Jun Lu's research while affiliated with Hangzhou University and other places
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Publications (741)
To meet the ever‐increasing demand for high‐energy lithium‐ion batteries (LIBs), it is imperative to develop next‐generation anode materials. Compared to conventional carbon‐based anodes, Si‐based materials are promising due to their high theoretical capacity and reasonable cost. SiOx, as a Si‐derivative anode candidate, is particularly encouraging...
Solid‐state electrolytes (SSE) exhibit great promise in enhancing the safety of Li metal batteries by replacing flammable liquid electrolytes. However, the practical application of SSE is hampered mainly due to the poor electrode–electrolyte interface, low ion conductivity, and inferior electrochemical stability. Herein, superior nonflammable solid...
Nickel‐rich layered oxide cathode material LiNi x Co y Mn z O 2 (NCM) has emerged as a promising candidate for next‐generation lithium‐ion batteries (LIBs). These cathode materials possess high theoretical specific capacity, fast electron/ion transfer rate, and high output voltage. However, their potential has been impeded by interface instability,...
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Clarifying the formation mechanism of single‐atom sites guides the design of emerging single‐atom catalysts (SACs) and facilitates the identification of the active sites at atomic scale. Herein, a molten‐salt atomization strategy is developed for synthesizing zinc (Zn) SACs with temperature universality from 400 to 1000/1100 °C and an evolved coord...
Rechargeable aqueous zinc-ion batteries (AZIBs), renowned for their safety, high energy density and rapid charging, are prime choices for grid-scale energy storage. Historically, ion-shuttling models centring on ion-migration behaviour have dominated explanations for charge/discharge processes in aqueous batteries, like classical ion insertion/extr...
The limited visible light response is a critical drawback that hampers the photocatalytic efficacy of Ti‐MOFs. However, study concerning the enhancement of the visible‐light response of Ti‐MOFs is still in its nascent stage. In this study, we employ the ‘dual‐ligand decrystallization strategy’ to manipulate the electronic environment of Ti4+, leadi...
The sluggish kinetics of lithium‐sulfur (Li‐S) batteries severely impedes the application in extreme conditions. Bridging the electrodes, the electrolyte plays a crucial role in regulating kinetic behaviors of Li‐S batteries. Herein, we report a multifunctional electrolyte additive of phenyl selenium bromide (PhSeBr) to simultaneously exert positiv...
The sluggish kinetics of lithium‐sulfur (Li‐S) batteries severely impedes the application in extreme conditions. Bridging the electrodes, the electrolyte plays a crucial role in regulating kinetic behaviors of Li‐S batteries. Herein, we report a multifunctional electrolyte additive of phenyl selenium bromide (PhSeBr) to simultaneously exert positiv...
Cathode materials of sodium‐based batteries with high specific capacity and fast charge–discharge mode, as well as ultralong reversible cycles at wide applied temperatures, are essential for future development of advanced energy storage system. Developing transition metal selenides with intercalation features provides a new strategy for realizing t...
Sodium‐ion batteries (SIBs) have emerged as a compelling alternative to lithium‐ion batteries (LIBs), exhibiting comparable electrochemical performance while capitalizing on the abundant availability of sodium resources. In SIBs, P2/O3 biphasic cathodes, despite their high energy, require furthur improvements in stability to meet current energy dem...
The conversion of CO2 into formate through electrochemical methods is emerging as an elegant approach for industrial‐scale CO2 utilization in the near future. Although Bismuth (Bi)‐based materials have shown promise thank to their excellent selectivity, their limited reactivity remains a challenge. Herein, this study demonstrates a significant enha...
Waste tyres (WTs) are a major global issue that needs immediate attention to ensure a sustainable environment. They are often dumped in landfills or incinerated in open environments, which leads to environmental pollution. However, various thermochemical conversion methods have shown promising results as treatment routes to tackle the WT problem wh...
Effective thermal safety management relies on the thermal conductivity of interlayer materials, yet current designs lack the needed responsiveness for both performance and safety. Here we design a thermal-switching material with high switching ratio from thermal conduction to thermal insulation state to address this predicament. The designed therma...
