically designed electrocatalysts capable of declining energy consumption and environmental consequences is one of the major challenges in this field. Therefore, the goal is to achieve a resistant, low-cost, and environmentally friendly electrocatalyst. Herein, a water-stable fluorinated Cu(II) metalorganic framework (MOF) {[Cu2 (L)(H2 O)2 ]·(5DMF)(4H2 O)}n (Cu-FMOF-NH2 ; H4 L = 3,5-bis(2,4-dicarboxylic acid)-4-(trifluoromethyl)aniline) is developed utilizing an angular tetracarboxylic acid ligand that incorporates both trifluoromethyl (-CF3 ) and amine (-NH2 ) groups. The tailored structure of Cu-FMOF-NH2 where linkers are connected by fluoride bridges and surrounded by dicopper nodes reveals a 4,24T1 topology. When employed as electrocatalyst, Cu-FMOF-NH2 requires only 1.31 V versus reversible hydrogen electrode (RHE) to deliver 10 mA cm-2 current density in 1.0 m KOH with 0.33 m urea electrolyte and delivered an even higher current density (50 mA cm-2 ) at 1.47 V versus RHE. This performance is superior to several reported catalysts including commercial RuO2 catalyst with overpotential of 1.52 V versus RHE. This investigation opens new opportunities to develop and utilize pristine MOFs as a potential electrocatalyst for various catalytic reactions.

Electronic Structure Engineered Heteroatom Doped All Transition Metal Sulfide Carbon Confined Heterostructure for Extrinsic Pseudocapacitor.

Ultra-high energy density battery-type materials are promising candidates for supercapacitors (SCs); however, slow ion kinetics and significant volume expansion remain major barriers to their practical applications. To address these issues, hierarchical lattice distorted α-/γ-MnS@Cox Sy core-shell heterostructure constrained in the sulphur (S), nitrogen (N) co-doped carbon (C) metal-organic frameworks (MOFs) derived nanosheets (α-/γ-MnS@Cox Sy @N, SC) have been developed. The coordination bonding among Cox Sy , and α-/γ-MnS nanoparticles at the interfaces and the π-π stacking interactions developed across α-/γ-MnS@Cox Sy and N, SC restrict volume expansion during cycling. Furthermore, the porous lattice distorted heteroatom-enriched nanosheets contain a sufficient number of active sites to allow for efficient electron transportation. Density functional theory (DFT) confirms the significant change in electronic states caused by heteroatom doping and the formation of core-shell structures, which provide more accessible species with excellent interlayer and interparticle conductivity, resulting in increased electrical conductivity. . The α-/γ-MnS@Cox Sy @N, SC electrode exhibits an excellent specific capacity of 277 mA hg-1 and cycling stability over 23 600 cycles. A quasi-solid-state flexible extrinsic pseudocapacitor (QFEPs) assembled using layer-by-layer deposited multi-walled carbon nanotube/Ti3 C2 TX nanocomposite negative electrode. QFEPs deliver specific energy of 64.8 Wh kg-1 (1.62 mWh cm-3 ) at a power of 933 W kg-1 and 92% capacitance retention over 5000 cycles.

Reconfiguring the Electronic Structure of Heteroatom Doped Carbon Supported Bimetallic Oxide@Metal Sulfide Core-Shell Heterostructure via In Situ Nb Incorporation toward Extrinsic Pseudocapacitor.

High-energy-density battery-type materials have sparked considerable interest as supercapacitors electrode; however, their sluggish charge kinetics limits utilization of redox-active sites, resulting in poor electrochemical performance. Here, the unique core-shell architecture of metal organic framework derived N-S codoped carbon@Cox Sy micropetals decorated with Nb-incorporated cobalt molybdate nanosheets (Nb-CMO4 @Cx Sy NC) is demonstrated. Coordination bonding across interfaces and π-π stacking interactions between CMO4 @Cx Sy and N and, S-C can prevent volume expansion during cycling. Density functional theory analysis reveals that the excellent interlayer and the interparticle conductivity imparted by Nb doping in heteroatoms synergistically alter the electronic states and offer more accessible species, leading to increased electrical conductivity with lower band gaps. Consequently, the optimized electrode has a high specific capacity of 276.3 mAh g-1 at 1 A g-1 and retains 98.7% of its capacity after 10 000 charge-discharge cycles. A flexible quasi-solid-state SC with a layer-by-layer deposited reduced graphene oxide /Ti3 C2 TX anode achieves a specific energy of 75.5 Wh kg-1 (volumetric energy of 1.58 mWh cm-3 ) at a specific power of 1.875 kWh kg-1 with 96.2% capacity retention over 10 000 charge-discharge cycles.

