An all-solid-state battery with a lithium metal anode is a strong candidate for surpassing conventional lithium-ion battery capabilities. However, undesirable Li dendrite growth and low Coulombic efficiency impede their practical application. Here we report that a high-performance all-solid-state lithium metal battery with a sulfide electrolyte is enabled by a Ag–C composite anode with no excess Li. We show that the thin Ag–C layer can effectively regulate Li deposition, which leads to a genuinely long electrochemical cyclability. In our full-cell demonstrations, we employed a high-Ni layered oxide cathode with a high specific capacity (>210 mAh g−1) and high areal capacity (>6.8 mAh cm−2) and an argyrodite-type sulfide electrolyte. A warm isostatic pressing technique was also introduced to improve the contact between the electrode and the electrolyte. A prototype pouch cell (0.6 Ah) thus prepared exhibited a high energy density (>900 Wh l−1), stable Coulombic efficiency over 99.8% and long cycle life (1,000 times). Solid-state Li metal batteries represent one of the most promising rechargeable battery technologies. Here the authors report an exceptional high-performance prototype solid-state pouch cell made of a sulfide electrolyte, a high-Ni layered oxide cathode and, in particular, a silver–carbon composite anode with no excess Li.

High-energy long-cycling all-solid-state lithium metal batteries enabled by silver–carbon composite anodes

Rechargeable sodium-ion batteries (SIBs), as the most promising alternative to commercial lithium-ion batteries, have received tremendous attention during the last decade. Among all the anode materials for SIBs, metal sulfides/selenides (MXs) have shown inspiring results because of their versatile material species and high theoretical capacity. They suffer from large volume expansion, however, which leads to bad cycling performance. Thus, methods such as carbon modification, nanosize design, electrolyte optimization, and cut-off voltage control are used to obtain enhanced performance. Here, recent progress on MXs is summarized in terms of arranging the crystal structure, synthesis methods, electrochemical performance, mechanisms, and kinetics. Challenges are presented and effective ways to solve the problems are proposed, and a perspective for future material design is also given. It is hoped that light is shed on the development of MXs to help finally find applications for next-generation rechargeable batteries.

Advances and Challenges in Metal Sulfides/Selenides for Next-Generation Rechargeable Sodium-Ion Batteries.

Carbon-oxide and carbon-sulfide nanocomposites have attracted tremendous interest as the anode materials for Li and Na ion batteries. Such composites are fascinating as they often show synergistic effect compared to their singular components. Carbon nanomaterials are often used as the matrix due to their high conductivity, tensile strength, and chemical stability under the battery condition. Metal oxides and sulfides are often used as active material fillers because of their large capacity. Numerous works have shown that by taking one step further into fabricating nanocomposites with rational structure design, much better performance can be achieved. The present review aims to present and discuss the development of carbon-based nanocomposite anodes in both Li ion batteries and Na ion batteries. The authors introduce the individual components in the composites, i.e., carbon matrices (e.g., carbon nanotube, graphene) and metal oxides/sulfides; followed by evaluating how advanced nanostructures benefit from the synergistic effect when put together. Particular attention is placed on strategies employed in fabricating such composites, with examples such as yolk–shell structure, layered-by-layered structure, and composite comprising one or more carbon matrices. Lastly, the authors conclude by highlighting challenges that still persist and their perspective on how to further develop the technologies.

A Review on Design Strategies for Carbon Based Metal Oxides and Sulfides Nanocomposites for High Performance Li and Na Ion Battery Anodes

MoSe2 grown on N,P-co-doped carbon nanosheets is synthesized by a solvothermal reaction followed with a high-temperature calcination. This composite has an interlayer spacing of MoSe2 expanded to facilitate sodium-ion diffusion, MoSe2 immobilized on carbon nanosheets to improve charge-transfer kinetics, and N and P incorporated into carbon to enhance its interaction with active species upon cycling. These features greatly improve the electrochemical performance of this composite, as compared to all the controls. It presents a specific capacity of 378 mAh g−1 after 1000 cycles at 0.5 A g−1, corresponding to 87% of the capacity at the second cycle. Ex situ Raman spectra and high-resolution transmission electron microscopy images confirm that it is element Se, rather than MoSe2, formed after the charging process. The interaction of the active species with modified carbon is simulated using density functional theory to explain this excellent stability. The superior rate capability, where the capacity at 15 A g−1 equals ≈55% of that at 0.5 A g−1, could be associated with the significant contribution of pseudocapacitance. By pairing with homemade Na3V2(PO4)3/C, this composite also exhibits excellent performances in full cells.