Global efforts to tackle climate change and the rise in popularity of electric vehicles and portable electronic devices have engendered a demand explosion for lithium-ion batteries (LIBs). Effectuated by the green and digital revolution, this exponential rise in the demand for LIBs raises a host of logistical and environmental concerns centered aro...
Lithium–sulfur (Li–S) battery is identified as an ideal candidate for next‐generation energy storage systems in consideration of its high theoretical energy density and abundant sulfur resources. However, the shuttling behavior of soluble polysulfides (LiPSs) and their sluggish reaction kinetics severely limit the practical application of the curre...
Lithium metal shows a great advantage as the most promising anode for its unparalleled theoretical specific capacity and extremely low electrochemical potential. However, uncontrolled lithium dendrite growth and severe side reactions of the reactive intermediates and organic electrolytes still limit the broad application of lithium metal batteries....
In spite of the competitive performance at room temperature, the development of sodium‐ion batteries (SIBs) is still hindered by sluggish electrochemical reaction kinetics and unstable electrode/electrolyte interphase under subzero environments. Herein, a low‐concentration electrolyte, consisting of 0.5M NaPF 6 dissolving in diethylene glycol dimet...
In spite of the competitive performance at room temperature, the development of sodium‐ion batteries (SIBs) is still hindered by sluggish electrochemical reaction kinetics and unstable electrode/electrolyte interphase under subzero environments. Herein, a low‐concentration electrolyte, consisting of 0.5M NaPF6 dissolving in diethylene glycol dimeth...
Zinc metal is an attractive anode material for rechargeable aqueous Zn‐ion batteries (ZIBs). However, the dendrite growth, water‐induced parasitic reactions, and freezing problem of aqueous electrolyte at low temperatures are the major roadblocks that hinder the widely commercialization of ZIBs. Herein, tetrahydrofuran (THF) is proposed as the elec...
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The cost‐effectiveness and environmentally friendly nature of aqueous zinc‐ion batteries (ZIBs) have garnered significant attention. Nevertheless, obstacles such as dendrite growth and side reactions have hindered their practical application. Here, an alkaline earth metal ion, strontium ions (Sr²⁺), is chosen as a dual‐functional electrolyte additi...
The plastic waste issue has posed a series of formidable challenges for the ecological environment and human health. While conventional recycling strategies often lead to plastic down‐cycling, the electrochemical strategy of recovering valuable monomers enables an ideal, circular plastic economy. Here a corrosion synthesized single atom Pt1/Ni(OH)2...
All‐solid–state lithium metal batteries (LMBs) are currently one of the best candidates for realizing the yearning high‐energy–density batteries with high safety. However, even polyethylene oxide (PEO), the most popular polymeric solid‐state electrolyte (SSE) with the largest ionic conductivity in the category so far, has significant challenges due...
Rechargeable lithium‐oxygen (Li‐O2) batteries with high theoretical energy density are regarded as a promising candidate for the booming electric vehicle manufacturing industry, whereas their commercial application is hindered due to poor cyclic stability caused by the sluggish kinetics and inevitable cathode passivation. Herein, a synergistic work...
Lithium- and manganese-rich layered oxide cathode materials have attracted extensive interest because of their high energy density. However, the rapid capacity fading and serve voltage decay over cycling make the waste management and recycling of key components indispensable. Herein, we report a facile concentrated solar radiation strategy for the...
Nickel‐rich layered oxides are a class of promising cathodes for high‐energy‐density lithium‐ion batteries (LIBs). However, their structural instability derived from crystallographic planar gliding and microcracking under high voltages has significantly hindered their practical applications. Herein, resurfacing engineering for single‐crystalline Li...
Water‐based secondary batteries with multivalent metals anode provide a promising option for energy storage with low cost and high security. However, the electrochemical performance of aqueous Zinc ion batteries (AZIBs) is mainly restricted by problems such as poor reversibility and hydrogen evolution. Herein, an “amphoteric polymer strategy” with...
Sodium-ion batteries have not only garnered substantial attention for grid-scale energy storage owing to the higher abundance of sodium compared with lithium, but also present the possibility of fast charging because of the inherently higher sodium-ion mobility. However, it remains a phenomenal challenge to achieve a combination of these merits, gi...
