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Showing papers by "Yi Cui published in 2019"


Journal ArticleDOI
TL;DR: Liu et al. as mentioned in this paper discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg−1, up to 500 Wh kg −1, for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials.
Abstract: State-of-the-art lithium (Li)-ion batteries are approaching their specific energy limits yet are challenged by the ever-increasing demand of today’s energy storage and power applications, especially for electric vehicles. Li metal is considered an ultimate anode material for future high-energy rechargeable batteries when combined with existing or emerging high-capacity cathode materials. However, much current research focuses on the battery materials level, and there have been very few accounts of cell design principles. Here we discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg−1, up to 500 Wh kg−1, for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials. We also provide an analysis of key factors such as cathode loading, electrolyte amount and Li foil thickness that impact the cell-level cycle life. Furthermore, we identify several important strategies to reduce electrolyte-Li reaction, protect Li surfaces and stabilize anode architectures for long-cycling high-specific-energy cells. Jun Liu and Battery500 Consortium colleagues contemplate the way forward towards high-energy and long-cycling practical batteries.

1,747 citations


Journal ArticleDOI
22 Nov 2019-Science
TL;DR: Examples indicate that nanostructured materials and nanoarchitectured electrodes can provide solutions for designing and realizing high-energy, high-power, and long-lasting energy storage devices.
Abstract: Lithium-ion batteries, which power portable electronics, electric vehicles, and stationary storage, have been recognized with the 2019 Nobel Prize in chemistry. The development of nanomaterials and their related processing into electrodes and devices can improve the performance and/or development of the existing energy storage systems. We provide a perspective on recent progress in the application of nanomaterials in energy storage devices, such as supercapacitors and batteries. The versatility of nanomaterials can lead to power sources for portable, flexible, foldable, and distributable electronics; electric transportation; and grid-scale storage, as well as integration in living environments and biomedical systems. To overcome limitations of nanomaterials related to high reactivity and chemical instability caused by their high surface area, nanoparticles with different functionalities should be combined in smart architectures on nano- and microscales. The integration of nanomaterials into functional architectures and devices requires the development of advanced manufacturing approaches. We discuss successful strategies and outline a roadmap for the exploitation of nanomaterials for enabling future energy storage applications, such as powering distributed sensor networks and flexible and wearable electronics.

941 citations


Journal ArticleDOI
TL;DR: In this article, the authors discuss the challenges and future research directions towards fast charging at the level of battery materials from mass transport, charge transfer and thermal management perspectives, and highlight advanced characterization techniques to understand the failure mechanisms of batteries during fast charging, which in turn would inform more rational battery designs.
Abstract: Extreme fast charging, with a goal of 15 minutes recharge time, is poised to accelerate mass market adoption of electric vehicles, curb greenhouse gas emissions and, in turn, provide nations with greater energy security. However, the realization of such a goal requires research and development across multiple levels, with battery technology being a key technical barrier. The present-day high-energy lithium-ion batteries with graphite anodes and transition metal oxide cathodes in liquid electrolytes are unable to achieve the fast-charging goal without negatively affecting electrochemical performance and safety. Here we discuss the challenges and future research directions towards fast charging at the level of battery materials from mass transport, charge transfer and thermal management perspectives. Moreover, we highlight advanced characterization techniques to fundamentally understand the failure mechanisms of batteries during fast charging, which in turn would inform more rational battery designs. Along with high energy density, fast-charging ability would enable battery-powered electric vehicles. Here Yi Cui and colleagues review battery materials requirements for fast charging and discuss future design strategies.