Graphene-Based Metal-Organic Framework Hybrids for Applications in Catalysis, Environmental, and Energy Technologies.

Current energy and environmental challenges demand the development and design of multifunctional porous materials with tunable properties for catalysis, water purification, and energy conversion and storage. Because of their amenability to de novo reticular chemistry, metal-organic frameworks (MOFs) have become key materials in this area. However, their usefulness is often limited by low chemical stability, conductivity and inappropriate pore sizes. Conductive two-dimensional (2D) materials with robust structural skeletons and/or functionalized surfaces can form stabilizing interactions with MOF components, enabling the fabrication of MOF nanocomposites with tunable pore characteristics. Graphene and its functional derivatives are the largest class of 2D materials and possess remarkable compositional versatility, structural diversity, and controllable surface chemistry. Here, we critically review current knowledge concerning the growth, structure, and properties of graphene derivatives, MOFs, and their graphene@MOF composites as well as the associated structure-property-performance relationships. Synthetic strategies for preparing graphene@MOF composites and tuning their properties are also comprehensively reviewed together with their applications in gas storage/separation, water purification, catalysis (organo-, electro-, and photocatalysis), and electrochemical energy storage and conversion. Current challenges in the development of graphene@MOF hybrids and their practical applications are addressed, revealing areas for future investigation. We hope that this review will inspire further exploration of new graphene@MOF hybrids for energy, electronic, biomedical, and photocatalysis applications as well as studies on previously unreported properties of known hybrids to reveal potential "diamonds in the rough".

Hierarchical porous metal-organic gels and derived materials: from fundamentals to potential applications.

Metal-organic gels (MOGs) emerged as a novel class of functional soft materials in which the scaffolding framework is fabricated by metal-ligand coordination in combination with other supramolecular interactions (for example, hydrogen bonding or π-π stacking). Through the combination of organic and inorganic (metal/metal-oxo clusters) building blocks, significant steps forward have been made in the development of new electrochemical sensors, superhydrophobic materials and ion storage devices, among others. These leaps forward are to some extend induced by the intrinsic hierarchical microporous/mesoporous pore structure of these metal-organic materials. Within this review we give an overview of recent developments of this growing field. First, we shed light onto the parallels to the well-established field of conventional gels and outline similarities and differences. Afterwards, we classify different types of MOGs according to their architectural/structural nature: (1) pristine MOGs, (2) hybrid MOGs, (3) crosslinking-based MOGs and (4) MOG-derived materials. Furthermore, we look at the different properties of MOGs and the requirements for the preparation of spatially patterned macro-structured MOGs by emerging additive manufacturing technologies. Moreover, different potential fields of application for MOGs and MOG derived materials are critically evaluated and potential improvements and pitfalls in comparison to traditional gel-based materials are given. Finally, a comprehensive outlook into future directions for the development of MOGs is provided.

Emerging MXene@Metal-Organic Framework Hybrids: Design Strategies toward Versatile Applications.

Rapid progress on developing smart materials and design of hybrids is motivated by pressing challenges associated with energy crisis and environmental remediation. While emergence of versatile classes of nanomaterials has been fascinating, the real excitement lies in the design of hybrid materials with tunable properties. Metal-organic frameworks (MOFs) are the key materials for gas sorption and electrochemical applications, but their sustainability is challenged by limited chemical stability, poor electrical conductivity, and intricate, inaccessible pores. Despite tremendous efforts towards improving the stability of MOF materials, little progress has made researchers inclined toward developing hybrid materials. MXenes, a family of two-dimensional transition-metal carbides, nitrides and carbonitrides, are known for their compositional versatility and formation of a range of structures with rich surface chemistry. Hybridization of MOFs with functional layered MXene materials may be beneficial if the host structure provides appropriate interactions for stabilizing and improving the desired properties. Recent efforts have focused on integrating Ti3C2Tx and V2CTx MXenes with MOFs to result in hybrid materials with augmented electrochemical and physicochemical properties, widening the scope for emerging applications. This review discusses the potential design strategies of MXene@MOF hybrids, attributes of tunable properties in the resulting hybrids, and their applications in water treatment, sensing, electrochemical energy storage, smart textiles, and electrocatalysis. Comprehensive discussions on the recent efforts on rapidly evolving MXene@MOF materials for various applications and potential future directions are highlighted.