Calcium–oxygen (Ca–O2) batteries can theoretically afford high capacity by the reduction of O2 to calcium oxide compounds (CaOx) at low cost1–5. Yet, a rechargeable Ca–O2 battery that operates at room temperature has not been achieved because the CaOx/O2 chemistry typically involves inert discharge products and few electrolytes can accommodate both...
Fe‐based Prussian blue (Fe‐PB) cathode material shows great application potential in sodium (Na)‐ion batteries due to its high theoretical capacity, long cycle life, low cost, and simple preparation process. However, the crystalline water and vacancies of Fe‐PB lattice, the low electrical conductivity, and the dissolution of metal ions lead to limi...
Polyanionic sodium ion cathodes have attracted lots of concern because of their excellent structural stability. However, the low specific capacity is still a pressing issue hampering their practical application. In this work, a medium‐entropy NASICON‐structure cathode Na3.5V0.5Mn0.5Fe0.5Ti0.5(PO4)3 (Me‐NVMP) is proposed. The Me‐NVMP achieves a high...
High electrochemical reversibility is required for the application of high-energy-density lithium (Li) metal batteries; however, inactive Li formation and SEI (solid electrolyte interface)-instability-induced electrolyte consumption cause low Coulombic efficiency (CE). The prior interfacial chemical designs in terms of alloying kinetics have been u...
![a) The mosaic model of SEI films. Reproduced with permission.[¹⁵]...](publication/377626578/figure/fig3/AS:11431281251518552@1718246503273/a-The-mosaic-model-of-SEI-films-Reproduced-with-permission-Copyright-2018_Q320.jpg)
Lithium (Li) metal has emerged as a viable alternative anode material to address the current energy density shortfalls in Li batteries. However, its integration into widespread implementation remains somewhat constrained due to the substandard reversibility issues and safety concerns arising from erratic Li deposition. To effectively tackle these o...
Scandium oxide (Sc2O3) is considered as omnipotent “Industrial Ajinomoto” and holds promise in catalytic applications. However, rarely little attention is paid to its electrochemistry. Here, the first nanocasting design of high‐surface area Sc2O3 with abundant oxygen vacancies (mesoporous VO‐Sc2O3) for efficient electrochemical biomass valorization...
Lithium‐sulfur batteries utilizing sulfide solid electrolytes hold considerable potential for achieving both high energy density and enhanced safety. However, the substantial volume changes experienced by sulfur during cycling result in mechanical stress accumulation, leading to mechanical degradation and thereby degrading overall electrochemical p...
Zn metal, as one of the most promising anode materials for aqueous batteries, suffers from uncontrollable dendrite growth and water‐induced parasitic reactions, which drastically compromise its cycle life and Coulombic efficiency (CE). Herein, a nonionic amphipathic additive Tween‐20 (TW20) is proposed that bears both zincophilic and hydrophobic un...
A unique Li ⁺ -crosslinked ionic conductive elastomer (ICE) was developed and the resultant ICE-SEI demonstrates remarkable elasticity, self-healing capability, and high ionic conductivity, thus realizing long-life Li metal batteries.
Facing high overpotential, severe Li corrosion and degradation of electrolytes caused by the reactive oxygen species, the development of lithium–oxygen batteries is seriously limited. Although the iodine species have been considered to be effective redox mediators (RMs) for lowering the charging overpotential, the shuttling of oxidized I3⁻ may atta...
Tunnel‐structured manganese dioxides (MnO2), also known as octahedral molecule sieves (OMS), are widely studied in geochemistry, deionization, energy storage and (electro)catalysis. These functionalities originate from their characteristic sub‐nanoscale tunnel framework, which, with a high degree of structural polymorphism and rich surface chemistr...
The reaction rate bottleneck during interconversion between insulating S8 (S) and Li2S fundamentally leads to incomplete conversion and restricted lifespan of Li−S battery, especially under high S loading and lean electrolyte conditions. Herein, we demonstrate a new catalytic chemistry: soluble semiquinone, 2‐tertbutyl‐semianthraquinone lithium (Li...
