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A flexible Prussian blue electrode has been finely fabricated by galvanic-driven deposition for building mechanically stable Zn/PB flexible battery-type electrochromic devices.

A surface-grafting strategy of molecular brushes is demonstrated to create a robust ion-regulating interface toward calendar-life Zn anodes with a high Coulombic efficiency of 99.9% and ultralong cyclability over 2500 h at 10 mA cm−2.

Proton exchange membrane fuel cells convert hydrogen and oxygen into electricity without emissions. The high cost and low durability of Pt-based electrocatalysts for the oxygen reduction reaction hinder their wide application, and the development of non-precious metal electrocatalysts is limited by their low performance. Here we design a hybrid electrocatalyst that consists of atomically dispersed Pt and Fe single atoms and Pt–Fe alloy nanoparticles. Its Pt mass activity is 3.7 times higher than that of commercial Pt/C in a fuel cell. More importantly, the fuel cell with a low Pt loading in the cathode (0.015 mgPt cm−2) shows an excellent durability, with a 97% activity retention after 100,000 cycles and no noticeable current drop at 0.6 V for over 200 hours. These results highlight the importance of the synergistic effects among active sites in hybrid electrocatalysts and provide an alternative way to design more active and durable low-Pt electrocatalysts for electrochemical devices.

Surface charge recombination is regarded as a detrimental factor that severely downgrades the photoelectrochemical (PEC) performance of bismuth vanadate (BiVO

NiHCF nanocubes are in situ etched away and simultaneously induce the reconstruction of underneath Ni(OH)2 to form highly disordered Fe–Ni(O)OH.

A universal and versatile metal–organic complex interphase strategy is proposed as a splendid dendrite and corrosion inhibitor for achieving ultrastable Zn anodes with substantially improved Coulombic efficiency and extended cycling lifetime.

A self-adaptive semiconductor–liquid junction with reduced interface recombination and fast water oxidation kinetics is constructed via a novel and efficient reconstruction strategy for highly active and stable solar water splitting.

Hard carbons as a kind of nongraphitized amorphous carbon have been recognized as potential anode materials for sodium-ion batteries (SIBs) due to its large interlayer spacing. However, the issues in terms of onerous synthetic procedure and elusive working mechanism remains critical bottlenecks for practical implement. Herein, we report a facile production of tubular hard carbon through direct carbonization of platanus flosses (FHC) for the first time. Through optimizing the pyrolysis temperatures, the FHC obtained at 1300 °C possesses a key balance between the interlayer spacing and surface area, which can maintain the substantial active sites as well as reduce the irreversible sodium storage. Accordingly, it can deliver a reversible capacity of 324.6 mAh g

Formamidinium-lead triiodide (FAPbI

Corrosion engineering is an efficient strategy to achieve durable oxygen evolution reaction (OER) catalysts at high current densities beyond 500 mA cm

Rechargeable aqueous zinc-ion batteries hold great prospects in grid-level energy storage due to their virtues of good safety, low cost and eco-friendliness. However, the sluggish intercalation kinetics of divalent Zn2+ makes the exploration of a suitable Zn2+-host cathode being a formidable challenge. In this work, we unveil the crucial role of crystal water on boosting the Zn2+ intercalation kinetics of layered MoS2 host. The crystal water molecules could function as structural pillars to enlarge the interlayer distance of MoS2 and improve the surface hydrophilicity. Notably, a substantially-enhanced Zn2+ intercalation kinetics is realized by accelerating the charge-transfer transportation and Zn2+ diffusivity. Consequently, the hydrated MoS2 nanosheets enable efficacious Zn2+ insertion/extraction to achieve a high specific capacity of 182 mAh g−1 at 0.1 A g−1 and superior rate/cycling performance. The present study will enlighten the water implantation strategy to engineering hydrated cathode materials toward high-performance aqueous batteries.

Rechargeable aqueous zinc-ion batteries (ZIBs) are considered to be one of the most promising energy storage devices for grid-scale applications due to their high safety, eco-friendliness, and low cost. In recent years, enormous efforts have been devoted to developing a great number of high-efficient cathodes, anodes, and electrolytes for improving the electrochemical properties of aqueous ZIBs. However, the as-documented ZIBs and their associated energy storage mechanisms are still in infancy and need to be further investigated for real practice. To expedite the development of ZIBs, this review will offer a comprehensive summary and a detailed discussion of the significant progress and breakthroughs. A brief overview of the battery configuration and various energy storage mechanisms are first introduced. The following emphasis will be mainly dedicated to discussing different design strategies regarding cathodes, anodes, and electrolytes, aiming to provide insightful design principles for future research activities from a fundamental perspective. Finally, the current challenges of developing high-performance ZIBs and their opportunities for practical viability are discussed.

