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Designing high-performance electrocatalysts with superior catalytic activity and stability is essential for large-scale hydrogen production via water electrolysis. Heterostructure nanoarrays are promising candidates, though achieving both high activity and stability simultaneously, especially under high current densities, remains challenging. To this end, we have developed a cascade reaction process that constructs a series of heterostructure nanoarrays with rich heterointerfaces. This process involves treating nickel foam (NF) with molten KSCN and transition metal salts. Initially, NF reacts with KSCN to form Ni 9 S 8 nanoarrays and S 2- ions, which are subsequently captured by transition metal ions to form sulfides that are directly integrated onto the nanoarrays, resulting in abundant heterointerfaces. Both experimental and theoretical results indicate that these rich heterointerfaces significantly enhance the interfacial interaction between Ni 9 S 8 and RuS 2 within the nanoarrays (termed RH-Ni 9 S 8 /RuS 2 ), markedly improving both the intrinsic activity and stability for the hydrogen evolution reaction (HER). Impressively, the RH-Ni 9 S 8 /RuS 2 demonstrates exceptional HER performance, achieving a low overpotential of just 180 mV at 1000 mA cm -2 and maintaining stability for up to 500 h under such high-current-density conditions. This innovative approach paves the way for the interfacial design and synthesis of high-performance catalysts for ampere-level hydrogen production., (© 2024 Wiley-VCH GmbH.)

Blade-coating techniques have attracted significant attention for perovskite solar cells (PSCs) due to their high precursor utilization and simplicity. However, the power conversion efficiency (PCE) of blade-coated PSCs often lags behind that of spin-coated devices, mainly due to difficulties in precisely controlling perovskite film formation during pre-nucleation, heterogeneous nucleation, and crystallization in the blade-coating and N 2 -knife drying processes. In this work, a three-step restraining strategy is introduced utilizing functional glycine amide hydrochloride to regulate pre-nucleation clustering, suppress excessive heterogeneous nucleation, and decelerate crystallization, enabling comprehensive control of the perovskite film formation processes. This approach results in enlarged grains, reduced defect densities, and highly oriented crystalline wide-bandgap perovskite films with significantly prolonged carrier lifetimes, achieving a maximum PCE of 19.97% for 1.77 eV-bandgap blade-coated PSCs. Furthermore, two-terminal tandem cells, composed of wide-bandgap perovskite top cells and 1.25 eV-bandgap perovskite bottom cells fabricated via blade coating, yield an impressive PCE of 27.11% (stabilized at 26.87%). This study offers comprehensive insights into controlling pre-nucleation, heterogeneous nucleation, and crystallization during blade coating, providing valuable guidance for developing high-performance, large-area devices in the future., (© 2024 Wiley‐VCH GmbH.)

Controlling exchange bias (EB) by electric fields is crucial for next-generation magnetic random access memories and spintronics with ultralow energy consumption and ultrahigh speed. Multiferroic heterostructures have been traditionally used to electrically control EB and interfacial ferromagnetism through weak/indirect coupling between ferromagnetic and ferroelectric films. However, three major bottlenecks (lattice mismatch, interface defects, and weak/indirect coupling in multiferroic heterostructures) remain, resulting in only a few tens of milli-tesla EB field. Here, this study reports a robust electric-field control recipe to dynamically tailor the EB effect in a pure CrI 3 homotrilayer on a ferroelectric Y-doped HfO 2 (HYO) substrate, and demonstrate a colossal and tunable EB field (H E ) from -0.15 to +0.33 T, giving rise to an EB modulation of 0.48 T. The charge doping due to ferroelectric HYO film divides a homo-configuration of CrI 3 homotrilayer into one antiferromagnetic (AFM) bilayer CrI 3 and one ferromagnetic (FM) monolayer CrI 3 , favoring direct exchange coupling. The synergies of charge doping and electric field induce a transition of magnetic orders from AFM to FM phase in bilayer CrI 3 , which is also supported by first-principles calculations, leading to the robust electric control of colossal EB effect. The results therefore open numerous opportunities for exploring 2D spintronics, memories, and braininspired in-memory computing., (© 2024 Wiley‐VCH GmbH.)

