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Poor fast-charge capabilities limit the usage of rechargeable Li metal anodes. Understanding the connection between charging rate, electroplating mechanism, and Li morphology could enable fast-charging solutions. Here, we develop a combined electroanalytical and nanoscale characterization approach to resolve the current-dependent regimes of Li plating mechanisms and morphology. Measurement of Li

Designing materials with ultralow thermal conductivity has broad technological impact, from thermal protection to energy harvesting. Low thermal conductivity is commonly observed in anharmonic and strongly disordered materials, yet a microscopic understanding of the correlation to atomic motion is often lacking. Here we report that molecular insertion into an existing two-dimensional layered lattice structure creates a hybrid superlattice with extremely low thermal conductivity. Vibrational characterization and

A new synthetic approach has recently been developed for the fabrication of freestanding crystalline perovskite oxide nanomembranes, which involves the epitaxial growth of a water-soluble sacrificial layer. By utilizing an ultrathin capping layer of SrTiO3, here we show that this sacrificial layer, as grown by pulsed laser deposition, can be stabilized in air and therefore be used as transferrable templates for ex situ epitaxial growth using other techniques. We find that the stability of these templates depends on the thickness of the capping layer. On these templates, freestanding superconducting SrTiO3 membranes were synthesized ex situ using molecular beam epitaxy, enabled by the lower growth temperature which preserves the sacrificial layer. This study paves the way for the synthesis of an expanded selection of freestanding oxide membranes and heterostructures with a wide variety of ex situ growth techniques.

Safety issues associated with lithium-ion batteries are of major concern, especially with the ever-growing demand for higher-energy-density storage devices. Although flame retardants (FRs) added to electrolytes can reduce fire hazards, large amounts of FRs are required and they severely deteriorate battery performance. Here, we report a feasible method to balance flame retardancy and electrochemical performance by coating an electrolyte-insoluble FR on commercial battery separators. By integrating dual materials via a two-pronged mechanism, the quantity of FR required could be limited to an ultrathin coating layer (4 μm) that rarely influences electrochemical performance. The developed composite separator has a four-times better flame retardancy than conventional polyolefin separators in full pouch cells. Additionally, this separator can be fabricated easily on a large scale for industrial applications. High-energy-density batteries (2 Ah) were assembled to demonstrate the scaling of the composite separator and to confirm its enhanced safety through nail penetration tests.

Aqueous Zn-based batteries are attractive because of the low cost and high theoretical capacity of the Zn metal anode. However, the Zn-based batteries developed so far utilize an excess amount of Zn (i.e., thick Zn metal anode), which decreases the energy density of the whole battery. Herein, we demonstrate an anode-free design (i.e., zero-excess Zn), which is enabled by employing a nanocarbon nucleation layer. Electrochemical studies show that this design allows for uniform Zn electrodeposition with high efficiency and stability over a range of current densities and plating capacities. Using this anode-free configuration, we showcase a Zn-MnO2 battery prototype, showing 68.2% capacity retention after 80 cycles. Our anode-free design opens a new direction for implementing aqueous Zn-based batteries in energy storage systems.

Gas-phase heterogeneous catalysis is a process spatially constrained on the two-dimensional surface of a solid catalyst. Here, we introduce a new toolkit to open up the third dimension. We discovered that the activity of a solid catalyst can be dramatically promoted by covering its surface with a nanoscale-thin layer of liquid electrolyte while maintaining efficient delivery of gas reactants, a strategy we call three-phase catalysis. Introducing the liquid electrolyte converts the original surface catalytic reaction into an electrochemical pathway with mass transfer facilitated by free ions in a three-dimensional space. We chose the oxidation of formaldehyde as a model reaction and observed a 25000-times enhancement in the turnover frequency of Pt in three-phase catalysis as compared to conventional heterogeneous catalysis. We envision three-phase catalysis as a new dimension for catalyst design and anticipate its applications in more chemical reactions from pollution control to the petrochemical industry.

Solid-state Li–S batteries are attractive due to their high energy density and safety. However, it is unclear whether the concepts from liquid electrolytes are applicable in the solid state to improve battery performance. Here, we demonstrate that the nanoscale encapsulation concept based on Li2S@TiS2 core–shell particles, originally developed in liquid electrolytes, is effective in solid polymer electrolytes. Using in situ optical cell and sulfur K-edge X-ray absorption, we find that polysulfides form and are well-trapped inside individual particles by the nanoscale TiS2 encapsulation. This TiS2 encapsulation layer also functions to catalyze the oxidation reaction of Li2S to sulfur, even in solid-state electrolytes, proven by both experiments and density functional theory calculations. A high cell-level specific energy of 427 W·h·kg–1 is achieved by integrating the Li2S@TiS2 cathode with a poly­(ethylene oxide)-based electrolyte and a lithium metal anode. This study points to the fruitful direction of borrowing concepts from liquid electrolytes into solid-state batteries.