Impact of Annealing Temperature on the Morphological, Optical and Photoelectrochemical Properties of Cauliflower-like CdSe0.6Te0.4 Photoelectrodes; Enhanced Solar Cell Performance.

We are reporting on the impact of air annealing temperatures on the physicochemical properties of electrochemically synthesized cadmium selenium telluride (CdSe0.6Te0.4) samples for their application in a photoelectrochemical (PEC) solar cell. The CdSe0.6Te0.4 samples were characterized with several sophisticated techniques to understand their characteristic properties. The XRD results presented the pure phase formation of the ternary CdSe0.6Te0.4 nanocompound with a hexagonal crystal structure, indicating that the annealing temperature influences the XRD peak intensity. The XPS study confirmed the existence of Cd, Se, and Te elements, indicating the formation of ternary CdSe0.6Te0.4 compounds. The FE-SEM results showed that the morphological engineering of the CdSe0.6Te0.4 samples can be achieved simply by changing the annealing temperatures from 300 to 400 °C with intervals of 50 °C. The efficiencies (ƞ) of the CdSe0.6Te0.4 photoelectrodes were found to be 2.0% for the non-annealed and 3.1, 3.6, and 2.5% for the annealed at 300, 350, and 400 °C, respectively. Most interestingly, the PEC cell analysis indicated that the annealing temperatures played an important role in boosting the performance of the photoelectrochemical properties of the solar cells.

Nickel Cobaltite: A Positive Electrode Material for Hybrid Supercapacitors.

The increased demand of energy due to the recent technological advances in diverse fields such as portable electronics and electric vehicles is often hindered by the poor capability of energy-storage systems. Although supercapacitors (SCs) exhibit higher power density than state-of-the art batteries, their insufficient energy density remains a major challenge. An emerging concept of hybrid supercapacitors (HSCs) with the combination of one capacitive and one battery electrode in a single cell holds a great promise to deliver high energy density without sacrificing power density and cycling stability. This Minireview elaborates the recent advances of use of nickel cobaltite (NiCo2 O4 ) as a potential positive electrode (battery-like) for HSCs. A brief introduction on the structural benefits and charge storage mechanisms of NiCo2 O4 was provided. It further shed a light on composites of NiCo2 O4 with different materials like carbon, polymers, metal oxides, and others, which altogether helps in increasing the electrochemical performance of HSCs. Finally, the key scientific challenges and perspectives on building high-performance HSCs for future-generation applications were reviewed.

Emergence of Ni-Based Chalcogenides (S and Se) for Clean Energy Conversion and Storage.

Nickel chalcogenide (S and Se) based nanostructures intrigued scientists for some time as materials for energy conversion and storage systems. Interest in these materials is due to their good electrochemical stability, eco-friendly nature, and low cost. The present review compiles recent progress in the area of nickel-(S and Se)-based materials by providing a comprehensive summary of their structural and chemical features and performance. Improving properties of the materials, such as electrical conductivity and surface characteristics (surface area and morphology), through strategies like nano-structuring and hybridization, are systematically discussed. The interaction of the materials with electrolytes, other electro-active materials, and inactive components are analyzed to understand their effects on the performance of energy conversion and storage devices. Finally, outstanding challenges and possible solutions are briefly presented with some perspectives toward the future development of these materials for energy-oriented devices with high performance.

Bimetallic Phosphides for Hybrid Supercapacitors.

Supercapacitors (SCs) are considered promising energy storage systems because of their high power output and long-term cycling stability; however, they usually exhibit poor energy density. The hybrid supercapacitor (HSC) is an emerging concept in which two dissimilar electrodes with different charge storage mechanisms are paired to deliver high energy without sacrificing power output. This Perspective highlights the features of transition-metal phosphides (TMPs) as the positive electrode in HSCs. In particular, bimetallic nickel cobalt phosphide (NiCoP) with multiple redox sites, excellent electrochemical reversibility, and stability is discussed. We outline how the rational heterostructures, elemental variations, and nanocomposite morphologies tune the electrochemical properties of NiCoP as the positive electrode in HSCs. The Perspective further sheds light on NiCoP-based composites that help in improving the overall performance of HSCs in terms of energy density and cycling stability. The key scientific challenges and perspectives on building efficient and stable HSCs for future applications are discussed.