Magnesium metal batteries (MMBs), recognized as promising contenders for post-lithium battery technologies, face challenges such as uneven magnesium (Mg) plating and stripping behaviors, leading to uncontrollable dendrite growth and irreversible structural damage. Herein, we have developed a Mg foil featuring prominently exposed (002) facets and an architecture of nanosheet arrays (termed (002)-Mg), created through a one-step acid etching method. Specifically, the prominent exposure of Mg (002) facets, known for their inherently low surface and adsorption energies with Mg atoms, not only facilitates smooth nucleation and dense deposition but also significantly mitigates side reactions on the Mg anode. Moreover, the nanosheet arrays on the surface evenly distribute the electric field and Mg ion flux, enhancing Mg ion transfer kinetics. As a result, the fabricated (002)-Mg electrodes exhibit unprecedented long-cycle performance, lasting over 6000 h (>8 months) at a current density of 3 mA cm -2 for a capacity of 3 mAh cm -2 . Furthermore, the corresponding pouch cells equipped with various electrolytes and cathodes demonstrate remarkable capacity and cycling stability, highlighting the superior electrochemical compatibility of the (002)-Mg electrode. This study provides new insights into the advancement of durable MMBs by modifying the crystal structure and morphology of Mg., (© 2024 Wiley-VCH GmbH.)

Electrocatalytic conversion of CO 2 into formate is recognized an economically-viable route to upgrade CO 2 , but requires high overpotential to realize the high selectivity owing to high energy barrier for driving the involved proton-coupled electron transfer (PCET) processes and serious ignorance of the second PCET. Herein, we surmount the challenge through sequential regulation of the potential-determining step (PDS) over Te-doped Bi (TeBi) nanotips. Computational studies unravel the incorporation of Te heteroatoms alters the PDS from the first PCET to the second one by substantially lowering the formation barrier for *OCHO intermediate, and the high-curvature nanotips induce enhanced electric field that can steer the formation of asymmetric *HCOOH. In this scenario, the thermodynamic barrier for *OCHO and *HCOOH can be sequentially decreased, thus enabling a high formate selectivity at low overpotential. Experimentally, distinct TeBi nanostructures are obtained via controlling Te content in the precursor and TeBi nanotips achieve >90 % of Faradaic efficiency for formate production over a comparatively positive potential window (-0.57 V to -1.08 V). The strong Bi-Te covalent bonds also afford a robust stability. In an optimized membrane electrode assembly device, the formate production rate at 3.2 V reaches 10.1 mmol h -1  cm -2 , demonstrating great potential for practical application., (© 2024 Wiley-VCH GmbH.)

Narrow-bandgap (NBG) mixed tin-lead (Sn-Pb) perovskite solar cells (PSCs) serve as crucial top subcells in all-perovskite tandem solar cells (TSCs). However, the prevalent use of poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT: PSS) hole transport layers (HTLs) in NBG PSCs compromises device efficiency and stability. To address this, the study proposes a revitalizing strategy for the buried interface of Sn-Pb perovskites by directly immersing acetylcholine chloride (ACh) into PEDOT: PSS. ACh acts as a proficient "diver," not only modulating the bottom PEDOT: PSS HTLs but also facilitating the reconstruction of the buried interface and significantly enhancing the quality of the top perovskite layers. This intervention with ACh prevents Sn 2+ oxidation, mitigates buried defects, and encourages the growth of large, densely packed grains within Sn-Pb perovskites. Consequently, the optimized NBG PSCs exhibit significantly improved hole transport and reduced carrier recombination, achieving a steady-state efficiency of 22.98% with enhanced stability. Furthermore, these optimized NBG Sn-Pb cells enable highly efficient two-terminal and four-terminal all-perovskite TSCs, boasting steady-state efficiencies of 27.54% (certified at 26.41%) and 28.01%, respectively. This study emphasizes the importance of optimizing NBG PSCs through buried interface reconstruction, propelling the advancement of all-perovskite TSCs., (© 2024 Wiley‐VCH GmbH.)