Rechargeable hydrogen gas batteries show promises for the integration of renewable yet intermittent solar and wind electricity into the grid energy storage. Here, we describe a rechargeable, high-rate, and long-life hydrogen gas battery that exploits a nanostructured lithium manganese oxide cathode and a hydrogen gas anode in an aqueous electrolyte. The proposed lithium manganese oxide-hydrogen battery shows a discharge potential of ∼1.3 V, a remarkable rate of 50 C with Coulombic efficiency of ∼99.8%, and a robust cycle life. A systematic electrochemical study demonstrates the significance of the electrocatalytic hydrogen gas anode and reveals the charge storage mechanism of the lithium manganese oxide-hydrogen battery. This work provides opportunities for the development of new rechargeable hydrogen batteries for the future grid-scale energy storage.

Safety issues in lithium-ion batteries have raised serious concerns due to their ubiquitous utilization and close contact with the human body. Replacing flammable liquid electrolytes, solid-state electrolytes (SSEs) is thought to address this issue as well as provide unmatched energy densities in Li-based batteries. However, among the most intensively studied SSEs, polymeric solid electrolyte and polymer/ceramic composites are usually flammable, leaving the safety issue unattended. Here, we report the first design of a fireproof, ultralightweight polymer-polymer SSE. The SSE is composed of a porous mechanic enforcer (polyimide, PI), a fire-retardant additive (decabromodiphenyl ethane, DBDPE), and a ionic conductive polymer electrolyte (poly(ethylene oxide)/lithium bis(trifluoromethanesulfonyl)imide). The whole SSE is made from organic materials, with a thin, tunable thickness (10-25 μm), which endorse the energy density comparable to conventional separator/liquid electrolytes. The PI/DBDPE film is thermally stable, nonflammable, and mechanically strong, preventing Li-Li symmetrical cells from short-circuiting after more than 300 h of cycling. LiFePO

With the increasing strategies aimed at repressing shuttle problems in the lithium–sulfur battery, dissolved contents of polysulfides are significantly reduced. Except for solid-state Li2S2 and Li2...

Aqueous Zn-ion batteries present low-cost, safe, and high-energy battery technology but suffer from the lack of suitable cathode materials because of the sluggish intercalation kinetics associated with the large size of hydrated zinc ions. Herein we report an effective and general strategy to transform inactive intercalation hosts into efficient Zn2+ storage materials through intercalation energy tuning. Using MoS2 as a model system, we show both experimentally and theoretically that even hosts with an originally poor Zn2+ diffusivity can allow fast Zn2+ diffusion. Through simple interlayer spacing and hydrophilicity engineering that can be experimentally achieved by oxygen incorporation, the Zn2+ diffusivity is boosted by 3 orders of magnitude, effectively enabling the otherwise barely active MoS2 to achieve a high capacity of 232 mAh g–1, which is 10 times that of its pristine form. The strategy developed in our work can be generally applied for enhancing the ion storage capacity of metal chalcogenides ...

The Mg/S battery is attractive because of its high theoretical energy density and the abundance of Mg and S on the earth. However, its development is hindered by the lack of understanding to the underlying electrochemical reaction mechanism of its charge-discharge processes. Here, using a unique in situ X-ray absorption spectroscopic tool, we systematically study the reaction pathways of the Mg/S cells in Mg(HMDS)

A new synthetic approach has recently been developed for the fabrication of freestanding crystalline perovskite oxide nanomembranes, which involves the epitaxial growth of a water-soluble sacrificial layer. By utilizing an ultrathin capping layer of SrTiO

Aqueous Zn-based batteries are attractive because of the low cost and high theoretical capacity of the Zn metal anode. However, the Zn-based batteries developed so far utilize an excess amount of Zn (i.e., thick Zn metal anode), which decreases the energy density of the whole battery. Herein, we demonstrate an anode-free design (i.e., zero-excess Zn), which is enabled by employing a nanocarbon nucleation layer. Electrochemical studies show that this design allows for uniform Zn electrodeposition with high efficiency and stability over a range of current densities and plating capacities. Using this anode-free configuration, we showcase a Zn-MnO

The global COVID-19 pandemic has changed many aspects of daily lives. Wearing personal protective equipment, especially respirators (face masks), has become common for both the public and medical professionals, proving to be effective in preventing spread of the virus. Nevertheless, a detailed understanding of respirator filtration-layer internal structures and their physical configurations is lacking. Here, we report three-dimensional (3D) internal analysis of N95 filtration layers via X-ray tomography. Using deep learning methods, we uncover how the distribution and diameters of fibers within these layers directly affect contaminant particle filtration. The average porosity of the filter layers is found to be 89.1%. Contaminants are more efficiently captured by denser fiber regions, with fibers