866 citations


Journal ArticleDOI
29 Aug 2019-Nature
TL;DR: The observation of superconductivity in an infinite-layer nickelate that is isostructural to infinite- Layer copper oxides11–13 and the possibility of a family of nickelate superconductors analogous to Copper oxides and pnictides25 is suggested.
Abstract: The discovery of unconventional superconductivity in (La,Ba)2CuO4 (ref. 1) has motivated the study of compounds with similar crystal and electronic structure, with the aim of finding additional superconductors and understanding the origins of copper oxide superconductivity. Isostructural examples include bulk superconducting Sr2RuO4 (ref. 2) and surface-electron-doped Sr2IrO4, which exhibits spectroscopic signatures consistent with a superconducting gap3,4, although a zero-resistance state has not yet been observed. This approach has also led to the theoretical investigation of nickelates5,6, as well as thin-film heterostructures designed to host superconductivity. One such structure is the LaAlO3/LaNiO3 superlattice7–9, which has been recently proposed for the creation of an artificially layered nickelate heterostructure with a singly occupied $${d}_{{x}^{2}-{y}^{2}}$$ band. The absence of superconductivity observed in previous related experiments has been attributed, at least in part, to incomplete polarization of the eg orbitals10. Here we report the observation of superconductivity in an infinite-layer nickelate that is isostructural to infinite-layer copper oxides11–13. Using soft-chemistry topotactic reduction14–20, NdNiO2 and Nd0.8Sr0.2NiO2 single-crystal thin films are synthesized by reducing the perovskite precursor phase. Whereas NdNiO2 exhibits a resistive upturn at low temperature, measurements of the resistivity, critical current density and magnetic-field response of Nd0.8Sr0.2NiO2 indicate a superconducting transition temperature of about 9 to 15 kelvin. Because this compound is a member of a series of reduced layered nickelate crystal structures21–23, these results suggest the possibility of a family of nickelate superconductors analogous to copper oxides24 and pnictides25. Superconductivity is demonstrated in an infinite-layer nickelate similar to infinite-layer copper oxides, which is synthesized using soft- chemistry topotactic reduction of the perovskite precursor phase.

690 citations


Journal ArticleDOI
TL;DR: A nanoporous polyimide film filled with a solid polymer electrolyte has high ionic conductivity and high mechanical strength, and an all-solid-state lithium-ion batteries fabricated with PI/PEO/LiTFSI solid electrolyte show good cycling performance and withstand abuse tests such as bending, cutting and nail penetration.
Abstract: The urgent need for safer batteries is leading research to all-solid-state lithium-based cells. To achieve energy density comparable to liquid electrolyte-based cells, ultrathin and lightweight solid electrolytes with high ionic conductivity are desired. However, solid electrolytes with comparable thicknesses to commercial polymer electrolyte separators (~10 μm) used in liquid electrolytes remain challenging to make because of the increased risk of short-circuiting the battery. Here, we report on a polymer–polymer solid-state electrolyte design, demonstrated with an 8.6-μm-thick nanoporous polyimide (PI) film filled with polyethylene oxide/lithium bis(trifluoromethanesulfonyl)imide (PEO/LiTFSI) that can be used as a safe solid polymer electrolyte. The PI film is nonflammable and mechanically strong, preventing batteries from short-circuiting even after more than 1,000 h of cycling, and the vertical channels enhance the ionic conductivity (2.3 × 10−4 S cm−1 at 30 °C) of the infused polymer electrolyte. All-solid-state lithium-ion batteries fabricated with PI/PEO/LiTFSI solid electrolyte show good cycling performance (200 cycles at C/2 rate) at 60 °C and withstand abuse tests such as bending, cutting and nail penetration. A nanoporous polyimide film filled with a solid polymer electrolyte has high ionic conductivity and high mechanical strength. An all-solid-state battery made with an approximately 10-μm-thick film shows good cyclability at 60 °C and no dendrite formation.

661 citations


Journal ArticleDOI
TL;DR: In this article, a fluorinated orthoformate-based electrolyte was used to prevent dendritic Li formation and minimise Li loss and volumetric expansion in Li-metal batteries.
Abstract: Lithium (Li) pulverization and associated large volume expansion during cycling is one of the most critical barriers for the safe operation of Li-metal batteries. Here, we report an approach to minimize the Li pulverization using an electrolyte based on a fluorinated orthoformate solvent. The solid–electrolyte interphase (SEI) formed in this electrolyte clearly exhibits a monolithic feature, which is in sharp contrast with the widely reported mosaic- or multilayer-type SEIs that are not homogeneous and could lead to uneven Li stripping/plating and fast Li and electrolyte depletion over cycling. The highly homogeneous and amorphous SEI not only prevents dendritic Li formation, but also minimizes Li loss and volumetric expansion. Furthermore, this new electrolyte strongly suppresses the phase transformation of the LiNi0.8Co0.1Mn0.1O2 cathode (from layered structure to rock salt) and stabilizes its structure. Tests of high-voltage Li||NMC811 cells show long-term cycling stability and high rate capability, as well as reduced safety concerns. Parasitic reactions between Li metal and electrolytes need to be mitigated in Li-metal batteries. Here, the authors report the use of a fluorinated orthoformate-based electrolyte, leading to a monolithic solid–electrolyte interphase and subsequently a high-performance Li-metal battery.