Lithium-sulfur batteries are recognized as a promising high-energy-density and low-cost energy storage devices. However, the sulfur cathode suffers from poor cycling stability resulting from the serious polysulfide shuttle. Herein, we develop a nitrogen-rich and highly porous carbon polyhedron for effectively hosting sulfur. The carbon host manifests an ultrahigh specific surface area of 3400 m2 g−1, a dominated micropore volume of 0.96 cm3 g−1, and a high-level nitrogen doping of 8.3 at.%. Such an intriguing structure could suppress the polysulfide shuttle via physical confinement by micropores and strong chemical adsorption by polar nitrogen species. Moreover, the electrically conductive carbon enables a substantially enhanced electrochemical kinetics. Consequently, the carbon/sulfur composite electrode delivers an ultralow fading rate of 0.033% per cycle at 2 C over 500 cycles and superior rate capability (483 mAh g−1 at a high 5 C rate). The present study demonstrates the potential use of nitrogen-rich porous carbon framework as an efficient polysulfide host for lithium-sulfur batteries.

Achieving enhanced photoelectrochemical (PEC) activity and stability of a photoanode remains as a formidable challenge. In this study, a porous tannin nickel iron complex coated WO₃/BiVO₄ heterojunction (WO₃/BiVO₄@TANiFe) is constructed to achieve enhanced PEC activity and stability. The in situ construction of a type-II heterostructure is highly beneficial for broad visible light utilization and efficient separation of photogenerated carriers. In addition, the intact coating of ultrathin tannin nickel iron nanolayer could not only accelerate the reaction kinetics of water oxidation but also safeguard the semiconductors from photocorrosion during the PEC reaction. As a result, the as-designed WO₃/BiVO₄@TANiFe ternary photoelectrode exhibits an outstanding photocurrent density of 3.7 mA cm–² at 1.23 V vs RHE with substantially enhanced running durability at high photocurrent density. The present study would provide a rational route for developing highly active and stable photoanodes for solar-energy conversion applications.

The core challenge of MnO2 as the cathode material of zinc-ion batteries remains to be their poor electrochemical kinetics and stability. Herein, MnO2 superfine nanowires (∼10 nm) with rich crystal defects (oxygen vacancies and cavities) are demonstrated to possess high efficient zinc-ion storage capability. Experimental and theoretical studies demonstrate that the defects facilitate the adsorption and diffusion of hydrogen/zinc for fast ion transportation and the build of a local electric field for improved electron migration. In addition, the superfine nanostructure could provide sufficient active sites and short diffusion pathways for further promotion of capacity and reaction kinetics of MnO2. Remarkably, the defect-enriched MnO2 nanowires manifest an energy density as high as 406 W h kg-1 and an excellent durability over 1000 cycles without noticeable capacity degradation. Mechanistic analysis substantiates a reversible coinsertion/extraction process of H+ and Zn2+ with a simultaneous deposition/dissolution of zinc sulfate hydroxide hydrate nanoflakes. This work could enrich the fundamental understanding of defect engineering and nanostructuring on the development of advanced MnO2 materials toward high-performance zinc-ion batteries.

Water electrolysis has been considered as a sustainable way for producing renewable energy of hydrogen. However, this process requires a low-cost and high-efficient hydrogen evolution reaction (HER) catalyst to improve the overall reaction efficiency. Molybdenum (Mo)-based electrocatalysts are regarded as the promising candidates to replace the benchmark but expensive Pt-based HER catalysts, due to their high activity and stability in a wide pH range. In this review, we present a comprehensive and critical summary on the recent progress in the Mo-based electrodes for HER, including molybdenum alloys, molybdenum sulfides, molybdenum selenides, molybdenum carbides, molybdenum phosphides, molybdenum borides, molybdenum nitrides, and molybdenum oxides. Particular attention is mainly focused on the synthetic methods of Mo-based materials, the strategies for increasing the catalytic activity, and the relationship between structure/composition and electrocatalytic performance. Finally, the future development and perspectives of Mo-based electrocatalysts toward high HER performance are proposed.