Nanostructured electrodes are among the most important candidates for high-capacity battery chemistry. However, the high surface area they possess causes serious issues. First, it would decrease the Coulombic efficiencies. Second, they have significant intakes of liquid electrolytes, which reduce the energy density and increase the battery cost. Third, solid-electrolyte interphase growth is accelerated, affecting the cycling stability. Therefore, the interphase chemistry regarding electrolyte contact is crucial, which was rarely studied. Here, we present a completely new strategy of limiting effective surface area by introducing an "electrolyte-phobic surface". Using this method, the electrolyte intake was limited. The initial Coulombic efficiencies were increased up to ∼88%, compared to ∼60% of the control. The electrolyte-phobic layer of Si particles is also compatible with the binder, stabilizing the electrode for long-term cycling. This study advances the understanding of interphase chemistry, and the introduction of the universal concept of electrolyte-phobicity benefits the next-generation battery designs.

As Coronavirus disease 2019 (COVID-19) continues to spread, a detailed understanding on the transmission mechanisms is of paramount importance. The disease transmits mainly through respiratory droplets and aerosol. Although models for the evaporation and trajectory of respiratory droplets have been developed, how the environment impacts the transmission of COVID-19 is still unclear. In this study, we investigate the propagation of respiratory droplets and aerosol particles generated by speech under a wide range of temperature (0 °C to 40 °C) and relative humidity (0% to 92%) conditions. We show that droplets can travel three times farther in low temperature and high humidity environment, while the amount of aerosol increases in high temperature and low humidity environment. The results also underscore the importance of proper ventilation, as droplets and aerosol spread significantly farther in airstreams. This study contributes to the understanding of the environmental impact on COVID-19 transmission.

The COVID-19 pandemic is currently causing a severe disruption and shortage in the global supply chain of necessary personal protective equipment (e.g., N95 respirators). The U.S. CDC has recommended use of household cloth by the general public to make cloth face coverings as a method of source control. We evaluated the filtration properties of natural and synthetic materials using a modified procedure for N95 respirator approval. Common fabrics of cotton, polyester, nylon, and silk had filtration efficiency of 5–25%, polypropylene spunbond had filtration efficiency 6–10%, and paper-based products had filtration efficiency of 10–20%. An advantage of polypropylene spunbond is that it can be simply triboelectrically charged to enhance the filtration efficiency (from 6 to >10%) without any increase in pressure (stable overnight and in humid environments). Using the filtration quality factor, fabric microstructure, and charging ability, we are able to provide an assessment of suggested fabric materials for homemade facial coverings.

The nanostructure design of a prereserved hollow space to accommodate 300% volume change of silicon anodes has created exciting promises for high-energy batteries. However, challenges with weak mechanical stability during the calendering process of electrode fabrication and poor volumetric energy density remain to be solved. Here we fabricated a pressure-resistant silicon structure by designing a dense silicon shell coating on secondary micrometer particles, each consisting of many silicon nanoparticles. The silicon skin layer significantly improves mechanical stability, while the inner porous structure efficiently accommodates the volume expansion. Such a structure can resist a high pressure of over 100 MPa and is well-maintained after the calendering process, demonstrating a high volumetric capacity of 2041 mAh cm–3. In addition, the dense silicon shell decreases the surface area and thus increases the initial Coulombic efficiency. With further encapsulation with a graphene cage, which allows the silico...

Lithium-sulfur (Li-S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithium sulfide (Li

Electric-double-layer (EDL) gating with liquid electrolyte has been a powerful tool widely used to explore emerging interfacial electronic phenomena. Due to the large EDL capacitance, a high carrier density up to 1014 cm–2 can be induced, directly leading to the realization of field-induced insulator to metal (or superconductor) transition. However, the liquid nature of the electrolyte has created technical issues including possible side electrochemical reactions or intercalation, and the potential for huge strain at the interface during cooling. In addition, the liquid coverage of active devices also makes many surface characterizations and in situ measurements challenging. Here, we demonstrate an all solid-state EDL device based on a solid superionic conductor LaF3, which can be used as both a substrate and a fluorine ionic gate dielectric to achieve a wide tunability of carrier density without the issues of strain or electrochemical reactions and can expose the active device surface for external access...