512 citations


Journal ArticleDOI
11 Apr 2019-Chem
TL;DR: In this paper, the fundamental understandings and technological innovations in lithium-ion batteries are essential for delivering high energy density, stable cyclability, and cost-effective energy storages with the growing demands in the applications of electrical vehicles and smart grid.

505 citations


Journal ArticleDOI
TL;DR: In this paper, the design of polymeric materials for desired mechanical properties, increased ionic and electronic conductivity and specific chemical interactions is discussed, with a specific focus on silicon, lithium-metal and sulfur battery chemistries.
Abstract: Electrochemical energy storage devices are becoming increasingly important to our global society, and polymer materials are key components of these devices. As the demand for high-energy density devices increases, innovative new materials that build on the fundamental understanding of physical phenomena and structure–property relationships will be required to enable high-capacity next-generation battery chemistries. In this Review, we discuss core polymer science principles that are used to facilitate progress in battery materials development. Specifically, we discuss the design of polymeric materials for desired mechanical properties, increased ionic and electronic conductivity and specific chemical interactions. We also discuss how polymer materials have been designed to create stable artificial interfaces and improve battery safety. The focus is on these design principles applied to advanced silicon, lithium-metal and sulfur battery chemistries. Polymers are ubiquitous in batteries as binders, separators, electrolytes and electrode coatings. In this Review, we discuss the principles underlying the design of polymers with advanced functionalities to enable progress in battery engineering, with a specific focus on silicon, lithium-metal and sulfur battery chemistries.

494 citations


Journal ArticleDOI
TL;DR: The great effect of structure engineering on the performance is discussed in depth, which will benefit the better design ofollow nanostructures to fulfill the requirements of specific applications and simultaneously enrich the diversity of the hollow nanostructure family.
Abstract: Hollow nanostructures have shown great promise for energy storage, conversion, and production technologies Significant efforts have been devoted to the design and synthesis of hollow nanostructures with diverse compositional and geometric characteristics in the past decade However, the correlation between their structure and energy-related performance has not been reviewed thoroughly in the literature Here, some representative examples of designing hollow nanostructure to effectively solve the problems of energy-related technologies are highlighted, such as lithium-ion batteries, lithium-metal anodes, lithium-sulfur batteries, supercapacitors, dye-sensitized solar cells, electrocatalysis, and photoelectrochemical cells The great effect of structure engineering on the performance is discussed in depth, which will benefit the better design of hollow nanostructures to fulfill the requirements of specific applications and simultaneously enrich the diversity of the hollow nanostructure family Finally, future directions of hollow nanostructure design to solve emerging challenges and further improve the performance of energy-related technologies are also provided

325 citations


Journal ArticleDOI
TL;DR: The strategy developed in this work can be generally applied for enhancing the ion storage capacity of metal chalcogenides and other layered materials, making them promising cathodes for challenging multivalent ion batteries.
Abstract: 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 ...