Ag/AgCl@MIL-88A(Fe) heterojunction ternary composites: towards the photocatalytic degradation of organic pollutants.

The efficient utilization of solar energy has received tremendous interest due to the increasing environmental and energy concerns. The present paper discusses the efficient integration of a plasmonic photocatalyst (Ag/AgCl) with an iron-based metal-organic framework (MIL-88A(Fe)) for boosting the visible light photoreactivity of MIL-88A(Fe). Two composites of Ag/AgCl@MIL-88A(Fe), namely MAG-1 and MAG-2 (stoichiometric ratio of Fe to Ag is 5 : 1 and 2 : 1), were successfully synthesized via facile in situ hydrothermal methods followed by UV reduction. The synthesized composite materials are characterized by FTIR, PXRD, UVDRS, PL, FESEM/EDX, TEM and BET analyses. The Ag/AgCl@MIL-88A(Fe) (MAG-2) hybrid system shows excellent photocatalytic activity for the degradation of p-nitrophenol (PNP), rhodamine B (RhB), and methylene blue (MB) under sunlight. We found that 91% degradation of PNP in 80 min, 99% degradation of RhB in 70 min and 94% degradation of MB in 70 min have taken place by using MAG-2 as a catalyst under sunlight. The superior activity of Ag/AgCl@MIL-88A(Fe) (MAG-2) is attributed to the synergistic effects from the surface plasmon resonance (SPR) of Ag NPs and the electron transfer from MIL-88A(Fe) to Ag nanoparticles for effective separation of electron-hole pairs. Furthermore, the mechanism of degradation of PNP, RhB and MB is proposed by analyzing the electron transfer pathway in Ag/AgCl@MIL-88A(Fe).

Metal Halide Perovskite@Metal-Organic Framework Hybrids: Synthesis, Design, Properties, and Applications.

Metal halide perovskites (MHPs) have excellent optoelectronic and photovoltaic applications because of their cost-effectiveness, tunable emission, high photoluminescence quantum yields, and excellent charge carrier properties. However, the potential applications of the entire MHP family are facing a major challenge arising from its weak resistance to moisture, polar solvents, temperature, and light exposure. A viable strategy to enhance the stability of MHPs could lie in their incorporation into a porous template. Metal-organic frameworks (MOFs) have outstanding properties, with a unique network of ordered/functional pores, which render them promising for functioning as such a template, accommodating a wide range of MHPs to the nanosized region, alongside minimizing particle aggregation and enhancing the stability of the entrapped species. This review highlights recent advances in design strategies, synthesis, characterization, and properties of various hybrids of MOFs with MHPs. Particular attention is paid to a critical review of the emergence of MHP@MOF for comprehensive studies of next-generation materials for various technological applications including sensors, photocatalysis, encryption/decryption, light-emitting diodes, and solar cells. Finally, by summarizing the state-of-the-art, some promising future applications of reported hybrids are proposed. Considering the inherent correlation and synergic functionalities of MHPs and MOFs, further advancement; new functional materials; and applications can be achieved through designing MHP@MOF hybrids.

Dual Carbon Potassium-Ion Capacitors: Biomass-Derived Graphene-like Carbon Nanosheet Cathodes.

Potassium-ion storage devices are attracting tremendous attention for wide-ranging applications on account of their low cost, fast charge transport in electrolytes, and large working voltage. However, developing cost-effective, high-energy electrodes with excellent structural stability to ensure long-term cycling performance is a major challenge. In this contribution, we have derived two different forms of carbon materials from almond shells using different chemical treatments. For instance, hard carbon (HC) and graphene-like activated carbon (AC) nanosheets are developed by employing simple carbonization and chemical activation routes, respectively. The resultant hard carbon (AS-HC) and activated carbon (AS-AC) exhibit outstanding electrochemical performance as negative and positive electrodes in a potassium-ion battery (KIB), respectively, through their tailor-made surface properties. These promising benefits pave a way to construct a biomass-derived carbon potassium-ion capacitor (KIC) by employing AS-HC as the negative electrode and AS-AC as the positive electrode in a K-based electrolyte. The as-fabricated KIC delivers a reasonable specific energy of 105 Wh/kg and excellent cycling life with negligible capacitance fading over 10 000 cycles. This "waste-to-wealth" approach can promote the development of sustainable KICs at low cost and inspire their use for fast-rate K-based energy storage applications.

