Layered reduced graphene oxide with nanoscale interlayer gaps as a stable host for lithium metal anodes.
TL;DR: A composite lithium metal anode is reported that exhibits low dimension variation (∼20%) during cycling and good mechanical flexibility and a full-cell battery with a LiCoO2 cathode shows good rate capability and flat voltage profiles.
Abstract: Metallic lithium is a promising anode candidate for future high-energy-density lithium batteries. It is a light-weight material, and has the highest theoretical capacity (3,860 mAh g–1) and the lowest electrochemical potential of all candidates. There are, however, at least three major hurdles before lithium metal anodes can become a viable technology: uneven and dendritic lithium deposition, unstable solid electrolyte interphase and almost infinite relative dimension change during cycling. Previous research has tackled the first two issues, but the last is still mostly unsolved. Here we report a composite lithium metal anode that exhibits low dimension variation (∼20%) during cycling and good mechanical flexibility. The anode is composed of 7 wt% ‘lithiophilic’ layered reduced graphene oxide with nanoscale gaps that can host metallic lithium. The anode retains up to ∼3,390 mAh g–1 of capacity, exhibits low overpotential (∼80 mV at 3 mA cm–2) and a flat voltage profile in a carbonate electrolyte. A full-cell battery with a LiCoO2 cathode shows good rate capability and flat voltage profiles. Volumetric changes during cycling in lithium metal anodes can be largely suppressed by using a lithophilic carbonaceous host.
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TL;DR: The current understanding on Li anodes is summarized, the recent key progress in materials design and advanced characterization techniques are highlighted, and the opportunities and possible directions for future development ofLi anodes in applications are discussed.
Abstract: Lithium-ion batteries have had a profound impact on our daily life, but inherent limitations make it difficult for Li-ion chemistries to meet the growing demands for portable electronics, electric vehicles and grid-scale energy storage. Therefore, chemistries beyond Li-ion are currently being investigated and need to be made viable for commercial applications. The use of metallic Li is one of the most favoured choices for next-generation Li batteries, especially Li-S and Li-air systems. After falling into oblivion for several decades because of safety concerns, metallic Li is now ready for a revival, thanks to the development of investigative tools and nanotechnology-based solutions. In this Review, we first summarize the current understanding on Li anodes, then highlight the recent key progress in materials design and advanced characterization techniques, and finally discuss the opportunities and possible directions for future development of Li anodes in applications.
4,302 citations
TL;DR: This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium growth, summarizing the theoretical and experimental achievements and endeavors to realize the practical applications of lithium metal batteries.
Abstract: The lithium metal battery is strongly considered to be one of the most promising candidates for high-energy-density energy storage devices in our modern and technology-based society. However, uncontrollable lithium dendrite growth induces poor cycling efficiency and severe safety concerns, dragging lithium metal batteries out of practical applications. This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium growth. First, the working principles and technical challenges of a lithium metal anode are underscored. Specific attention is paid to the mechanistic understandings and quantitative models for solid electrolyte interphase (SEI) formation, lithium dendrite nucleation, and growth. On the basis of previous theoretical understanding and analysis, recently proposed strategies to suppress dendrite growth of lithium metal anode and some other metal anodes are reviewed. A section dedicated to the potential of full-cell lithium metal batteries for practical applicatio...
3,812 citations
TL;DR: Research in materials science is contributing to progress towards a sustainable future based on clean energy generation, transmission and distribution, the storage of electrical and chemical energy, energy efficiency, and better energy management systems.
Abstract: Civilization continues to be transformed by our ability to harness energy beyond human and animal power. A series of industrial and agricultural revolutions have allowed an increasing fraction of the world population to heat and light their homes, fertilize and irrigate their crops, connect to one another and travel around the world. All of this progress is fuelled by our ability to find, extract and use energy with ever increasing dexterity. Research in materials science is contributing to progress towards a sustainable future based on clean energy generation, transmission and distribution, the storage of electrical and chemical energy, energy efficiency, and better energy management systems.
2,894 citations
TL;DR: In this paper, the authors highlight the recent progress in high-sulfur-loading Li-S batteries enabled by hierarchical design principles at multiscale, particularly, basic insights into the interfacial reactions, strategies for mesoscale assembly, unique architectures, and configurational innovation in the cathode, anode, and separator.
Abstract: Owing to high specific energy, low cost, and environmental friendliness, lithium–sulfur (Li–S) batteries hold great promise to meet the increasing demand for advanced energy storage beyond portable electronics, and to mitigate environmental problems. However, the application of Li–S batteries is challenged by several obstacles, including their short life and low sulfur utilization, which become more serious when sulfur loading is increased to the practically accepted level above 3–5 mg cm−2. More and more efforts have been made recently to overcome the barriers toward commercially viable Li–S batteries with a high sulfur loading. This review highlights the recent progress in high-sulfur-loading Li–S batteries enabled by hierarchical design principles at multiscale. Particularly, basic insights into the interfacial reactions, strategies for mesoscale assembly, unique architectures, and configurational innovation in the cathode, anode, and separator are under specific concerns. Hierarchy in the multiscale design is proposed to guide the future development of high-sulfur-loading Li–S batteries.
1,364 citations
TL;DR: The Li-S battery is a complex device and its useful energy density is determined by a number of design parameters, most of which are often ignored, leading to the failure to meet commercial requirements, so how to pave the way for reliableLi-S batteries is discussed.