316 citations


Journal ArticleDOI
TL;DR: Cui et al. as discussed by the authors used cryo-electron microscopy to reveal a drastically different solid electrolyte interface nanostructure emerging at 60°C, which maintains mechanical stability, inhibits continuous side reactions and guarantees good cycling stability and low electrochemical impedance.
Abstract: Operations of lithium-ion batteries have long been limited to a narrow temperature range close to room temperature. At elevated temperatures, cycling degradation speeds up due to enhanced side reactions, especially when high-reactivity lithium metal is used as the anode. Here, we demonstrate enhanced performance in lithium metal batteries operated at elevated temperatures. In an ether-based electrolyte at 60 °C, an average Coulombic efficiency of 99.3% is obtained and more than 300 stable cycles are realized, but, at 20 °C, the Coulombic efficiency drops dramatically within 75 cycles, corresponding to an average Coulombic efficiency of 90.2%. Cryo-electron microscopy reveals a drastically different solid electrolyte interface nanostructure emerging at 60 °C, which maintains mechanical stability, inhibits continuous side reactions and guarantees good cycling stability and low electrochemical impedance. Furthermore, larger lithium particles grown at the elevated temperature reduce the electrolyte/electrode interfacial area, which decreases the per-cycle lithium loss and enables higher Coulombic efficiencies. The performance of Li-ion batteries deteriorates at elevated temperatures due to increased activity of electrode materials and parasitic reactions. Here Yi Cui and colleagues report much-improved battery cyclability at 60 °C and use cryo-electron microscopy to shed light on the origin of the phenomenon.

Journal ArticleDOI
TL;DR: Li et al. as discussed by the authors developed a method of forming a uniform lithium sulfide (Li2S) protective layer for suppressing dendrite growth and stabilizing the lithium metal anode.
Abstract: DOI: 10.1002/aenm.201900858 dendrites,[6] guided lithium plating,[7] and nanostructured electrode design.[8] Among all the methods, the focus on solidelectrolyte interphase (SEI) between anode materials and electrolyte is one of the most critical issues. During LMB operation, the SEI that primarily originated from electrolyte decomposition, is easily cracked. This will locally enhance ion flux and promote nonuniform lithium depositing/stripping,[9] resulting in Li dendrites that can trigger internal short circuit and compromise battery safety. Repeated breakdown and repair of SEI during cycling create a vicious cycle which alternates between “uneven stripping/plating and SEI fracture,” brings about continuous loss of active materials and limited battery cycle life. Therefore, an ideal SEI should continuously passivate the anode and prevent the parasitic reactions between reactive anode and electrolyte to address the aforementioned problems in principle.[3] Previous studies have demonstrated several effective artificial SEI to protect lithium metal anode such as polymer,[10] inorganic conductive compounds,[11,12] electrolyte additives,[13,14] and carbonbased materials.[7,15] However, the evolution of SEI during cycling and key mechanisms such as impact of SEI quality on its stability need to be further explored.[16] Herein, we demonstrate a “simultaneous homogeneous and high ionic conductivity” strategy by developing a method of forming a uniform lithium sulfide (Li2S) protective layer for suppressing dendrite growth and stabilizing the lithium metal anode. Although Li2S interfacial layers through soluble electrolyte additives have been studied before,[14,17–20] the work here demonstrates that the elevated temperature (170 °C) and gas phase reaction are critical for the synthesis of a homogenous Li2S coating, which importantly can be used as SEI in carbonate electrolyte system. We reveal the evolution of thus formed Li2S artificial SEI component distribution during battery operation: the uniform and high ionic conductivity protective layer turns into a layered SEI that preserves protective function, rather than into a disordered, broken SEI mainly made up of parasitic reaction products. Simulation results also confirm the critical importance of compositional homogeneity and high ionic conductivity in stabilizing SEI. With this strategy, stable cycles in both high capacity symmetric cells and Li–LiFePO4 full cells were realized. We believe that this practical fabrication method, fundamental design strategy, and understanding on Artificial solid-electrolyte interphase (SEI) is one of the key approaches in addressing the low reversibility and dendritic growth problems of lithium metal anode, yet its current effect is still insufficient due to insufficient stability. Here, a new principle of “simultaneous high ionic conductivity and homogeneity” is proposed for stabilizing SEI and lithium metal anodes. Fabricated by a facile, environmentally friendly, and low-cost lithium solidsulfur vapor reaction at elevated temperature, a designed lithium sulfide protective layer successfully maintains its protection function during cycling, which is confirmed by both simulations and experiments. Stable dendritefree cycling of lithium metal anode is realized even at a high areal capacity of 5 mAh cm−2, and prototype Li–Li4Ti5O12 cell with limited lithium also achieves 900 stable cycles. These findings give new insight into the ideal SEI composition and structure and provide new design strategies for stable lithium metal batteries.