1T-MoSe 2 is recognized as a promising anode material for sodium-ion batteries, thanks to its excellent electrical conductivity and large interlayer distance. However, its inherent thermodynamic instability often presents unparalleled challenges in phase control and stabilization. Here, a molecular intercalation strategy is developed to synthesize thermally stable 1T-rich MoSe 2 , covalently bonded to an intercalated carbon layer (1T R /2H-MoSe 2 @C). Density functional theory calculations uncover that the introduced ethylene glycol molecules not only serve as electron donors, inducing a reorganization of Mo 4d orbitals, but also as sacrificial guest materials that generate a conductive carbon layer. Furthermore, the C─Se/C─O─Mo bonds encourage strong interfacial electronic coupling, and the carbon layer prevents the restacking of MoSe 2 , regulating the maximum 1T phase to an impressive 80.3%. Consequently, the 1T R /2H-MoSe 2 @C exhibits an extraordinary rate capacity of 326 mAh g -1 at 5 A g -1 and maintains a long-term cycle stability up to 1500 cycles, with a capacity of 365 mAh g -1 at 2 A g -1 . Additionally, the full cell delivers an appealing energy output of 194 Wh kg -1 at 208 W kg -1 , with a capacity retention of 87.3% over 200 cycles. These findings contribute valuable insights toward the development of innovative transition metal dichalcogenides for next-generation energy storage technologies., (© 2024 Wiley‐VCH GmbH.)

Achieving a high depth of discharge (DOD) in lithium metal anodes (LMAs) is crucial for developing high areal energy density batteries suitable for wearable electronics. Yet, the persistent growth of dendrites compromises battery performance, and the significant lithium consumption during pre-lithiation obstructs their broad application. Herein, A flexible 3D Li 13 Sn 5 scaffold is designed by allowing molten lithium to infiltrate carbon cloth adorned with SnO 2 nanocrystals. This design markedly curbs the troublesome dendrite growth, thanks to the uniform electric field distribution and swift Li + diffusion dynamics. Additionally, with a minimal SnO 2 nanocrystals loading (2 wt.%), only 0.6 wt.% of lithium is consumed during pre-lithiation. Insights from in situ optical microscope observations and COMSOL simulations reveal that lithium remains securely anchored within the scaffold, a result of the rapid mass/charge transfer and uniform electric field distribution. Consequently, this electrode achieves a remarkable DOD of 87.1% at 10 mA cm -2 for 40 mAh cm -2 . Notably, when coupled with a polysulfide cathode, the constructed flexible Li/Li 13 Sn 5 @CC||Li 2 S 6 /SnO 2 @CC pouch cell delivers a high-areal capacity of 5.04 mAh cm -2 and an impressive areal-energy density of 10.6 mWh cm -2 . The findings pave the way toward the development of high-performance LMAs, ideal for long-lasting wearable electronics., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

The development of advanced magnesium metal batteries (MMBs) has been hindered by longstanding challenges, such as the inability to induce uniform magnesium (Mg) nucleation and the inefficient utilization of Mg foil. This study introduces a novel solution in the form of a flexible, lightweight, paper-based scaffold that incorporates gradient conductivity, magnesiophilicity, and pore size. This design is achieved through an industrially adaptable papermaking process in which the ratio of carboxylated multi-walled carbon nanotubes to softwood cellulose fibers is meticulously adjusted. The triple-gradient structure of the scaffold enables the regulation of Mg ion flux, promoting bottom-up Mg deposition. Owing to its high flexibility, low thickness, and reduced density, the scaffold has potential applications in flexible and wearable electronics. Accordingly, the triple-gradient electrodes exhibit stable operation for over 1200 h at 3 mA cm -2 /3 mAh cm -2 in symmetrical cells, markedly outperforming the non-gradient and metallic Mg alternatives. Notably, this study marks the first successful fabrication of a flexible MMB pouch full cell, achieving an impressive volumetric energy density of 244 Wh L -1 . The simplicity and scalability of the triple-gradient design, which uses readily available materials through an industrially compatible papermaking process, open new doors for the production of flexible, high-energy-density metal batteries., (© 2023 Wiley-VCH GmbH.)

Hosts hold great prospects for addressing the dendrite growth and volume expansion of the Li metal anode, but Li dendrites are still observable under the conditions of high deposition capacity and/or high current density. Herein, a nitrogen-doped graphene mesh (NGM) is developed, which possesses a conductive and lithiophilic scaffold for efficient Li deposition. The abundant nanopores in NGM can not only provide sufficient room for Li deposition, but also speed up Li ion transport to achieve a high-rate capability. Moreover, the evenly distributed N dopants on the NGM can guide the uniform nucleation of Li so that to inhibit dendrite growth. As a result, the composite NGM@Li anode shows satisfactory electrochemical performances for Li-S batteries, including a high capacity of 600 mAh g -1 after 300 cycles at 1 C and a rate capacity of 438 mAh g -1 at 3 C. This work provides a new avenue for the fabrication of graphene-based hosts with large areal capacity and high-rate capability for Li metal batteries., (© 2023 Wiley-VCH GmbH.)