Electrolytes with high stability against both Li anode and high‐voltage cathode are critical for high‐energy and long‐cycling lithium metal batteries (LMBs). However, the free active solvents in common electrolytes are susceptible to decomposition at both Li anode and high‐voltage cathode. Although recently developed locally high‐concentration elec...
Suppressing dendrite growth in zinc (Zn) anodes for aqueous Zn batteries remains a significant challenge. Modifying the Zn/electrolyte interface stands out as one of the most promising strategies to tackle this problem. In this study, a nanometer‐thick ZnO coating layer with a uniform concave surface geometry is in situ constructed to modify the Zn...
Tunnel‐structured manganese dioxides (MnO2), also known as octahedral molecule sieves (OMS), are widely studied in fields of geochemistry, deionization, energy storage and (electro)catalysis. These functionalities originate from their characteristic sub‐nanoscale (Å‐scale) tunnel framework, which, with a high degree of structural polymorphism and r...
The reaction rate bottleneck during interconverson between insulating S8 (S) and Li2S fundamentally leads to incomplete conversion and restricts lifespan of Li‐S battery, especially under high S loading and lean electrolyte conditions. Herein, we demonstrate a new catalytic chemistry: soluble semiquinone, 2‐tertbutyl‐semianthraquinone lithium (Li+T...
The interfacial compatibility between cathode materials and sulfide solid‐electrolytes (SEs) is a critical limiting factor of electrochemical performance in all‐solid‐state lithium‐ion batteries (ASSLBs). In response to this challenge, this work presents a novel approach: the development of a gas‐solid interface reduction reaction (GSIRR). This GSI...
The long‐term reversible plating/stripping of Zn metal anode is a critical aspect within aqueous zinc‐ion batteries (ZIBs). However, it is limited by uncontrolled electrodeposition and side reactions occurring at the anode/electrolyte interface. Guided by the metal‐coordination chemistry, a novel additive, sodium diphenylamine sulfonate (DASS), is...
The thriving field of atomic defect engineering towards advanced electrocatalysis relies on the critical role of electric field polarization at the atomic scale. While this is proposed theoretically, the spatial configuration, orientation, and correlation with specific catalytic properties of materials are yet to be understood. Here, by targeting m...
Rechargeable batteries are widely used as power sources for portable electronics, electric vehicles and smart grids. Their practical performances are, however, largely undermined under extreme conditions, such as in high‐altitude drones, ocean exploration and polar expedition. These extreme environmental conditions not only bring new challenges for...
Energy storage via anionic redox provides extra capacity for lithium-rich manganese-based oxide cathodes at high voltage but causes gradual structural collapse and irreversible capacity loss with generation of On- (0≤n<2) species upon deep oxidation. Herein, the stability and reversibility of anionic redox reactions are enhanced by a simple sulfur-...
Despite the high energy of LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode, it still suffers serious decay due to the continuous solvents decomposition and unstable cathode electrolyte interphase (CEI) layers, especially under high temperatures. The intense exothermic reaction between delithiated NCM811 and flammable organic solvents, on the other hand, pushe...
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Quasi‐solid‐state lithium metal batteries (QSSLMBs) necessitate stable electro‐electrolyte interfaces to ensure reliable stationary power supply, thereby placing significant emphasis on the development of polymer electrolytes with high and uniform conductivity. However, while preparing the polymer electrolytes, the uncontrolled radical polymerizati...
![a) Schematic of adhesion process. Reproduced with permission.[²²]...](publication/375041994/figure/fig2/AS:11431281222326520@1707199351191/a-Schematic-of-adhesion-process-Reproduced-with-permission-Copyright-2018_Q320.jpg)
![Timeline of the development of binders for RSBs.[27,36] CMCNa....](publication/375041994/figure/fig3/AS:11431281222344933@1707199351378/Timeline-of-the-development-of-binders-for-RSBs27-36-CMCNa-Reproduced-with_Q320.jpg)
Supply restrictions and associated price increase of lithium limit the large‐scale application of rechargeable lithium batteries (RLBs) in electric energy storage. Rechargeable sodium batteries (RSBs) with the advantage of large abundance and low cost of sodium, are developed to relieve the supply pressure of RLBs. Binders serve as a bridge between...