Journal ArticleDOI
TL;DR: This review gives a systematic overview of the state-of-the-art research progress on nanowires for electrochemical energy storage, from rational design and synthesis, in situ structural characterizations, to several important applications in energy storage including lithium-ion batteries, lithium-sulfur batteries, sodium-ION batteries, and supercapacitors.
Abstract: Nanomaterials provide many desirable properties for electrochemical energy storage devices due to their nanoscale size effect, which could be significantly different from bulk or micron-sized materials. Particularly, confined dimensions play important roles in determining the properties of nanomaterials, such as the kinetics of ion diffusion, the magnitude of strain/stress, and the utilization of active materials. Nanowires, as one of the representative one-dimensional nanomaterials, have great capability for realizing a variety of applications in the fields of energy storage since they could maintain electron transport along the long axis and have a confinement effect across the diameter. In this review, we give a systematic overview of the state-of-the-art research progress on nanowires for electrochemical energy storage, from rational design and synthesis, in situ structural characterizations, to several important applications in energy storage including lithium-ion batteries, lithium-sulfur batteries, sodium-ion batteries, and supercapacitors. The problems and limitations in electrochemical energy storage and the advantages in utilizing nanowires to address the issues and improve the device performance are pointed out. At the end, we also discuss the challenges and demonstrate the prospective for the future development of advanced nanowire-based energy storage devices.

Journal ArticleDOI
01 Jan 2019
TL;DR: Cui et al. as mentioned in this paper used density functional theory to investigate the effect of alloying Cu and Sn on the activity and selectivity towards formate, and reported that the designed CuSn3 catalysts by co-electrodeposition exhibit a Faradaic efficiency of 95% toward formate generation at −0.5'V versus RHE.
Abstract: Electrochemical CO2 reduction to formate provides an avenue to reduce globally accelerating CO2 emissions and produce value-added products. Unfortunately, high selectivity in formate electrosynthesis has thus far only been achieved at highly cathodic potentials. Here we use density functional theory to investigate the effect of alloying Cu and Sn on the activity and selectivity towards formate. A theoretical thermodynamic analysis of the reaction energetics suggests that the incorporation of copper into tin could suppress hydrogen evolution and CO production, thus favouring formate generation. Consistent with theoretical trends, the designed CuSn3 catalysts by co-electrodeposition exhibit a Faradaic efficiency of 95% towards formate generation at −0.5 V versus RHE. Furthermore, the catalysts show no degradation over 50 h of operation. In situ Sn L3-edge and Cu K-edge X-ray absorption spectroscopy indicate electron donation from Sn to Cu, which indicates positive oxidation states of Sn in CuSn3 under operating conditions. The electroreduction of carbon dioxide to formate represents a desirable strategy for the production of fuels and commodity chemicals. Now, guided by density functional theory, Cui and colleagues report CuSn3 alloys that exhibit high activity and selectivity for formate production from CO2 electroreduction at potentials as low as −0.5 V versus RHE.

Journal ArticleDOI
TL;DR: The method reported here of decoupling ionic conductivity from mechanical properties opens a promising route to create high-toughness ion transport materials for energy storage applications.
Abstract: The emergence of wearable electronics puts batteries closer to the human skin, exacerbating the need for battery materials that are robust, highly ionically conductive, and stretchable. Herein, we introduce a supramolecular design as an effective strategy to overcome the canonical tradeoff between mechanical robustness and ionic conductivity in polymer electrolytes. The supramolecular lithium ion conductor utilizes orthogonally functional H-bonding domains and ion-conducting domains to create a polymer electrolyte with unprecedented toughness (29.3 MJ m−3) and high ionic conductivity (1.2 × 10−4 S cm−1 at 25 °C). Implementation of the supramolecular ion conductor as a binder material allows for the creation of stretchable lithium-ion battery electrodes with strain capability of over 900% via a conventional slurry process. The supramolecular nature of these battery components enables intimate bonding at the electrode-electrolyte interface. Combination of these stretchable components leads to a stretchable battery with a capacity of 1.1 mAh cm−2 that functions even when stretched to 70% strain. The method reported here of decoupling ionic conductivity from mechanical properties opens a promising route to create high-toughness ion transport materials for energy storage applications. Typically, ion conducting polymers exhibit a trade-off between mechanical robustness and ionic conducting performance. Here, the authors utilize supramolecular chemistry obtaining extremely tough electrolytes with high ionic conductivity and enabling stretchable lithium-ion batteries.