Nanoarray electrocatalysts with unique advantage of facilitating gas bubble detachment have garnered significant interest in gas evolution reactions (GERs). Existing research is largely based on a static hypothesis, assuming that buoyancy is the only driving force for the release of bubbles during GERs. However, this hypothesis overlooks the effect of the self-dynamic electrolyte flow, which is induced by the release of mature bubbles and helps destabilize and release the smaller, immature bubbles nearby. Herein, the enhancing effect of self-dynamic electrolyte flow on nanoarray structures is examined. Phase-field simulations demonstrate that the flow field of electrode with arrayed surface focuses shear force directly onto the gas bubble for efficient detachment, due to the flow could pass through voids and channels to bypass the shielding effect. The flow field therefore has a more substantial impact on the arrayed surface than the nanoscale smooth surface in terms of reducing the critical bubble size. To validate this, superaerophobic ferrous-nickel sulfide nanoarrays are fabricated and employed for water splitting, which display improved efficiency for GERs. This study contributes to understanding the influence of self-dynamic electrolyte on GERs and emphasizes that it should be considered when designing and evaluating nanoarray electrocatalysts., (© 2023 Wiley-VCH GmbH.)

3D Cu current collectors have been demonstrated to improve the cycling stability of Li metal anodes, however, the role of their interfacial structure for Li deposition pattern has not been investigated thoroughly. Herein, a series of 3D integrated gradient Cu-based current collectors are fabricated by the electrochemical growth of CuO nanowire arrays on Cu foil (CuO@Cu), where their interfacial structures can be readily controlled by modulating the dispersities of the nanowire arrays. It is found that the interfacial structures constructed by sparse and dense dispersion of CuO nanowire arrays are both disadvantageous for the nucleation and deposition of Li metal, consequently fast dendrite growth. In contrast, a uniform and appropriate dispersity of CuO nanowire arrays enables stable bottom Li nucleation associated with smooth lateral deposition, affording the ideal bottom-up Li growth pattern. The optimized CuO@Cu-Li electrodes exhibit a highly reversible Li cycling including a coulombic efficiency of up to ≈99% after 150 cycles and a long-term lifespan of over 1200 h. When coupling with LiFePO 4 cathode, the coin and pouch full-cells deliver outstanding cycling stability and rate capability. This work provides a new insight to design the gradient Cu current collectors toward high-performance Li metal anodes., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Lithium-sulfur batteries (LSBs) with superior energy density are among the most promising candidates of next-generation energy storage techniques. As the key step contributing to 75% of the overall capacity, Li 2 S deposition remains a formidable challenge for LSBs applications because of its sluggish kinetics. The severe kinetic issue originates from the huge interfacial impedances, indicative of the interface-dominated nature of Li 2 S deposition. Accordingly, increasing efforts have been devoted to interface engineering for efficient Li 2 S deposition, which has attained inspiring success to date. However, a systematic overview and in-depth understanding of this critical field are still absent. In this review, the principles of interface-controlled Li 2 S precipitation are presented, clarifying the pivotal roles of electrolyte-substrate and electrolyte-Li 2 S interfaces in regulating Li 2 S depositing behavior. For the optimization of the electrolyte-substrate interface, efforts on the design of substrates including metal compounds, functionalized carbons, and organic compounds are systematically summarized. Regarding the regulation of electrolyte-Li 2 S interface, the progress of applying polysulfides catholytes, redox mediators, and high-donicity/polarity electrolytes is overviewed in detail. Finally, the challenges and possible solutions aiming at optimizing Li 2 S deposition are given for further development of practical LSBs. This review would inspire more insightful works and, more importantly, may enlighten other electrochemical areas concerning heterogeneous deposition processes., (© 2023 Wiley-VCH GmbH.)

Electrodes made of composites with heterogeneous structure hold great potential for boosting ionic and charge transfer and accelerating electrochemical reaction kinetics. Herein, hierarchical and porous double-walled NiTeSe-NiSe 2 nanotubes are synthesized by a hydrothermal process assisted in situ selenization. Impressively, the nanotubes have abundant pores and multiple active sites, which shorten the ion diffusion length, decrease Na + diffusion barriers, and increase the capacitance contribution ratio of the material at a high rate. Consequently, the anode shows a satisfactory initial capacity (582.5 mA h g -1 at 0.5 A g -1 ), a high-rate capability, and long cycling stability (1400 cycles, 398.6 mAh g -1 at 10 A g -1 , 90.5% capacity retention). Moreover, the sodiation process of NiTeSe-NiSe 2 double-walled nanotubes and underlying mechanism of the enhanced performance are revealed by in situ and ex situ transmission electron microscopy and theoretical calculations., (© 2023 Wiley-VCH GmbH.)