Layered metal chalcogenide materials provide a versatile platform to investigate emergent phenomena and two-dimensional (2D) superconductivity at/near the atomically thin limit. In particular, gate-induced interfacial superconductivity realized by the use of an electric-double-layer transistor (EDLT) has greatly extended the capability to electrically induce superconductivity in oxides, nitrides and transition metal chalcogenides and enable one to explore new physics, such as the Ising pairing mechanism. Exploiting gate-induced superconductivity in various materials can provide us with additional platforms to understand emergent interfacial superconductivity. Here, we report the discovery of gate-induced 2D superconductivity in layered 1T-SnSe2, a typical member of the main-group metal dichalcogenide (MDC) family, using an EDLT gating geometry. A superconducting transition temperature Tc around 3.9 K was demonstrated at the EDL interface. The 2D nature of the superconductivity therein was further confirmed based on 1) a 2D Tinkham description of the angle-dependent upper critical field, 2) the existence of a quantum creep state as well as a large ratio of the coherence length to the thickness of superconductivity. Interestingly, the in-plane approaching zero temperature was found to be 2-3 times higher than the Pauli limit, which might be related to an electric field-modulated spin-orbit interaction. Such results provide a new perspective to expand the material matrix available for gate-induced 2D superconductivity and the fundamental understanding of interfacial superconductivity., Comment: 18 pages, 4 figures, accepted by Nano Letters

Aerosol-induced haze problem has become a serious environmental concern. Filtration is widely applied to remove aerosols from gas streams. Despite classical filtration theories, the nanoscale capture and evolution of aerosols is not yet clearly understood. Here we report an in situ investigation on the nanoscale capture and evolution of aerosols on polyimide nanofibers. We discovered different capture and evolution behaviors among three types of aerosols: wetting liquid droplets, nonwetting liquid droplets, and solid particles. The wetting droplets had small contact angles and could move, coalesce, and form axisymmetric conformations on polyimide nanofibers. In contrast, the nonwetting droplets had a large contact angle on polyimide nanofibers and formed nonaxisymmetric conformations. Different from the liquid droplets, the solid particles could not move along the nanofibers and formed dendritic structures. This study provides an important insight for obtaining a deep understanding of the nanoscale capture and evolution of aerosols and benefits future design and development of advanced filters.

Face masks are widely used to filter airborne pollutants, especially when particulate matter (PM) pollution has become a serious concern to public health. Here, the concept of thermal management is introduced into face masks for the first time to enhance the thermal comfort of the user. A system of nanofiber on nanoporous polyethylene (fiber/nanoPE) is developed where the nanofibers with strong PM adhesion ensure high PM capture efficiency (99.6% for PM2.5) with low pressure drop and the nanoPE substrate with high-infrared (IR) transparency (92.1%, weighted based on human body radiation) results in effective radiative cooling. We further demonstrate that by coating nanoPE with a layer of Ag, the fiber/Ag/nanoPE mask shows a high IR reflectance (87.0%) and can be used for warming purposes. These multifunctional face mask designs can be explored for both outdoor and indoor applications to protect people from PM pollutants and simultaneously achieve personal thermal comfort.

An all solid-state lithium-ion battery with high energy density and high safety is a promising solution for a next-generation energy storage system. High interface resistance of the electrodes and poor ion conductivity of solid-state electrolytes are two main challenges for solid-state batteries, which require operation at elevated temperatures of 60–90 °C. Herein, we report the facile synthesis of Al3+/Nb5+ codoped cubic Li7La3Zr2O12 (LLZO) nanoparticles and LLZO nanoparticle-decorated porous carbon foam (LLZO@C) by the one-step Pechini sol–gel method. The LLZO nanoparticle-filled poly(ethylene oxide) electrolyte shows improved conductivity compared with filler-free samples. The sulfur composite cathode based on LLZO@C can deliver an attractive specific capacity of >900 mAh g–1 at the human body temperature 37 °C and a high capacity of 1210 and 1556 mAh g–1 at 50 and 70 °C, respectively. In addition, the solid-state Li–S batteries exhibit high Coulombic efficiency and show remarkably stable cycling perfo...

Intercalation of exotic atoms or molecules into the layered materials remains an extensively investigated subject in current physics and chemistry. However, traditionally melt-growth and chemical interaction strategies are either limited by insufficiency of intercalant concentrations or destitute of accurate controllability. Here, we have developed a general electrochemical intercalation method to efficaciously regulate the concentration of zerovalent copper atoms into layered Bi2Se3, followed by comprehensive experimental characterization and analyses. Up to 57% copper atoms (Cu6.7Bi2Se3) can be intercalated with no disruption to the host lattice. Meanwhile the unconventional resistance dip accompanied by a hysteresis loop below 40 K, as well as the emergence of new Raman peak in CuxBi2Se3, is a distinct manifestation of the interplay between intercalated Cu atoms with Bi2Se3 host. Our work demonstrates a new methodology to study fundamentally new and unexpected physical behaviors in intercalated metasta...