True Meaning of Pseudocapacitors and Their Performance Metrics: Asymmetric versus Hybrid Supercapacitors.

The development of pseudocapacitive materials for energy-oriented applications has stimulated considerable interest in recent years due to their high energy-storing capacity with high power outputs. Nevertheless, the utilization of nanosized active materials in batteries leads to fast redox kinetics due to the improved surface area and short diffusion pathways, which shifts their electrochemical signatures from battery-like to the pseudocapacitive-like behavior. As a result, it becomes challenging to distinguish "pseudocapacitive" and "battery" materials. Such misconceptions have further impacted on the final device configurations. This Review is an earnest effort to clarify the confusion between the battery and pseudocapacitive materials by providing their true meanings and correct performance metrics. A method to distinguish battery-type and pseudocapacitive materials using the electrochemical signatures and quantitative kinetics analysis is outlined. Taking solid-state supercapacitors (SSCs, only polymer gel electrolytes) as an example, the distinction between asymmetric and hybrid supercapacitors is discussed. The state-of-the-art progress in the engineering of active materials is summarized, which will guide for the development of real-pseudocapacitive energy storage systems.

Recycle, Recover and Repurpose Strategy of Spent Li-ion Batteries and Catalysts: Current Status and Future Opportunities.

The disposal of hazardous waste of any form has become a great concern for the industrial sector due to increased environmental awareness. The increase in usage of hydroprocessing catalysts by petrochemical industries and lithium-ion batteries (LIBs) in portable electronics and electric vehicles will soon generate a large amount of scrap and create significant environmental problems. Like general electronic wastes, spent catalysts and LIBs are currently discarded in municipal solid waste and disposed of in landfills in the absence of policy and feasible technology to drive alternatives. Such inactive catalyst materials and spent LIBs not only contain not only hazardous heavy metals but also toxic and carcinogenic chemicals. Besides polluting the environment, these systems (spent catalysts and LIBs) contain valuable metals such as Ni, Mo, Co, Li, Mn, Rh, Pt, and Pd. Therefore, the extraction and recovery of these valuable metals has significant importance. In this Review, we have summarized the strategies used to recover valuable (expensive) as well as cheap metals from secondary resources-especially spent catalysts and LIBs. The first section contains the background and sources of LIBs and catalyst scraps with their current recycling status, followed by a brief explanation of metal recovery methods such as pyrometallurgy, hydrometallurgy, and biometallurgy. The recent advances achieved in these methods are critically summarized. Thus, the Review provides a guide for the selection of adequate methods for metal recovery and future opportunities for the repurposing of recovered materials.

Two-Dimensional Materials for High-Energy Solid-State Asymmetric Pseudocapacitors with High Mass Loadings.

A porous nanostructure and high mass loading are crucial for a pseudocapacitor to achieve a good electrochemical performance. Although pseudocapacitive materials, such as MnO2 and MoS2 , with record capacitances close to their theoretical values have been realized, the achieved capacitances are possible only when the electrode mass loading is less than 1 mg cm-2 . Increasing the mass loading affects the capacitance as electron conduction and ion diffusion become sluggish. Achieving fast ion and electron transport at high mass loadings through all active sites remains a challenge for high-mass-loading electrodes. In this study, 2D MnO2 nanosheets supported on carbon fibers (MnO2 @CF) as well as MoS2 @CF with high mass loadings (6.6 and 7.2 mg cm-2 , respectively) were used in a high-energy pseudocapacitor. These hierarchical 2D nanosheets yielded outstanding areal capacitances of 1187 and 495 mF cm-2 at high current densities with excellent cycling stabilities. A pliable pseudocapacitive solid-state asymmetric supercapacitor was designed using MnO2 @CF and MoS2 @CF as the positive and negative electrodes, respectively, with a high mass loading of 14.2 mg cm-2 . The assembled solid-state asymmetric cell had an energy density of 2.305 mWh cm-3 at a power density of 50 mW cm-3 and a capacitance retention of 92.25 % over 11 000 cycles and a very small diffusion resistance (1.72â€…Ω s-1/2 ). Thus, it is superior to most state-of-the-art reported pseudocapacitors. The rationally designed nanostructured electrodes with high mass loading are likely to open up new opportunities for the development of a supercapacitor device capable of supplying higher energy and power.