Journal ArticleDOI
TL;DR: In this paper, the authors performed a guided search of materials space with a machine learning (ML)-based prediction model for material selection and density functional theory molecular dynamics (DFT-MD) simulations for calculating ionic conductivity.
Abstract: We discover many new crystalline solid materials with fast single crystal Li ion conductivity at room temperature, discovered through density functional theory simulations guided by machine learning-based methods. The discovery of new solid Li superionic conductors is of critical importance to the development of safe all-solid-state Li-ion batteries. With a predictive universal structure–property relationship for fast ion conduction not well understood, the search for new solid Li ion conductors has relied largely on trial-and-error computational and experimental searches over the last several decades. In this work, we perform a guided search of materials space with a machine learning (ML)-based prediction model for material selection and density functional theory molecular dynamics (DFT-MD) simulations for calculating ionic conductivity. These materials are screened from over 12 000 experimentally synthesized and characterized candidates with very diverse structures and compositions. When compared to a r...

Journal ArticleDOI
TL;DR: With its roll-to-roll compatible fabrication procedure, WGC serves as a highly promising material for the practical realization of Li metal anodes in next-generation high energy density secondary batteries.
Abstract: 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 u...

Journal ArticleDOI
TL;DR: It is revealed that the enhanced lithiophilicity and the increased Li ion diffusion coefficient in aprotic electrolytes at high temperature are essential factors contributing to the dendrite-free Li growth behavior.
Abstract: It is essential to develop a facile and effective method to enhance the electrochemical performance of lithium metal anodes for building high-energy-density Li-metal based batteries. Herein, we explored the temperature-dependent Li nucleation and growth behavior and constructed a dendrite-free Li metal anode by elevating temperature from room temperature (20 °C) to 60 °C. A series of ex situ and in situ microscopy investigations demonstrate that increasing Li deposition temperature results in large nuclei size, low nucleation density, and compact growth of Li metal. We reveal that the enhanced lithiophilicity and the increased Li-ion diffusion coefficient in aprotic electrolytes at high temperature are essential factors contributing to the dendrite-free Li growth behavior. As anodes in both half cells and full cells, the compact deposited Li with minimized specific surface area delivered high Coulombic efficiencies and long cycling stability at 60 °C.

Journal ArticleDOI
TL;DR: The abundant nitrogen species within g-C3 N4 nanosheets can form transient LiN bonds to powerfully stabilize the lithium-ion flux and thus enable a CE over 99% for 900 cycles and smooth deposition at high current densities and capacities, surpassing most previous works.
Abstract: Commercial deployment of lithium anodes has been severely impeded by the poor battery safety, unsatisfying cycling lifespan, and efficiency. Recently, building artificial interfacial layers over a lithium anode was regarded as an effective strategy to stabilize the electrode. However, the fabrications reported so far have mostly been conducted directly upon lithium foil, often requiring stringent reaction conditions with indispensable inert environment protection and highly specialized reagents due to the high reactivity of metallic lithium. Besides, the uneven lithium-ion flux across the lithium surface should be more powerfully tailored via mighty interfacial layer materials. Herein, g-C3 N4 is employed as a Li+ -modulating material and a brand-new autotransferable strategy to fabricate this interfacial layer for Li anodes without any inert atmosphere protection and limitation of chemical regents is developed. The g-C3 N4 film is filtrated on the separator in air using a common alcohol solution and then perfectly autotransferred to the lithium surface by electrolyte wetting during normal cell assembly. The abundant nitrogen species within g-C3 N4 nanosheets can form transient LiN bonds to powerfully stabilize the lithium-ion flux and thus enable a CE over 99% for 900 cycles and smooth deposition at high current densities and capacities, surpassing most previous works.