Aqueous rechargeable Zn batteries incorporating MnO 2 cathodes possess favourable sustainability properties and are being considered for low‐cost, high‐safety energy storage. However, unstable electrode structures and unclear charge storage mechanisms limit their development. Here, we utilize advanced transmission electron microscopy, electrochemic...
Electrochemical oxygen evolution reaction (OER) kinetics are heavily correlated with hybridization of the transition metal d ‐orbital and oxygen intermediate p ‐orbital, which dictates the barriers of intermediate adsorption/desorption on the active sites of catalysts. Herein, w e develop a strategy involving strain engineering and coordination reg...
The low cost and intrinsic safety of rechargeable aqueous zinc‐ion batteries (ZIBs) contribute to their significant potential in grid‐level energy storage systems. However, the limited cathode options still hinder the development of ZIBs, which always delivers poor rate capacities and cycling stability. Herein, Monoclinic phase H3.78V6O13 microsphe...
Poly (ethylene oxide) (PEO)‐based electrolytes are extensively applied to LiFePO4/Li solid‐state batteries on account of their high safety and good flexibility. Nevertheless, the unsatisfactory energy density and inferior lifespan of the batteries still inhibit their large‐scale applications. Herein, graphitic carbon nitride nanosheets (GCN)‐assist...
Lithium–sulfur (Li–S) batteries are considered as one of the top competitors to go beyond Li‐ion batteries. However, the shuttle effect triggered by soluble lithium polysulfides (LPSs) brings great troubles for understanding the solid–liquid–solid conversion process of the sulfur cathode. Herein, a new characterization technique is developed to dee...
Although biomass‐derived carbon (biochar) has been widely used in the energy field, the relation between the carbonization condition and the physical/chemical property of the product remains elusive. Here, we revealed the carbonization condition's effect on the morphology, surface property, and electrochemical performance of the obtained carbon. An...
Layered Li-rich transition metal oxides (LR TM O) are one of the most promising cathode candidates for high energy density lithium batteries due to the redox contributions from transition metal ( TM ) cations and oxygen (O) anion. However, their practical application is hindered by gradual capacity fading and voltage decay. Although oxygen loss and...
Bi-based materials are one of the most promising candidates for electrochemical CO2 reduction to formate, however, the majority of them still suffer from low current density and stability that essentially constrain their potential applications at the industrial scale. Surface modification represents an effective approach to modulate the electrode m...
Heterogeneous oxides with multiple interfaces provide significant advantages in electrocatalytic activity and stability. However, controlling the local structure of these oxides is challenging. In this work, unique heterojunctions are demonstrated based on two oxide types, which are formed via pyrolysis of a ruthenocene metal–organic framework (Ru‐...
Using ethanol electrocatalytic oxidation reaction (EOR) with a lower reaction potential to replace oxygen evolution reaction (OER) and integrating hydrogen evolution reaction (HER) have a promising development prospect for more energy‐saving electrolytic hydrogen production. However, the main challenges of EOR are insufficient catalytic activity, h...
Silicon oxide (SiOx) is a promising anode candidate of lithium‐ion batteries (LIBs) owing to its extremely high specific capacity. However, the low initial Coulombic efficiency (ICE) and rapid capacity degradation of SiOx, triggered by the enormous volume variation upon repeated (de)lithiation, gravely hinder its practical use. Herein, two mass‐pro...
Atomically dispersed iron–nitrogen–carbon (FeNC) catalysts have sparked great interest by virtue of the highly active isolated FeN4 sites. The catalysts with pyrolysis treatment usually induce inevitable FeN4 sites agglomeration, leading to fast degradation in catalytic activity. Herein, a pre‐coordinated protection strategy is proposed to eliminat...
Redox flow batteries have been discussed as scalable and simple stationary energy storage devices. However, currently developed systems encounter less competitive energy density and high costs, restricting their wider application. There is a lack of appropriate redox chemistry, preferably based on active materials that are abundant in nature and sh...
Electrochemical conversion of nitrate to ammonia offers an efficient approach to reducing nitrate pollutants and a potential technology for low-temperature and low-pressure ammonia synthesis. However, the process is limited by multiple competing reactions and NO3⁻ adsorption on cathode surfaces. Here, we report a Fe/Cu diatomic catalyst on holey ni...