Abstract: Lithium-sulfur (Li-S) batteries have attracted tremendous interest because of their high theoretical energy density and cost effectiveness. The target of Li-S battery research is to produce batteries with a high useful energy density that at least outperforms state-of-the-art lithium-ion batteries. However, due to an intrinsic gap between fundamental research and practical applications, the outstanding electrochemical results obtained in most Li-S battery studies indeed correspond to low useful energy densities and are not really suitable for practical requirements. The Li-S battery is a complex device and its useful energy density is determined by a number of design parameters, most of which are often ignored, leading to the failure to meet commercial requirements. The purpose of this review is to discuss how to pave the way for reliable Li-S batteries. First, the current research status of Li-S batteries is briefly reviewed based on statistical information obtained from literature. This includes an analysis of how the various parameters influence the useful energy density and a summary of existing problems in the current Li-S battery research. Possible solutions and some concerns regarding the construction of reliable Li-S batteries are comprehensively discussed. Finally, insights are offered on the future directions and prospects in Li-S battery field.
1,269 citations
References
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TL;DR: Owing to its unusual electronic spectrum, graphene has led to the emergence of a new paradigm of 'relativistic' condensed-matter physics, where quantum relativistic phenomena can now be mimicked and tested in table-top experiments.
Abstract: Graphene is a rapidly rising star on the horizon of materials science and condensed-matter physics. This strictly two-dimensional material exhibits exceptionally high crystal and electronic quality, and, despite its short history, has already revealed a cornucopia of new physics and potential applications, which are briefly discussed here. Whereas one can be certain of the realness of applications only when commercial products appear, graphene no longer requires any further proof of its importance in terms of fundamental physics. Owing to its unusual electronic spectrum, graphene has led to the emergence of a new paradigm of 'relativistic' condensed-matter physics, where quantum relativistic phenomena, some of which are unobservable in high-energy physics, can now be mimicked and tested in table-top experiments. More generally, graphene represents a conceptually new class of materials that are only one atom thick, and, on this basis, offers new inroads into low-dimensional physics that has never ceased to surprise and continues to provide a fertile ground for applications.
35,293 citations
TL;DR: This study reports an experimental study of a condensed-matter system (graphene, a single atomic layer of carbon) in which electron transport is essentially governed by Dirac's (relativistic) equation and reveals a variety of unusual phenomena that are characteristic of two-dimensional Dirac fermions.
Abstract: Quantum electrodynamics (resulting from the merger of quantum mechanics and relativity theory) has provided a clear understanding of phenomena ranging from particle physics to cosmology and from astrophysics to quantum chemistry. The ideas underlying quantum electrodynamics also influence the theory of condensed matter, but quantum relativistic effects are usually minute in the known experimental systems that can be described accurately by the non-relativistic Schrodinger equation. Here we report an experimental study of a condensed-matter system (graphene, a single atomic layer of carbon) in which electron transport is essentially governed by Dirac's (relativistic) equation. The charge carriers in graphene mimic relativistic particles with zero rest mass and have an effective 'speed of light' c* approximately 10(6) m s(-1). Our study reveals a variety of unusual phenomena that are characteristic of two-dimensional Dirac fermions. In particular we have observed the following: first, graphene's conductivity never falls below a minimum value corresponding to the quantum unit of conductance, even when concentrations of charge carriers tend to zero; second, the integer quantum Hall effect in graphene is anomalous in that it occurs at half-integer filling factors; and third, the cyclotron mass m(c) of massless carriers in graphene is described by E = m(c)c*2. This two-dimensional system is not only interesting in itself but also allows access to the subtle and rich physics of quantum electrodynamics in a bench-top experiment.
18,958 citations
TL;DR: A brief historical review of the development of lithium-based rechargeable batteries is presented, ongoing research strategies are highlighted, and the challenges that remain regarding the synthesis, characterization, electrochemical performance and safety of these systems are discussed.
Abstract: Technological improvements in rechargeable solid-state batteries are being driven by an ever-increasing demand for portable electronic devices. Lithium-ion batteries are the systems of choice, offering high energy density, flexible and lightweight design, and longer lifespan than comparable battery technologies. We present a brief historical review of the development of lithium-based rechargeable batteries, highlight ongoing research strategies, and discuss the challenges that remain regarding the synthesis, characterization, electrochemical performance and safety of these systems.
17,496 citations
TL;DR: Researchers must find a sustainable way of providing the power their modern lifestyles demand to ensure the continued existence of clean energy sources.
Abstract: Researchers must find a sustainable way of providing the power our modern lifestyles demand.
15,980 citations
TL;DR: An improved method for the preparation of graphene oxide (GO) is described, finding that excluding the NaNO(3), increasing the amount of KMnO(4), and performing the reaction in a 9:1 mixture of H(2)SO(4)/H(3)PO(4) improves the efficiency of the oxidation process.
Abstract: An improved method for the preparation of graphene oxide (GO) is described. Currently, Hummers’ method (KMnO4, NaNO3, H2SO4) is the most common method used for preparing graphene oxide. We have found that excluding the NaNO3, increasing the amount of KMnO4, and performing the reaction in a 9:1 mixture of H2SO4/H3PO4 improves the efficiency of the oxidation process. This improved method provides a greater amount of hydrophilic oxidized graphene material as compared to Hummers’ method or Hummers’ method with additional KMnO4. Moreover, even though the GO produced by our method is more oxidized than that prepared by Hummers’ method, when both are reduced in the same chamber with hydrazine, chemically converted graphene (CCG) produced from this new method is equivalent in its electrical conductivity. In contrast to Hummers’ method, the new method does not generate toxic gas and the temperature is easily controlled. This improved synthesis of GO may be important for large-scale production of GO as well as the ...
9,812 citations