Atomically dispersed Zn moieties are efficient active sites for accelerating the electrode kinetics of carbons for sodium-ion hybrid capacitors (SIHCs), but the low utilization and symmetric configuration of Zn single-atom greatly hamper the Na ion storage capability. Herein, a molecular design strategy is employed to synthesize high-density Zn single atoms with asymmetric Zn-N 3 S coordination embedded in nitrogen/sulfur codoped carbon (Zn-N 3 S-NSC). The key to this strategy lies in the Zn power-catalyzed condensation of trithiocyanuric acid molecules to generate S-doped g-C 3 N 4 , which can in situ coordinate with Zn sources to form Zn-N 3 S moieties during pyrolysis. By virtue of the highly exposed Zn-N 3 S moieties, Zn-N 3 S-NSC presents ultrahigh reactivity, efficient electron transfer, and decreased ion diffusion barriers for SIHCs, rendering an impressive energy density of 215 Wh kg -1 and a maximum power density of 15625 W kg -1 . Moreover, the pouch cell displays a high capacity of 279 mAh g -1 after 4000 cycles. This work provides a new avenue for the regulation of the coordination configuration of single metal atoms in carbons toward high-performance electrochemical energy technologies at the molecular level., (© 2023 Wiley-VCH GmbH.)

Graphene has long been recognized as a potential anode for next-generation lithium-ion batteries (LIBs). The past decade has witnessed the rapid advancement of graphene anodes, and considerable breakthroughs are achieved so far. In this review, the aim is to provide a research roadmap of graphene anodes toward practical LIBs. The Li storage mechanism of graphene is started with and then the approaches to improve its electrochemical performance are comprehensively summarized. First, morphologically engineered graphene anodes with porous, spheric, ribboned, defective and holey structures display improved capacity and rate performance owing to their highly accessible surface area, interconnected diffusion channels, and sufficient active sites. Surface-modified graphene anodes with less aggregation, fast electrons/ions transportation, and optimal solid electrolyte interphase are discussed, demonstrating the close connection between the surface structure and electrochemical activity of graphene. Second, graphene derivatives anodes prepared by heteroatom doping and covalent functionalization are outlined, which show great advantages in boosting the Li storage performances because of the additionally introduced defect/active sites for further Li accommodation. Furthermore, binder-free and free-standing graphene electrodes are presented, exhibiting great prospects for high-energy-density and flexible LIBs. Finally, the remaining challenges and future opportunities of practically available graphene anodes for advanced LIBs are highlighted., (© 2023 Wiley-VCH GmbH.)

Developing high-efficiency electrocatalysts for the hydrogen evolution and oxidation reactions (HER/HOR) in alkaline electrolytes is of critical importance for realizing renewable hydrogen technologies. Ruthenium phosphides (RuP x ) are promising candidates to substitute Pt-based electrodes; however, great challenges still remain in their electronic structure regulation for optimizing intermediate adsorption. Herein, it is reported that a homologous RuP@RuP 2 core-shell architecture constructed by a phosphatization-controlled phase-transformation strategy enables strong electron coupling for optimal intermediate adsorption by virtue of the emergent interfacial functionality. Density functional theory calculations show that the RuP core and RuP 2 shell present efficient electron transfer, leading to a close to thermoneutral hydrogen adsorption Gibbs free energy of 0.04 eV. Impressively, the resulting material exhibits superior HER/HOR activities in alkaline media, which outperform the benchmark Pt/C and are among the best reported bifunctional hydrogen electrocatalysts. The present work not only provides an efficient and cost-effective bifunctional hydrogen electrocatalyst, but also offers a new synthetic protocol to rationally synthesize homologous core-shell nanostructures for widespread applications., (© 2022 Wiley-VCH GmbH.)