Journal ArticleDOI
TL;DR: It is discovered that temperature hotspots can induce significant lithium metal growth as compared to the surrounding lower temperature area due to the locally enhanced surface exchange current density.
Abstract: Fast-charging and high-energy-density batteries pose significant safety concerns due to high rates of heat generation. Understanding how localized high temperatures affect the battery is critical but remains challenging, mainly due to the difficulty of probing battery internal temperature with high spatial resolution. Here we introduce a method to induce and sense localized high temperature inside a lithium battery using micro-Raman spectroscopy. We discover that temperature hotspots can induce significant lithium metal growth as compared to the surrounding lower temperature area due to the locally enhanced surface exchange current density. More importantly, localized high temperature can be one of the factors to cause battery internal shorting, which further elevates the temperature and increases the risk of thermal runaway. This work provides important insights on the effects of heterogeneous temperatures within batteries and aids the development of safer batteries, thermal management schemes, and diagnostic tools.

Journal ArticleDOI
22 May 2019-ACS Nano
TL;DR: This method can tolerate a much wider range of heavy-metal pollution in point-of-use water than traditional adsorption methods and can further selectively recover Cu, Cd, and Pb separately, which adds values to theheavy-metal removal process.
Abstract: Treatment of heavy-metal pollution in both point-of-use water and industrial wastewater is critical in protecting human health and the environment. Current methods for heavy-metal treatment in both sources have limitations. For point-of-use water, current methods usually suffer from limited capacity and difficulties in spontaneously removing multiple heavy metals. For industrial wastewater, current methods greatly reduce the value of heavy metal by precipitating them as sludge which requires further treatment. Here we developed an electrochemical method that can treat both low-concentration and high-concentration heavy-metal pollution using either direct current (DC) or alternating current (AC) electrodeposition with graphene-oxide-modified carbon felt electrode (CF-GO). The graphene oxide provides a high density of surface functional groups to assist the electrodeposition. The electrodeposition method showed 2 orders of magnitude higher capacity (>29 g heavy metal for 1 g of graphene oxide) compared with traditional adsorption methods. For low levels of heavy-metal pollution in point-of-use water, DC electrodeposition with a CF-GO electrode can reduce single heavy-metal ion pollution (Cu, Cd, and Pb) as well as multiple ion mixtures to below safe water drinking levels. This method can tolerate a much wider range of heavy-metal pollution in point-of-use water than traditional adsorption methods. For high-level pollution in industrial wastewater, AC electrodeposition can recover >99.9% heavy-metal ions. By tuning the AC frequency and voltage, the electrodeposition method can further selectively recover Cu, Cd, and Pb separately, which adds values to the heavy-metal removal process.

Journal ArticleDOI
TL;DR: A remediation method based on asymmetrical alternating current electrochemistry that achieves high degrees of contaminant removal for different heavy metals at different initial concentrations and enables recycling of soil washing chemicals and eliminates secondary pollution is reported.
Abstract: Soil contamination by heavy metals constitutes an important environmental problem, whereas field applicability of existing remediation technologies has encountered numerous obstacles, such as long operation time, high chemical cost, large energy consumption, secondary pollution, and soil degradation. Here we report the design and demonstration of a remediation method based on a concept of asymmetrical alternating current electrochemistry that achieves high degrees of contaminant removal for different heavy metals (copper, lead, cadmium) at different initial concentrations (from 100 to 10,000 ppm), all reaching corresponding regulation levels for residential scenario after rational treatment time (from 30 min to 6 h). No excessive nutrient loss in treated soil is observed and no secondary toxic product is produced. Long-term experiment and plant assay show the high sustainability of the method and its feasibility for agricultural use. Soil pollution by heavy metals is a problem of global concern, requiring the development of remediation technologies. Here the authors report a method based on asymmetrical alternating current electrochemistry, which enables recycling of soil washing chemicals and eliminates secondary pollution.

Journal ArticleDOI
19 Jun 2019-Joule
TL;DR: In this article, a new strategy utilizing inorganic nanoparticles as a coloring component for scalable brightly colored, infrared-transparent textiles was reported, which showed a high infrared transparency of ∼80% and a passive cooling effect of ∼1.6°C-1.8°C but also exhibit intense visible colors with good stability against washing.