Rechargeable magnesium batteries (RMBs) are promising next‐generation low‐cost and high‐energy devices. Among all RMBs, anode‐free magnesium metal batteries that use in situ magnesium‐plated current collectors as negative electrodes can afford optimal energy densities. However, anode‐free magnesium metal batteries have remained elusive so far, as t...
Redox flow batteries have been discussed as scalable and simple stationary energy storage devices. However, currently developed systems encounter less competitive energy density and high costs, restricting their wider application. There is a lack of appropriate redox chemistry, preferably based on active materials that are abundant in nature and sh...
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Salt precipitation at temperatures far above the freezing point of solvents is primarily responsible for performance decay of rechargeable batteries at low temperature, yet is still challenged by a lack of in-depth understanding of the design principle and ultimate solutions. Here, we resolve this via tuning the entropy of solvation in a strong-sol...
Abstract Sodium (Na) ion batteries (SIBs) promise low‐cost energy storage systems but are still restricted by insufficient energy density. Introducing oxygen (O) redox into the design of the Na‐storage cathode is presently considered an effective avenue to generate extra capacity in solving the energy density bottleneck. The succeeding issues are h...
Co‐free high‐Ni layered transition metal oxide is a promising cost‐effective cathode material for high‐energy Li‐ion batteries, but it suffers from undesirable rate performance and rapid capacity decay upon high‐rate cycling. The underlying structural changes under fast electrochemical processes remain unclear to date. In this study, atomic scale s...
The practical viability of high energy density lithium-sulfur (Li-S) batteries stipulates the use of a high-loading cathode and lean electrolyte. However, under such harsh conditions, the liquid-solid sulfur redox reaction is much-retarded due to the poor sulfur and polysulfides utilization, leading to low capacity and fast fading. Herein, a self-a...
Structural modulation of graphitic carbon nitride (g‐C3N4) remains a major challenge in rational catalyst design for artificial photosynthesis of valuable chemicals. Herein, a cellulose nanofiber (CNF) assisted polymerization is utilized to prepare 1D holey g‐C3N4 nanorods (HCN) with nitrogen vacancies and oxygen dopants for photochemical synthesis...
Maintaining a steady affinity between gallium-based liquid metals (LM) and polymer binders, particularly under continuous mechanical deformation, such as extrusion-based 3D printing or Zn2+ plating/stripping, is very challenging. Here, a LM-initialized polyacrylamide-hemicellulose/EGaIn microdroplets hydrogel is used as a multifunctional ink to 3D-...
Catalysts with FeNC moieties have demonstrated remarkable activity toward oxygen reduction reaction (ORR), but precise synthesis and configuration regulation of FeNC to achieve bi‐functional catalytic sites for ORR and oxygen evolution reaction (OER) remain a great challenge. Herein, a pomegranate‐like catalyst with optimized FeN4 configuration is...
Non‐equilibrium kinetic intermediates are usually preferentially generated instead of thermodynamic stable phases in the solid‐state synthesis of layered oxides. Understanding the inherent complexity between thermodynamics and kinetics is important for designing high cationic ordering cathodes. Single‐crystal strategy is an effective way to solve t...
Considerable efforts have been devoted to Li-S batteries, typically the soluble polysulfides shuttling effect. As a typical transition metal sulfide, MoS2 is a magic bullet for addressing the issues of Li-S batteries, drawing increasing attention. In this study, we introduce amorphous MoS3 as analogous sulfur cathode material and elucidate the dyna...
We report a facile in‐situ etching method for the synthesis of defective CuBTC (H‐CuBTC) with hierarchical pore structure. The fabricated mixed matrix membranes (MMMs) containing H‐CuBTC was prepared for the separation of CO2/CH4, showing superior separation performance due to the defective structure with larger pore size and more open Cu sites, wh...
Lithium-sulfur batteries with liquid electrolytes have been obstructed by severe shuttle effects and intrinsic safety concerns. Introducing inorganic solid-state electrolytes into lithium-sulfur systems is believed as an effective approach to eliminate these issues without sacrificing the high-energy density, which determines sulfide-based all-soli...