Fibrous material with high strength and large stretchability is an essential component of high-performance wearable electronic devices. Wearable electronic systems require a material that is strong to ensure durability and stability, and a wide range of strain to expand their applications. However, it is still challenging to manufacture fibrous materials with simultaneously high mechanical strength and the tensile property. Herein, the ultra-robust (≈17.6 MPa) and extensible (≈700%) conducting microfibers are developed and demonstrated their applications in fabricating fibrous mechanical sensors. The mechanical sensor shows high sensitivity in detecting strains that have high strain resolution and a large detection range (from 0.0075% to 400%) simultaneously. Moreover, low frequency vibrations between 0 and 40 Hz are also detected, which covers most tremors that occur in the human body. As a further step, a wearable and smart health-monitoring system has been developed using the fibrous mechanical sensor, which is capable of monitoring health-related physiological signals, including muscle movement, body tremor, wrist pulse, respiration, gesture, and six body postures to predict and diagnose diseases, which will promote the wearable telemedicine technology., (© 2022 Wiley-VCH GmbH.)

WS 2 nanoflakes have great potential as electrode materials of lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs) because of their unique 2D structure, which facilitates the reversible intercalation and extraction of alkali metal ions. However, a fundamental understanding of the electrochemical lithiation/sodiation dynamics of WS 2 nanoflakes especially at the nanoscale level, remains elusive. Here, by combining battery electrochemical measurements, density functional theory calculations, and in situ transmission electron microscopy, the electrochemical-reaction kinetics and mechanism for both lithiation and sodiation of WS 2 nanoflakes are investigated at the atomic scale. It is found that compared to LIBs, SIBs exhibit a higher reversible sodium (Na) storage capacity and superior cyclability. For sodiation, the volume change due to ion intercalation is smaller than that in lithiation. Also, sodiated WS 2 maintains its layered structure after the intercalation process, and the reduced metal nanoparticles after conversion in sodiation are well-dispersed and aligned forming a pattern similar to the layered structure. Overall, this work shows a direct interconnection between the reaction dynamics of lithiated/sodiated WS 2 nanoflakes and their electrochemical performance, which sheds light on the rational optimization and development of advanced WS 2 -based electrodes., (© 2021 Wiley-VCH GmbH.)

Layered γ-type iron oxyhydroxide (γ-FeOOH) is a promising material for various applications; however, its sheet-shaped structure often suffers from instability that results in aggregation and leads to inferior performance. Herein, a kinetically controlled hydrolysis strategy is proposed for the scalable synthesis of γ-FeOOH nanosheets arrays (NAs) with enhanced structural stability on diverse substrates at ambient conditions. The underlying mechanisms for the growth of γ-FeOOH NAs associated with their structural evolution are systematically elucidated by alkalinity-controlled synthesis and time-dependent experiments. As a proof-of-concept application, γ-FeOOH NAs are developed as electrocatalysts for the oxygen evolution reaction (OER), where the sample grown on nickel foam (NF) exhibits superior performance of high catalytic current density, small Tafel slope, and exceptional durability, which is among the top level of FeOOH-based electrocatalysts. Density functional theory calculations suggest that γ-NiOOH in situ generated from the electrooxidation of NF would induce charge accumulation on the Fe sites of γ-FeOOH NAs, leading to enhanced OER intermediates adsorption for water splitting. This work affords a new technique to rationally design and synthesize γ-FeOOH NAs for various applications., (© 2021 Wiley-VCH GmbH.)

Li-chalcogen batteries, especially the Li-S batteries (LSBs), have received paramount interests as next generation energy storage techniques because of their high theoretical energy densities. However, the associated challenges need to be overcome prior to their commercialization. Elemental selenium, another chalcogen member, would be an attractive alternative to sulfur owing to its higher electronic conductivity, comparable capacity density, and moreover, excellent compatibility with carbonate electrolytes. Unlike LSBs, the research and development of Li-Se batteries (LSeBs) have garnered burgeoning attention but are still in their infant stage, where a comprehensive yet in-depth overview is highly imperative to guide future research. Herein, a critical review of LSeBs, in terms of the underlying mechanisms, cathode design, blocking layer engineering, and emerging solid-state electrolytes is provided. First, the electrolyte-dependent electrochemistry of LSeBs is discussed. Second, the advances in Se-based cathodes are comprehensively summarized, especially highlighting the state-of-the-art Se x S y cathodes, and mainly focusing on their structures, compositions, and synthetic strategies. Third, the versatile separators/interlayers optimization and interface regulation are outlined, with a particular focus on the emerging solid-state electrolytes for advanced LSeBs. Last, the remaining challenges and research orientations in this booming field are proposed, which are expected to motivate more insightful works., (© 2021 Wiley-VCH GmbH.)