Surface Fe with low-coordination plays a decisive role in the performance of OER catalysts in basic media, however, it is still a huge challenge to construct a Fe-enriched surface. Herein, a novel S-incorporation and ligand anchoring strategy is reported for in-situ synthesis of surface-Fe enriched OER catalysts. During the OER test, the co-etching of S elements and ligands enables the formation of surface-Fe enriched trimetallic (oxy)hydroxide OER catalysts. Benefiting from the high catalytic activity of Fe enriched species on surface, the electrode delivers an ultralow overpotential of 234 mV to reach the current density of 10 mA cm

Hierarchically two-dimensional (2D) heteroarchitecture with ultrafine MoS2 nanosheets vertically patterned on graphene is developed by using a facile solvothermal method. It is revealed that the strong interfacial interaction between acidic Mo precursors and graphene oxides allows for uniform and tight alignment of edge-oriented MoS2 nanosheets on planar graphene. The unique sheet-on-sheet architecture is of grand advantage in synergistically utilizing the highly conductive graphene and the electroactive MoS2, thus rendering boosted reaction kinetics and robust structural integrity for energy storage. Consequently, the heterostructured MoS2@graphene exhibits impressive Li/Na-ion storage properties, including high-capacity delivery and superior rate/cycling capability. The present study will provide a positive impetus on rational design of 2D metal sulfide/graphene composites as advanced electrode materials for high-efficient alkali–metal ion storage.

Hierarchically two-dimensional (2D) heteroarchitecture with ultrafine MoS2 nanosheets vertically patterned on graphene is developed by using a facile solvothermal method. It is revealed that the strong interfacial interaction between acidic Mo precursors and graphene oxides allows for uniform and tight alignment of edge-oriented MoS2 nanosheets on planar graphene. The unique sheet-on-sheet architecture is of grand advantage in synergistically utilizing the highly conductive graphene and the electroactive MoS2, thus rendering boosted reaction kinetics and robust structural integrity for energy storage. Consequently, the heterostructured MoS2@graphene exhibits impressive Li/Na-ion storage properties, including high-capacity delivery and superior rate/cycling capability. The present study will provide a positive impetus on rational design of 2D metal sulfide/graphene composites as advanced electrode materials for high-efficient alkali–metal ion storage.

Proton exchange membrane fuel cell converts hydrogen and oxygen into electricity with zero emission1. The high cost and low durability of Pt-based electrocatalysts for oxygen reduction reaction hinder its wide applications2,3. The development of non-precious metal electrocatalysts also reaches the bottleneck because of the low activity and durability4,5. Here we rationally design a hybrid electrocatalyst consisting of atomically dispersed Pt and Fe single atoms and intermetallic PtFe alloy nanoparticles. The Pt mass activity of the hybrid catalyst is 3.5 times higher than that of commercial Pt/C in a fuel cell. More importantly, the fuel cell with an ultra-low Pt loading in the cathode (0.015 mgPt cm-2) shows unprecedented durability, with 93.6% activity retention after 100,000 cycles and no noticeable current drop at 0.6 V for at least 206 h. These results highlight the importance of the synergistic effects among active sites in hybrid electrocatalysts and provide an alternative way to design more active and durable low-Pt electrocatalysts for electrochemical devices.

Iron and nitrogen co-doped carbon (Fe-N-C) catalysts hold great promise to replace platinum group metal used for the oxygen reduction reaction (ORR) in low-temperature fuel cells. However, general synthesis routes require tedious acid washing and extensive heat treatment, usually resulting in uncontrollable morphologies and undesirable compounds. In this work, a zeolitic imidazolate framework (ZIF-8) was employed as a self-template for one-pot synthesis of a Fe-N-C catalyst consisting of uniformly dispersed Fe single atoms. Atomically dispersed Fe atoms were well distributed along the edges of the porous carbon matrix. Each of the Fe atoms was coordinated with four N atoms in the plane and two O atoms in the axial direction. The optimized Fe-N-C catalyst showed excellent ORR activities with half-wave potentials of 0.81 and 0.90 V in acidic and alkaline solutions, respectively. The results may be important for the optimization of single-atom-based catalysts for various reactions.

Achieving a high photocatalytic activity toward photoelectrochemical (PEC) water splitting has become a formidable challenge for titanium oxide (TiO2) owing to its poor photoresponse to visible light and low electrical conductivity. Herein, we report the first demonstration of nonmetal TiN as a plasmonic booster to significantly enhancing the PEC water splitting performance of TiO2. A unique multiscaled architecture organized by interweaving hollow microfiber monolith and hierarchical TiN/N-TiO2 nanorod arrays is fabricated by a facile seamless nitridation process. The conductive TiN not only affords plasmon resonance on the N-TiO2 to enable high photoactivity in a broadband UV–vis light region, but also assists in the charge generation-separation-transportation-injection efficiency of TiO2 for enhanced water oxidation kinetics. The TiN/N-TiO2 heterostructure manifests an unprecedented high and durable photocurrent density of 3.12 mA cm−2 at 1.23 V (vs. reversible hydrogen electrode (RHE)) under standard AM 1.5 G illumination and substantiates an outstanding visible-light-driven photocurrent density of 1.63 mA cm−2 without the use of any hole scavenger and cocatalysts. This study will enrich the fundamental understanding of nonmetal plasmonic effect in and beyond the field of PEC water splitting.