Hierarchical assembly of polysaccharides into nanofiber is at the core of generating advanced biomimetic nano materials. However, the artificial synthesis of supramolecular nanofiber from polysaccharides remains an open challenge due to their complicated structure, irregular and strong interaction. Herein, by mimicking the assembly of natural macro...
The shortage of fresh water in the world has brought upon a serious crisis to human health and economic development. Solar‐driven interfacial photothermal conversion water evaporation including evaporating seawater, lake water, or river water has been recognized as an environmentally friendly process for obtaining clean water in a low‐cost way. How...
SiOx anode with higher specific capacity than graphite and better capacity retention than pure Si has received great attention from both academia and the industry. However, the further application of SiOx suffers from its low initial Coulombic efficiency and inadequate capacity retention. The academia has reported numerous strategies to overcome th...
Developing liquid electrolytes with higher kinetics and enhanced interphase stability is one of the key challenges for lithium batteries. However, the poor solubility of lithium salts in solvents sets constraints that compromises the electrolyte properties. Here we show that introducing multiple salts to form a high‐entropy solution, alters the sol...
Polymeric binders stabilize lithium–sulfur (Li–S) batteries by suppressing the shuttle of lithium polysulfide (LiPS) and volume variation, but the dosage of state‐of‐the‐art binders in sulfur cathodes (≈20 wt%) hinders the electron/ion transfer and decreases the cell‐specific density. Here, a wood‐inspired lignin binder is developed after modificat...
Non‐equilibrium kinetic intermediates are usually preferentially generated instead of thermodynamic stable phases in the solid‐state synthesis of layered oxides. Understanding the inherent complexity between thermodynamics and kinetics is important for designing high cationic ordering cathodes. Single‐crystal strategy is an effective way to solve t...
Due to recent developments in secondary ion batteries for high‐energy‐density applications, a thorough understanding of the underlying mechanism of advanced cathode materials is of vital importance. In situ transmission electron microscopy (TEM) techniques capable of high spatial and temporal resolution in operando analysis of dynamic battery syste...
The Ni‐rich layered oxide cathode is pushing the frontier of battery powered electric vehicles toward longer driving range and lower cost, whilst facing a major challenge with the compromised cycle life and thermal robustness. It is well recognized that irreversible oxygen evolution at the cathode‐electrolyte interphase is critical to the electroch...
Single‐atom catalysts (SACs) show great potential for rechargeable Zn–air batteries (ZABs); however, scalable production of SACs from sustainable resources is difficult owing to poor control of the local coordination environment. Herein, lignosulfonate, a by‐product of the papermaking industry, is utilized as a multifunctional bioligand for the mas...
The electrochemical stability window of the electrolyte solution limits the energy content of non-aqueous lithium metal batteries. In particular, although electrolytes comprising fluorinated solvents show good oxidation stability against high-voltage positive electrode active materials such as LiNi0.8Co0.1Mn0.1O2 (NCM811), the ionic conductivity is...
Citations
... [11,12] As for the inner inorganic SEI, it possesses the merits of optimal interfacial energy and superior ionic conductivity, which can accelerate the lateral diffusion of Li + along the SEI/Li interphase, and effectively form a uniform ionic flux for homogeneous deposition of Li, thus inhibiting the formation of dendrite and improving the stability of electrode structure. [13,14] Up to date, several conventional strategies, such as anion-rich additives, [15,16] atomic layer deposition method (ALD), [17,18] soaking method, [19,20] spray quenching method, [21] and sputtering approach, [22] are adopted to prepare inorganic SEI or inorganic-rich SEI layers. For instance, Yao et al. reported a lithium bromide-enriched SEI on the lithium anode by a chemical passivation dip-coating method. ...
... This decline in CE can be ascribed to the presence of insulating by-products and zinc dendrites, leading to compromised electron transfer and "dead Zn". [57][58][59] Comparably, the incorporation of the ZWO@Zn anode introduces a noteworthy reduction in electrode polarization, which is stemmed from a lowered energy barrier and accelerated Zn 2 + transfer rate, thus ensuring a consistent and stable cycling process with excellent reversibility. Moreover, the ZWO@Zn//Ti battery displays a substantial decrease in voltage hysteresis, maintaining a consistently stable value of around 28 mV (Figure 3i). ...