Photodynamic therapy (PDT) and photothermal therapy (PTT) are two kinds of treatment for tumors. Herein, a new aggregation-induced emission (AIE)gen (MeO-TPE-indo, MTi) is synthesized with a D-π-A conjugated structure. MTi, which has an electron donor and an acceptor on a tetraphenylethene (TPE) conjugated skeleton, can induce the effective generation of reactive oxygen species (ROS) for PDT. With the guide of the indolium group, MTi can target and image mitochondrion selectively. In order to get good dispersion in water and long-time retention in tumors, MTi is modified on the surface of polydopamine nanoparticles (PDA NPs) to form the nanocomposite (PDA-MeO-TPE-indo, PMTi) by π-π and hydrogen interactions. PMTi is a nanoscale composite for imaging-guided PDT and PTT in tumor treatment, which is constructed with AIEgens and PDA for the first time. The organic functional molecules are combined with nanomaterials for building a multifunctional diagnosis and treatment platform by utilizing the advantages of both sides., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Sodium-ion batteries are gradually regarded as a prospective alternative to lithium-ion batteries due to the cost consideration. Here, three kinds of tin (IV) sulfide nanosheets are controllably designed with progressively exposed active facets, leading to beneficial influences on the Na + storage kinetics, resulting in gradient improvements of pseudocapacitive response and rate performance. Interestingly, different forms of kinetics results are generated accompanying with the morphology and structure evolution of the three nanosheets. Finally, detailed density functional theory simulations are also applied to analyze the above experimental achievements, proving that different exposed facets of crystalline anodes possess dissimilar Na + storage kinetics. The investigation experiences and conclusions shown in this work are meaningful to explore many other proper structure design routes toward the high-rate and stable metal-ions storage., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Herein, a surfactant- and additive-free strategy is developed for morphology-controllable synthesis of cobalt pyrophosphate (CoPPi) nanostructures by tuning the concentration and ratio of the precursor solutions of Na 4 P 2 O 7 and Co(CH 3 COO) 2 . A series of CoPPi nanostructures including nanowires, nanobelts, nanoleaves, and nanorhombuses are prepared and exhibit very promising electrocatalytic properties toward the oxygen evolution reaction (OER). Acting as both reactant and pseudo-surfactant, the existence of excess Na 4 P 2 O 7 is essential to synthesize CoPPi nanostructures for unique morphologies. Among all CoPPi nanostructures, the CoPPi nanowires catalyst renders the best catalytic performance for OER in alkaline media, achieving a low Tafel slope of 54.1 mV dec -1 , a small overpotential of 359 mV at 10 mA cm -2 , and superior stability. The electrocatalytic activities of CoPPi nanowires outperform the most reported non-noble metal based catalysts, even better than the benchmark Ir/C (20%) catalyst. The reported synthesis of CoPPi gives guidance for morphology control of transition metal pyrophosphate based nanostructures for a high-performance inexpensive material to replace the noble metal-based OER catalysts., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Transition-metal disulfide with its layered structure is regarded as a kind of promising host material for sodium insertion, and intensely investigated for sodium-ion batteries. In this work, a simple solvothermal method to synthesize a series of MoS 2 nanosheets@nitrogen-doped graphene composites is developed. This newly designed recipe of raw materials and solvents leads the success of tuning size, number of layers, and interplanar spacing of the as-prepared MoS 2 nanosheets. Under cut-off voltage and based on an intercalation mechanism, the ultrasmall MoS 2 nanosheets@nitrogen-doped graphene composite exhibits more preferable cycling and rate performance compared to few-/dozens-layered MoS 2 nanosheets@nitrogen-doped graphene, as well as many other reported insertion-type anode materials. Last, detailed kinetics analysis and density functional theory calculation are also employed to explain the Na + - storage behavior, thus proving the significance in surface-controlled pseudocapacitance contribution at the high rate. Furthermore, this work offers some meaningful preparation and investigation experiences for designing electrode materials for commercial sodium-ion batteries with favorable performance., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Glycosides are a kind of highly important natural aromatic precursors in tobacco leaves. In this study, a novel HKUST-1-coated monolith dip-it sampler was designed for the fast and sensitive analysis of trace glycosides using direct analysis in real-time mass spectrometry. This device was prepared in two steps: in situ polymerization of monolith in a glass capillary of dip-it and layer-by-layer growth of HKUST-1 on the surface of monolith. Sufficient extraction was realized by immersing the tip to solution and in situ desorption was carried out by plasma direct analysis in real time. Compared with traditional solid-phase microextraction protocols, sample desorption was not needed anymore, and only extraction conditions were needed to be optimized in this method, including the gas temperature of direct analysis in real time, extraction time, and CH 3 COONH 4 additive concentration. This method enabled the simultaneous detection of six kinds of glycosides with the limits of detection of 0.02-0.05 μg/mL and the linear ranges covering two orders of magnitude with the limits of quantitation of 0.05-0.1 μg/mL. Moreover, the developed method was applied for the glycosides analysis of three tobacco samples, which only took about 2 s for every sample., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Hierarchically porous carbons are attracting tremendous attention in sustainable energy systems, such as lithium ion battery (LIB) and fuel cell, due to their excellent transport properties that arise from the high surface area and rich porosity. The state-of-the-art approaches for synthesizing hierarchically porous carbons normally require chemical- and/or template-assisted activation techniques, which is complicate, time consuming, and not feasible for large scale production. Here, a molecular-level design principle toward large-scale synthesis of nitrogen and phosphorus codoped hierarchically porous carbon (NPHPC) through an in situ self-activation process is proposed. The material is fabricated based on the direct pyrolysis of a well-designed polymer, melamine polyphosphate, which is capable of in situ self-activation to generate large specific surface area (1479 m 2 g -1 ) and hierarchical pores in the final NPHPC. As an anode material for LIB, NPHPC delivers a high reversible capacity of 1073 mAh g -1 and an excellent cyclic stability for 300 cycles with negligible capacity decay. The peculiar structural properties and synergistic effect of N and P codopants also enable NPHPC a promising electrocatalyst for oxygen reduction reaction, a key cathodic reaction process of many energy conversion devices (for example, fuel cells and metal air batteries). Electrochemical measurements show NPHPC a comparable electrocatalytic performance to commercial Pt/C catalyst (onset potential of 0.88 V vs reversible hydrogen electrode in alkaline medium) with excellent stability (89.8% retention after 20 000 s continuous operation) and superior methanol tolerance., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Pi-extended polyaromatics tend to exhibit improved electronic properties with respect to the intrinsic structures. Herein, the rational design of a π-extended diindole-fused diazapentacenone (IP), with a nine-ring-fused core, obtained by applying an intramolecular Friedel-Crafts diacylation synthetic routine, is reported. The chemical structure, physical properties, and morphology of IP were fully characterized. Serving as an organic cathode material for a lithium-ion battery, the as-prepared nanorods of π-extended IP display higher conductivity and superior electrochemical performance than those of the naked diazapentacenone without diindole fusion., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