Lithium metal has re-emerged as an exciting anode for high energy lithium-ion batteries due to its high specific capacity of 3860 mAh g–1 and lowest electrochemical potential of all known materials. However, lithium has been plagued by the issues of dendrite formation, high chemical reactivity with electrolyte, and infinite relative volume expansion during plating and stripping, which present safety hazards and low cycling efficiency in batteries with lithium metal electrodes. There have been a lot of recent studies on Li metal although little work has focused on the initial nucleation and growth behavior of Li metal, neglecting a critical fundamental scientific foundation of Li plating. Here, we study experimentally the morphology of lithium in the early stages of nucleation and growth on planar copper electrodes in liquid organic electrolyte. We elucidate the dependence of lithium nuclei size, shape, and areal density on current rate, consistent with classical nucleation and growth theory. We found that...

Particulate matter (PM) pollution has caused many serious public health issues. Whereas indoor air protection usually relies on expensive and energy-consuming filtering devices, direct PM filtration by window screens has attracted increasing attention. Recently, electrospun polymer nanofiber networks have been developed as transparent filters for highly efficient PM2.5 removal; however, it remains challenging to uniformly coat the nanofibers on window screens on a large scale and with low cost. Here, we report a blow-spinning technique that is fast, efficient, and free of high voltages for the large-scale direct coating of nanofibers onto window screens for indoor PM pollution protection. We have achieved a transparent air filter of 80% optical transparency with >99% standard removal efficiency level for PM2.5. A test on a real window (1 m × 2 m) in Beijing has proven that the nanofiber transparent air filter acquires excellent PM2.5 removal efficiency of 90.6% over 12 h under extremely hazy air condition...

A variety of methods including tuning chemical compositions, structures, crystallinity, defects and strain, and electrochemical intercalation have been demonstrated to enhance the catalytic activity. However, none of these tuning methods provide direct dynamical control during catalytic reactions. Here we propose a new method to tune the activity of catalysts through solid-state ion gating manipulation and adjustment (SIGMA) using a catalysis transistor. SIGMA can electrostatically dope the surface of catalysts with a high electron concentration over 5 × 10

The stability of modern lithium-ion batteries depends critically on an effective solid-electrolyte interphase (SEI), a passivation layer that forms on the carbonaceous negative electrode as a result of electrolyte reduction. However, a nanoscopic understanding of how the SEI evolves with battery aging remains limited due to the difficulty in characterizing the structural and chemical properties of this sensitive interphase. In this work, we image the SEI on carbon black negative electrodes using cryogenic transmission electron microscopy (cryo-TEM) and track its evolution during cycling. We find that a thin, primarily amorphous SEI nucleates on the first cycle, which further evolves into one of two distinct SEI morphologies upon further cycling: (1) a compact SEI, with a high concentration of inorganic components that effectively passivates the negative electrode; and (2) an extended SEI spanning hundreds of nanometers. This extended SEI grows on particles that lack a compact SEI and consists primarily of alkyl carbonates. The diversity in observed SEI morphologies suggests that SEI growth is a highly heterogeneous process. The simultaneous emergence of these distinct SEI morphologies highlights the necessity of effective passivation by the SEI, as large-scale extended SEI growths negatively impact lithium-ion transport, contribute to capacity loss, and may accelerate battery failure.

Aqueous Zn-ion batteries present low-cost, safe, and high-energy battery technology but suffer from the lack of suitable cathode materials because of the sluggish intercalation kinetics associated with the large size of hydrated zinc ions. Herein we report an effective and general strategy to transform inactive intercalation hosts into efficient Zn

Layered two-dimensional (2D) materials have highly anisotropic thermal properties between the in-plane and cross-plane directions. Conventionally, it is thought that cross-plane thermal conductivities (κ

Engineered nanoparticles (NPs) can negatively impact biological systems through induced generation of reactive oxygen species (ROS). Overproduced ROS cause biochemical damage and hence need to be effectively buffered by a sophisticated cellular oxidative stress response system. How this complex cellular system, which consists of multiple enzymes, responds to NP-induced ROS is largely unknown. Here, we apply a single cell analysis to quantitatively evaluate 10 key ROS responsive genes simultaneously to understand how the cell prioritizes tasks and reallocates resources in response to NP-induced oxidative stress. We focus on rainbow trout gill epithelial cells-a model cell type for environmental exposure-and their response to the massive generation of ROS induced by lithium cobalt oxide (LCO) NPs, which are extensively used as cathode materials in lithium ion batteries. Using multiplexed fluctuation localization imaging-based fluorescence in situ hybridization (fliFISH) in single cells, we found a shift in the expression of oxidative stress response genes with initial increase in genes targeting superoxide species, followed by increase in genes targeting peroxide and hydroxyl species. In contrast, Li+ and Co2+, at concentrations expected to be shed from the NPs, did not induce ROS generation but showed a potent inhibition of transcription for all 10 stress response genes. Taken together, our findings suggest a "two-hit" model for LCO NP toxicity, where the intact LCO NPs induce high levels of ROS that elicit sequential engagement of stress response genes, while the released metal ions suppress the expression of these genes. Consequently, these effects synergistically drive the exposed cells to become more vulnerable to ROS stress and damage.