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... Reproduced with permission. [22] Copyright 2024, Wiley-VCH. ...
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... Compared with the original NCA material, the peak shape of NCA@2wt%WO 3 material is relatively sharp, indicating that the material at this time has high activity. Note that the voltage difference (ΔV) of the redox potential reflects the degree of polarization and the reversibility of Li + insertion/extraction during charging/discharging [42]. The higher the capacity retention, the narrower the voltage difference ΔV [43]. ...
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... By contrast, ions with electronic configurations d 0 (for example, V 5+ and Cr 6+ ) and d 5 in high spin (for example, Fe 3+ and Mn 2+ ) are prone to migration across the tetrahedral site 35 . However, some ions, for example, Ti 4+ can stabilize octahedral structures 37,38 , which can thus be used to form CSRD oxides. This is realized in the presently designed CSRD LiTi 1/2 Mg 1/2 O 2 -LiNi 0.8 Co 0.1 Mn 0.1 O 2 , also considering that LiTi 1/2 Mg 1/2 O 2 crystallizes in the disordered rock-salt structure. ...
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... To accurately describe the interactions among the intermediates and active sites, the DFT-D3 dispersed corrections proposed by Grimme et al. were involved in evaluating their adsorbed-free energies. 50 Considering the practical electrochemical reaction surroundings, the solvation effect was drawn into the adsorbed free energy of intermediates using a polarized continuum model ~ VASP sol. The electronic kinetic cutoff with the plane wave basis set was 400 eV and the corresponding convergence criteria of total energy and residual force per atom were less than 10 − 4 eV and 0.02 eV/Å, respectively. ...
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... V vs Na + /Na) at 0.1 C (1 C = 171 mA g −1 ) via the stepwise redox reactions of Ti 3+ /Ti 4+ -Fe 2+ /Fe 3+ , V 3+ /V 4+ -Mn 2+ /Mn 3+ , and V 4+ /V 5+ -Mn 3+ /Mn 4+ . [39] Figure 6a presents the room temperature Nyquist plot of the NVMP/NZSP/Na battery, with the inset illustrating the structure of solid-state sodium metal batteries and the equivalent circuit diagram. The resistance of the battery is mainly composed of electrolyte resistance and interfacial resistance between solid electrodes and ceramic electrolyte. ...
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... The unsaturated Ce−O coordination in Y,Co-CeO 2 indicates an increase of oxygen vacancy sites. [38] In addition, the coordination structure of the Ce species in Y,Co-CeO 2 and CeO 2 is further investigated by wavelet transform-EXAFS (WT-EXAFS) with high resolution in both k and R spaces. As shown in Figure 4e,f, the WT contour maps further verify the existence of Ce−O in Y,Co-CeO 2 and CeO 2 , showing the decrease in the coordination length of the Ce─O bond in Y,Co-CeO 2 . ...
... Dendrite growth is partly suppressed in LHCE, but it is still evident on Na surface with obvious bubbles, demonstrating its poor compatibility with Na accompanied by the occurrence of side reactions. [15] In sharp contrast, no dendrite and no bubbles are found in DPSE within 50 min. The above analyses of Na j j Cu and Na j j Na cells demonstrate the superiority of DPSE in terms of compatibility, stability, and reversibility. ...
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... However, the adsorbed Zn 2+ ions onto the ND surface had a smoother diffusion path and uniform distribution, eventually suppressing dendrite formation. [15,21] The diffusion energy barriers of Zn on the ND surfaces, Zn and Cu surface with lowest value, and other reported artificial coatings or solid electrolyte interfaces (SEI) for Zn anode protection, including ZnO, [22] Sn, [23] ZnCO 3 , [24] Zn 3 (PO 4 ) 2 , [25] TiO 2 , [26] and ZnF 2 , [27] were compared in Figure 2i and Figure S13, Supporting Information. It was evident that ND showed considerably lower overall energy barriers among all these materials, demonstrating its significant role in achieving the dendrite-free Zn anode. ...
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