Molybdenum Nitride Nanocrystals Anchored on Phosphorus-Incorporated Carbon Fabric as a Negative Electrode for High-Performance Asymmetric Pseudocapacitor.

Pseudocapacitors hold great promise to provide high energy-storing capacity; however, their capacitances are still far below their theoretical values and they deliver much lower power than the traditional electric double-layer capacitors due to poor ionic accessibility. Here, we have engineered MoN nanoparticles as pseudocapacitive material on phosphorus-incorporated carbon fabric with enhanced ionic affinity and thermodynamic stability. This nanocomposite boosts surface redox kinetics, leading to pseudocapacitance of 400 mF/cm2 (2-fold higher than that of molybdenum nitride-based electrodes) with rapid charge-discharge rates. Density functional theory simulations are used to explain the origin of the good performance of MoN@P-CF in proton-based aqueous electrolytes. Finally, an all-pseudocapacitive solid-state asymmetric cell was assembled using MoN@P-CF and RuO2 (RuO2@CF) as negative and positive electrodes, respectively, which delivered good energy density with low relaxation time constant (τ0) of 13 ms (significantly lower than that of carbon-based supercapacitors).

Self-Assembled Nickel Pyrophosphate-Decorated Amorphous Bimetal Hydroxides 2D-on-2D Nanostructure for High-Energy Solid-State Asymmetric Supercapacitor.

To obtain a supercapacitor with a remarkable specific capacitance and rate performance, a cogent design and synthesis of the electrode material containing abundant active sites is necessary. In present work, a scalable strategy is developed for preparing 2D-on-2D nanostructures for high-energy solid-state asymmetric supercapacitors (ASCs). The self-assembled vertically aligned microsheet-structured 2D nickel pyrophosphate (Ni2 P2 O7 ) is decorated with amorphous bimetallic nickel cobalt hydroxide (NiCo-OH) to form a 2D-on-2D nanostructure arrays electrode. The resulting Ni2 P2 O7 /NiCo-OH 2D-on-2D array electrode exhibits peak specific capacity of 281 mA hg-1 (4.3 F cm-2 ), excellent rate capacity, and cycling stability over 10 000 charge-discharge cycles in the positive potential range. The excellent electrochemical features can be attributed to the high electrical conductivity and 2D layered structure of Ni2 P2 O7 along with the Faradic capacitance of the amorphous NiCo-OH nanosheets. The constructed Ni2 P2 O7 /NiCo-OH//activated carbon based solid-state ASC cell operates in a high voltage window of 1.8 V with an energy density of 78 Wh kg-1 (1.065 mWh cm-3 ) and extraordinary cyclic stability over 10 000 charge-discharge cycles with excellent energy efficiency (75%-80%) over all current densities. The excellent electrochemical performance of the prepared electrode and solid-state ASC device offers a favorable and scalable pathway for developing advanced electrodes.

Tungsten Nitride Nanodots Embedded Phosphorous Modified Carbon Fabric as Flexible and Robust Electrode for Asymmetric Pseudocapacitor.

Owing to the excellent physical properties of metal nitrides such as metallic conductivity and pseudocapacitance, they have recently attracted much attention as competitive materials for high-performance supercapacitors (SCs). However, the voltage window for metal nitride-based symmetric SCs is limited (0.6-0.8 V) in aqueous electrolyte due to the oxidation at high negative potentials. In this respect, ultra-small tungsten nitride particles onto the phosphorous modified carbon fabric (W2 N@P-CF) are engineered as a promising hybrid electrode for pseudocapacitors. Additionally, the fact that the W2 N@P-CF electrode can operate in the negative potential region is exploited to design asymmetric pseudocapacitors by coupling with a polypyrrole on carbon fabric (PPy@CF) as the positive electrode. Remarkably, the W2 N@P-CF//PPy@CF asymmetric cell can be cycled in a wide voltage window of 1.6 V that is almost two times higher than that of metal nitrides symmetric SCs. The pseudocapacitive behavior with matching different potential regions of W2 N@P-CF and PPy@CF, considerably enhance performance of asymmetric device. The device delivers high volumetric capacity (7.1 F cm-3 ), high energy (2.54 mWh cm-3 ), power densities, and good cycling stability (88%) over 20 000 cycles. Thus, pseudocapacitive metal nitride-based devices hold a great promise to provide high voltage and improved energy density in aqueous electrolyte.