The increasing demand for renewable energy boosts the exploration of energy conversion and storage devices, which to a large extent depends on the development of reliable electrode materials. In this work, hierarchically-structured MoO2/N-doped carbon hydrangea-like spheres (designated as MoO2/N-C thereafter) self-assembled from mesoporous nanosheets are successfully prepared via a facile hydrothermal reaction and a subsequent annealing process. Benefiting from the hierarchically mesoporous architecture, nanosheet configuration, and electrically conductive carbon matrix, the hydrangea-like MoO2/N-C spheres possess favorable electrochemical features including sufficient electrode/electrolyte interfacial areas, shortened ion diffusion length, and promoted reaction kinetics. Accordingly, the MoO2/N-C hybrid shows excellent electrochemical performance, delivering a large specific capacity of 899 mAh g−1 with an initial Coloumbic efficiency as high as 82.9% as well as long-term cycling performance. In addition, outstanding rate capability can be achieved with a high capacity retention of 400 mAh g−1 at 2000 mA g−1, which substantially outperforms that of the commercial MoO2 nanoparticles. The present study suggests the great potential of MoO2/N-C spheres as high-performance electrode materials for advanced energy storage applications.

As a new class of promising anode materials for Li-ion batteries, the application of transition metal oxides is hindered by poor electrochemical utilization and stability. In this work, we report a unique hollow structure of carbon-encapsulated MoO2 nanospheres as a high-rate and durable anode material for Li-ion batteries. Three-dimensional hierarchically porous carbon hollow nanospheres provide a universal and open framework for encapsulating MoO2 nanodeposits by a facile impregnation-calcination approach. The hybrid architecture is of great benefit in fast and stable Li-ion storage by shortening Li-ion and electron transport pathways, increasing electronic conductivity, and buffering volume fluctuation upon cycling. The electrochemical advantages bestow the MoO2/C nanocomposite with an outstanding specific capacity of 1051 mAh g−1 at 0.1 A g−1, superb rate capability (701 mAh g−1 at 2 A g−1) and excellent cycling stability. The present study demonstrates the promising use of hollow-structured MoO2/C nanocomposites for high performance Li-ion batteries.

Achieving fast and stable Li-ion energy storage in two-dimensional MoS2 materials has become a formidable challenge due to their sluggish electrochemical reaction kinetics and large structural chan...

Two-dimensional MoS2 is a promising anode material for Li-ion batteries, but suffers from poor electrochemical activity and stability. Herein, a facile approach for the controlled synthesis of onion-like nanospheres organized by carbon encapsulated MoS2 nanosheets is developed through a simple polymerization and sulfidation/carbonation process. Mo-containing polyoxometalate is demonstrated to enable polymerization of polypyrrole accompanying with uniform encapsulation of Mo-nanoclusters. The hybrid precursor confines the growth of few-layer MoS2 nanosheets (≤5 layers) into N-doped carbon framework, which is of great benefit in enhancing the electrical conductivity and structural integrity. As a result, the nanospherical MoS2@C hybrid electrode manifests high Li-ion storage capacity (1119 mAh g−1 at 0.1 A g−1), excellent rate capability (616 mAh g−1 at 2 A g−1), and long cycling stability. The substantial improvement is rationalized by fast electrode kinetics and great pseudocapacitive contribution. The present work may offer a powerful engineering strategy of MoS2@C nanomaterials for Li/Na-ion batteries and electrocatalysts.

Potassium-ion batteries (KIBs) with potential cost benefits are a promising alternative to lithium-ion batteries (LIBs). However, because of the large radius of K+, current anode materials usually undergo large volumetric expansion and structural collapse during the charge-discharge process. Self-supporting carbon nanotubes encapsulated in sub-micro carbon fiber (SMCF@CNTs) are utilized as the KIB anode in this study. The SMCF@CNT anode exhibits high specific capacity, good rate performance, and cycling stability. The SMCF@CNT electrode has specific capacities of 236 mAh g-1 at 0.1 C and 108 mAh g-1 at 5 C and maintains over 193 mAh g-1 after 300 cycles at 1 C. Furthermore, a combined capacitive and diffusion-controlled K+ storage mechanism is proposed on the basis of the investigation using in situ Raman and quantitative analyses. By coupling the SMCF@CNT anode with the K0.3MnO2 cathode, a pouch cell with good flexibility delivers a capacity of 74.0 mAh g-1 at 20 mA g-1. This work is expected to promote the application of KIBs in wearable electronics.