Lithium (Li) metal has long been considered the "holy grail" of battery anode chemistry but is plagued by low efficiency and poor safety due to its high chemical reactivity and large volume fluctuation, respectively. Here we introduce a new host of wrinkled graphene cage (WGC) for Li metal. Different from recently reported amorphous carbon spheres, WGC show highly improved mechanical stability, better Li ion conductivity, and excellent solid electrolyte interphase (SEI) for continuous robust Li metal protection. At low areal capacities, Li metal is preferentially deposited inside the graphene cage. Cryogenic electron microscopy characterization shows that a uniform and stable SEI forms on the WGC surface that can shield the Li metal from direct exposure to electrolyte. With increased areal capacities, Li metal is plated densely and homogeneously into the outer pore spaces between graphene cages with no dendrite growth or volume change. As a result, a high Coulombic efficiency (CE) of ∼98.0% was achieved under 0.5 mA/cm

Substitution of selenium for sulfur in the cathode of a rechargeable battery containing Sx molecules in microporous slits in carbon allows a better characterization of the electrochemical reactions that occur. Paired with a metallic lithium anode, the Sex chains are converted to Li2Se in a single-step reaction. With a sodium anode, a sequential chemical reaction is characterized by a continuous chain shortening of Sex upon initial discharge before completing the reduction to Na2Se; on charge, the reconstituted Sex molecules retain a smaller x value than the original Sex chain molecule. In both cases, the Se molecules remain almost completely confined to the micropore slits to give a long cycle life.

The initial lithium loss during the formation stage is a critical issue that significantly reduces the specific capacity and energy density of current rechargeable lithium-ion batteries (LIBs). An effective strategy to solve this problem is using electrode prelithiation additives that can work as a secondary lithium source and compensate the initial lithium loss. Herein we show that nanocomposites of lithium fluoride and metal (e.g., LiF/Co and LiF/Fe) can be efficient cathode prelithiation materials. The thorough mixing of ultrafine lithium fluoride and metal particles (∼5 nm) allows lithium to be easily extracted from the nanocomposites via an inverse conversion reaction. The LiF/Co nanocomposite exhibits an open circuit voltage (OCV, 1.5 V) with good compatibility with that of existing cathode materials and delivers a high first-cycle "donor" lithium-ion capacity (516 mA h g(-1)). When used as an additive to a LiFePO4 cathode, the LiF/Co nanocomposite provides high lithium compensation efficiency. Importantly, the as-formed LiF/metal nanocomposites possess high stability and good compatibility with the regular solvent, binder, and existing battery processing conditions, in contrast with the anode prelithiation materials that usually suffer from issues of high chemical reactivity and instability. The facile synthesis route, high stability in ambient and battery processing conditions, and high "donor" lithium-ion capacity make the LiF/metal nanocomposites ideal cathode prelithiation materials for LIBs.

Here, we studied the interwall friction and sliding behaviors of double-walled carbon nanotubes (DWCNTs). The interwall friction shows a linear dependence on the pullout velocity of the inner wall. The axial curvature in DWCNTs causes the significant increase of the interwall friction. The axial curvature also affects the sliding behavior of the inner wall. Compared with the axial curvature, the opening ends of DWCNTs play tiny roles in their interwall friction.

High ionic conductivity solid polymer electrolyte (SPE) has long been desired for the next generation high energy and safe rechargeable lithium batteries. Among all of the SPEs, composite polymer electrolyte (CPE) with ceramic fillers has garnered great interest due to the enhancement of ionic conductivity. However, the high degree of polymer crystallinity, agglomeration of ceramic fillers, and weak polymer-ceramic interaction limit the further improvement of ionic conductivity. Different from the existing methods of blending preformed ceramic particles with polymers, here we introduce an in situ synthesis of ceramic filler particles in polymer electrolyte. Much stronger chemical/mechanical interactions between monodispersed 12 nm diameter SiO2 nanospheres and poly(ethylene oxide) (PEO) chains were produced by in situ hydrolysis, which significantly suppresses the crystallization of PEO and thus facilitates polymer segmental motion for ionic conduction. In addition, an improved degree of LiClO4 dissociation can also be achieved. All of these lead to good ionic conductivity (1.2 × 10(-3) S cm(-1) at 60 °C, 4.4 × 10(-5) S cm(-1) at 30 °C). At the same time, largely extended electrochemical stability window up to 5.5 V can be observed. We further demonstrated all-solid-state lithium batteries showing excellent rate capability as well as good cycling performance.