Journal ArticleDOI
20 Mar 2019-Joule
TL;DR: In this paper, a quinone derivative with tailored properties (e.g., oxidation potential, solubility, and electrochemical stability) is added to an electrolyte as a redox mediator.

Journal ArticleDOI
26 Aug 2019-Joule
TL;DR: In this paper, the dynamic single-ion-conductive network (DSN) is proposed as a multifunctional artificial solid-electrolyte interphase (SEI) for Li-metal anodes.

Journal ArticleDOI
17 Apr 2019-Joule
TL;DR: In this article, a red phosphorus (P) nanocomposite has been fabricated, featuring amorphous red P nanodomains embedded in the nanopores of micrometer-scale porous conductive carbon with interior nanoscale void spaces.

Journal ArticleDOI
TL;DR: Vanadium-based compounds have been widely used as electrode materials in aqueous zinc ion batteries (ZIBs) due to the multiple oxidation states of vanadium and their open framework structure.
Abstract: Vanadium-based compounds have been widely used as electrode materials in aqueous zinc ion batteries (ZIBs) due to the multiple oxidation states of vanadium and their open framework structure. Howev...

Journal ArticleDOI
TL;DR: A previously overlooked mechanism by which lithium deposits can corrode on a copper surface is reported, and a Kirkendall-type mechanism is validated through electrochemical analysis.
Abstract: Developing a viable metallic lithium anode is a prerequisite for next-generation batteries. However, the low redox potential of lithium metal renders it prone to corrosion, which must be thoroughly understood for it to be used in practical energy-storage devices. Here we report a previously overlooked mechanism by which lithium deposits can corrode on a copper surface. Voids are observed in the corroded deposits and a Kirkendall-type mechanism is validated through electrochemical analysis. Although it is a long-held view that lithium corrosion in electrolytes involves direct charge-transfer through the lithium-electrolyte interphase, the corrosion observed here is found to be governed by a galvanic process between lithium and the copper substrate-a pathway largely neglected by previous battery corrosion studies. The observations are further rationalized by detailed analyses of the solid-electrolyte interphase formed on copper and lithium, where the disparities in electrolyte reduction kinetics on the two surfaces can account for the fast galvanic process.

Journal ArticleDOI
Emma Laks1, Emma Laks2, Andrew McPherson2, Andrew McPherson1  +156 moreInstitutions (3)
14 Nov 2019-Cell
TL;DR: DLP+, a scalable single-cell whole-genome sequencing platform implemented using commodity instruments, image-based object recognition, and open source computational methods, has been developed and joint analysis over the above features defined clone-specific chromosomal aneuploidy in polyclonal populations.

Journal ArticleDOI
TL;DR: This study illustrates that membrane curvatures induced by nanoscale surface topography can serve as a direct biochemical signal to activate curvature-sensing protein and regulate actin polymerization and mechanotransduction in the intracellular space.
Abstract: Surface topography profoundly influences cell adhesion, differentiation, and stem cell fate control. Numerous studies using a variety of materials demonstrate that nanoscale topographies change the intracellular organization of actin cytoskeleton and therefore a broad range of cellular dynamics in live cells. However, the underlying molecular mechanism is not well understood, leaving why actin cytoskeleton responds to topographical features unexplained and therefore preventing researchers from predicting optimal topographic features for desired cell behavior. Here we demonstrate that topography-induced membrane curvature plays a crucial role in modulating intracellular actin organization. By inducing precisely controlled membrane curvatures using engineered vertical nanostructures as topographies, we find that actin fibers form at the sites of nanostructures in a curvature-dependent manner with an upper limit for the diameter of curvature at ∼400 nm. Nanotopography-induced actin fibers are branched actin nucleated by the Arp2/3 complex and are mediated by a curvature-sensing protein FBP17. Our study reveals that the formation of nanotopography-induced actin fibers drastically reduces the amount of stress fibers and mature focal adhesions to result in the reorganization of actin cytoskeleton in the entire cell. These findings establish the membrane curvature as a key linkage between surface topography and topography-induced cell signaling and behavior.