An unprecedented rhodium(III)-catalyzed regioselective redox-neutral annulation reaction of 1-naphthylamine N-oxides with diazo compounds was developed to afford various biologically important 1H-benzo[g]indolines. This coupling reaction proceeds under mild reaction conditions and does not require external oxidants. The only by-products are dinitrogen and water. More significantly, this reaction represents the first example of dual functiaonalization of unactivated a primary C(sp(3) )H bond and C(sp(2) )H bond with diazocarbonyl compounds. DFT calculations revealed that an intermediate iminium is most likely involved in the catalytic cycle. Moreover, a rhodium(III)-catalyzed coupling of readily available tertiary aniline N-oxides with α-diazomalonates was also developed under external oxidant-free conditions to access various aminomandelic acid derivatives by an O-atom-transfer reaction., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A Rh(III)-catalyzed procedure for the C7-selective C-H alkylation of various indolines with α-diazo compounds at room temperature is reported. The advantages of this process are: 1) simple, mild, and pH-neutral reaction conditions, 2) broad substrate scope, 3) complete regioselectivity, 4) no need for an external oxidant, and 5) N2 as the sole byproduct. Furthermore, alkylation and bis-alkylation of carbazoles at the C1 and C8 positions have also been developed. More significantly, for the first time, a successful Ir(III)-catalyzed intermolecular insertion of arene C-H bonds into α-diazo compounds is reported., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

N and S codoping of graphene is realized by a novel approach: covalent functionalization of graphene oxide using 2-aminothiophenol as a source of both N and S followed by thermal treatment. The resulting N- and S-codoped graphene has potential applications in high-performance lithium-ion batteries and as a metal-free catalyst for oxygen reduction reaction., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)