Among all solid electrolytes, composite solid polymer electrolytes, comprised of polymer matrix and ceramic fillers, garner great interest due to the enhancement of ionic conductivity and mechanical properties derived from ceramic–polymer interactions. Here, we report a composite electrolyte with densely packed, vertically aligned, and continuous nanoscale ceramic–polymer interfaces, using surface-modified anodized aluminum oxide as the ceramic scaffold and poly(ethylene oxide) as the polymer matrix. The fast Li+ transport along the ceramic–polymer interfaces was proven experimentally for the first time, and an interfacial ionic conductivity higher than 10–3 S/cm at 0 °C was predicted. The presented composite solid electrolyte achieved an ionic conductivity as high as 5.82 × 10–4 S/cm at the electrode level. The vertically aligned interfacial structure in the composite electrolytes enables the viable application of the composite solid electrolyte with superior ionic conductivity and high hardness, allowin...

Layered metal chalcogenide materials provide a versatile platform to investigate emergent phenomena and two-dimensional (2D) superconductivity at/near the atomically thin limit. In particular, gate-induced interfacial superconductivity realized by the use of an electric-double-layer transistor (EDLT) has greatly extended the capability to electrically induce superconductivity in oxides, nitrides, and transition metal chalcogenides and enable one to explore new physics, such as the Ising pairing mechanism. Exploiting gate-induced superconductivity in various materials can provide us with additional platforms to understand emergent interfacial superconductivity. Here, we report the discovery of gate-induced 2D superconductivity in layered 1T-SnSe

One of the key challenges of Si-based anodes for lithium ion batteries is the large volume change upon lithiation and delithiation, which commonly leads to electrochemi-mechanical degradation and subsequent fast capacity fading. Recent studies have shown that applying nanometer-thick coating layers on Si nanoparticle (SiNPs) enhances cyclability and capacity retention. However, it is far from clear how the coating layer function from the point of view of both surface chemistry and electrochemi-mechanical effect. Herein, we use in situ transmission electron microscopy to investigate the lithiation/delithiation kinetics of SiNPs coated with a conductive polymer, polypyrrole (PPy). We discovered that this coating layer can lead to "self-delithiation" or "self-discharging" at different stages of lithiation. We rationalized that the self-discharging is driven by the internal compressive stress generated inside the lithiated SiNPs due to the constraint effect of the coating layer. We also noticed that the critical size of lithiation-induced fracture of SiNPs is increased from ∼150 nm for bare SiNPs to ∼380 nm for the PPy-coated SiNPs, showing a mechanically protective role of the coating layer. These observations demonstrate both beneficial and detrimental roles of the surface coatings, shedding light on rational design of surface coatings for silicon to retain high-power and high capacity as anode for lithium ion batteries.

A high throughput surface texturing process for optical and optoelectric devices based on a large-area self-assembly of nanospheres via a low-cost micropropulsive injection (MPI) method is presented. The novel MPI process enables the formation of a well-organized monolayer of hexagonally arranged nanosphere arrays (NAs) with tunable periodicity directly on the water surface, which is then transferred onto the preset substrates. This process can readily reach a throughput of 3000 wafers/h, which is compatible with the high volume photovoltaic manufacturing, thereby presenting a highly versatile platform for the fabrication of periodic nanotexturing on device surfaces. Specifically, a double-sided grating texturing with top-sided nanopencils and bottom-sided inverted-nanopyramids is realized in a thin film of crystalline silicon (28 μm in thickness) using chemical etching on the mask of NAs to significantly enhance antireflection and light trapping, resulting in absorptions nearly approaching the Lambertian limit over a broad wavelength range of 375-1000 nm and even surpassing this limit beyond 1000 nm. In addition, it is demonstrated that the NAs can serve as templates for replicas of three-dimensional conformal amorphous silicon films with significantly enhanced light harvesting. The MPI induced self-assembly process may provide a universal and cost-effective solution for boosting light utilization, a problem of crucial importance for ultrathin solar cells.

Transparent conductive film on plastic substrate is a critical component in low-cost, flexible, and lightweight optoelectronics. Industrial-scale manufacturing of high-performance transparent conductive flexible plastic is needed to enable wide-ranging applications. Here, we demonstrate a continuous roll-to-roll (R2R) production of transparent conductive flexible plastic based on a metal nanowire network fully encapsulated between graphene monolayer and plastic substrate. Large-area graphene film grown on Cu foil via a R2R chemical vapor deposition process was hot-laminated onto nanowires precoated EVA/PET film, followed by a R2R electrochemical delamination that preserves the Cu foil for reuse. The encapsulated structure minimized the resistance of both wire-to-wire junctions and graphene grain boundaries and strengthened adhesion of nanowires and graphene to plastic substrate, resulting in superior optoelectronic properties (sheet resistance of ∼8 Ω sq(-1) at 94% transmittance), remarkable corrosion resistance, and excellent mechanical flexibility. With these advantages, long-cycle life flexible electrochromic devices are demonstrated, showing up to 10000 cycles.

Although the rechargeable lithium-sulfur battery system has attracted significant attention due to its high theoretical specific energy, its implementation has been impeded by multiple challenges, especially the dissolution of intermediate lithium polysulfide (Li2Sn) species into the electrolyte. Introducing anchoring materials, which can induce strong binding interaction with Li2Sn species, has been demonstrated as an effective way to overcome this problem and achieve long-term cycling stability and high-rate performance. The interaction between Li2Sn species and anchoring materials should be studied at the atomic level in order to understand the mechanism behind the anchoring effect and to identify ideal anchoring materials to further improve the performance of Li-S batteries. Using first-principles approach with van der Waals interaction included, we systematically investigate the adsorption of Li2Sn species on various two-dimensional layered materials (oxides, sulfides, and chlorides) and study the detailed interaction and electronic structure, including binding strength, configuration distortion, and charge transfer. We gain insight into how van der Waals interaction and chemical binding contribute to the adsorption of Li2Sn species for anchoring materials with strong, medium, and weak interactions. We understand why the anchoring materials can avoid the detachment of Li2S as in carbon substrate, and we discover that too strong binding strength can cause decomposition of Li2Sn species.

Lithium metal is one of the most promising candidates as an anode material for next-generation energy storage systems due to its highest specific capacity (3860 mAh/g) and lowest redox potential of all. The uncontrolled lithium dendrite growth that causes a poor cycling performance and serious safety hazards, however, presents a significant challenge for the realization of lithium metal-based batteries. Here, we demonstrate a novel electrode design by placing a three-dimensional (3D) oxidized polyacrylonitrile nanofiber network on top of the current collector. The polymer fiber with polar surface functional groups could guide the lithium ions to form uniform lithium metal deposits confined on the polymer fiber surface and in the 3D polymer layer. We showed stable cycling of lithium metal anode with an average Coulombic efficiency of 97.4% over 120 cycles in ether-based electrolyte at a current density of 3 mA/cm(2) for a total of 1 mAh/cm(2) of lithium.

We demonstrate electrical control over coherent optical absorption in a graphene-based Salisbury screen consisting of a single layer of graphene placed in close proximity to a gold back reflector. The screen was designed to enhance light absorption at a target wavelength of 3.2 μm by using a 600 nm-thick, nonabsorbing silica spacer layer. An ionic gel layer placed on top of the screen was used to electrically gate the charge density in the graphene layer. Spectroscopic reflectance measurements were performed in situ as a function of gate bias. The changes in the reflectance spectra were analyzed using a Fresnel based transfer matrix model in which graphene was treated as an infinitesimally thin sheet with a conductivity given by the Kubo formula. The analysis reveals that a careful choice of the ionic gel layer thickness can lead to optical absorption enhancements of up to 5.5 times for the Salisbury screen compared to a suspended sheet of graphene. In addition to these absorption enhancements, we demonstrate very large electrically induced changes in the optical absorption of graphene of ∼3.3% per volt, the highest attained so far in a device that features an atomically thick active layer. This is attributable in part to the more effective gating achieved with the ion gel over the conventional dielectric back gates and partially by achieving a desirable coherent absorption effect linked to the presence of the thin ion gel that boosts the absorption by 40%.

Two-dimensional (2D) layered materials consist of covalently bonded 2D atomic layers stacked by van der Waals interactions. Such anisotropic bonding nature gives rise to the orientation-dependent functionalities of the 2D layered materials. Different from most studies of 2D materials with their atomic layers parallel to substrate, we have recently developed layer vertically aligned 2D material nanofilms. Built on these developments, here, we demonstrate the synthesis of vertical heterostructure of n-type MoS2 and p-type WSe2 with vertically aligned atomic layers. Thin film of MoS2/WSe2 vertical structure was successfully synthesized without significant alloy formation. The heterostructure synthesis is scalable to a large area over 1 cm2. We demonstrated the pn junction diode behavior of the heterostructure device. This novel device geometry opens up exciting opportunities for a variety of electronic and optoelectronic devices, complementary to the recent interesting vertical heterostructures with horizont...