MoSe2‐Covered N,P‐Doped Carbon Nanosheets as a Long‐Life and High‐Rate Anode Material for Sodium‐Ion Batteries

Global warming, environmental pollution, and an energy shortage in the current fossil fuel society may cause a severe ecological crisis. Storage and conversion of renewable, dispersive and non-perennial energy from the sun, wind, geothermal sources, water, or biomass could be a promising option to relieve this crisis. Carbon materials could be the most versatile platform materials applied in the field of modern energy storage and conversion. Conventional carbon materials produced from coal and petrochemical products are usually energy intensive or involve harsh synthetic conditions. It is highly desired to develop effective methods to produce carbon materials from renewable resources that have high performance and limited environmental impacts. In this regard, biochar, a bio-carbon with abundant surface functional groups and easily tuned porosity produced from biomass, may be a promising candidate as a sustainable carbon material. Recent studies have demonstrated that biochar-based materials show great application potential in energy storage and conversion because of their easily tuned surface chemistry and porosity. In this review, recent advances in the applications of biochar-based materials in various energy storage and conversion fields, including hydrogen storage and production, oxygen electrocatalysts, emerging fuel cell technology, supercapacitors, and lithium/sodium ion batteries, are summarized, highlighting the mechanisms and open questions in current energy applications. Finally, contemporary challenges and perspectives on how biochar-based materials will develop and, in particular, the fields in which the use of biochar-based materials could be expanded are discussed throughout the review. This review demonstrates significant potential for energy applications of biochar-based materials, and it is expected to inspire new discoveries to promote practical applications of biochar-based materials in more energy storage and conversion fields.

Emerging applications of biochar-based materials for energy storage and conversion

Scrupulous design and fabrication of advanced electrode materials are vital for developing high-performance sodium ion batteries. Herein, we report a facile one-step hydrothermal strategy for construction of a C-MoSe2/rGO composite with both high porosity and large surface area. Double modification of MoSe2 nanosheets is realized in this composite by introducing a reduced graphene oxide (rGO) skeleton and outer carbon protective layer. The MoSe2 nanosheets are well wrapped by a carbon layer and also strongly anchored on the interconnected rGO network. As an anode in sodium ion batteries, the designed C-MoSe2/rGO composite delivers noticeably enhanced sodium ion storage, with a high specific capacity of 445 mAh·g-1 at 200 mA·g-1 after 350 cycles, and 228 mAh·g-1 even at 4 A·g-1; these values are much better than those of C-MoSe2 nanosheets (258 mAh·g-1 at 200 mA·g-1 and 75 mAh·g-1 at 4 A·g-1). Additionally, the sodium ion storage mechanism is investigated well using ex situ X-ray diffraction and transmission electron microscopy methods. Our proposed electrode design protocol and sodium storage mechanism may pave the way for the fabrication of other high-performance metal diselenide anodes for electrochemical energy storage.
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https://link.springer.com/content/pdf/10.1007/s12274-020-3198-6.pdf

Erratum to: Facile fabrication of integrated three-dimensional CMoSe 2 /reduced graphene oxide composite with enhanced performance for sodium storage

Natural biomass-derived carbons for electrochemical energy storage

Smart design and construction of advanced electrodes are crucial for the development of new electrochemical energy storage systems. In this study, we realized hollow 1T MoS2 arrays grown on carbon cloth via a template-free solvothermal method. Hollow MoS2 arrays, with diameters of 400–500 nm, are composed of curved MoS2 nanosheets. This well-designed structure and the introduction of metallic phase MoS2 can improve electrical conductivity, shorten the electron/sodium ion diffusion, and accommodate the large volume changes during cycling. Due to these features, when employed as an anode of sodium ion batteries, the hollow 1T MoS2 array electrode delivers superior sodium ion storage properties, including enhanced cycling stability (576 mA h g−1 after 200 cycles at 200 mA g−1) and high rate capability (276 mA h g−1 at high current density of 2 A g−1). Our study may guide the synthesis of other nanostructured metal sulfide anodes for electrochemical energy applications.

Hollow metallic 1T MoS2 arrays grown on carbon cloth: a freestanding electrode for sodium ion batteries

Lithium-sulfur batteries (LSBs) are considered to be one of the most promising alternatives to the current lithium-ion batteries (LIBs) to meet the increasing demand for energy storage owing to their high energy density, natural abundance, low cost, and environmental friendliness. Despite great success, LSBs still suffer from several problems, including undermined capacity arising from low utilization of sulfur, unsatisfactory rate performance and poor cycling life owing to the shuttle effect of polysulfides, and poor electrical conductivity of sulfur. Under such circumstances, the design/fabrication of porous carbon-sulfur composite cathodes is regarded as an effective solution to overcome the above problems. In this review, different synthetic methods of porous carbon hosts and their corresponding integration into carbon-sulfur cathodes are summarized. The pore formation mechanism of porous carbon hosts is also addressed. The pore size effect on electrochemical performance is highlighted and compared. The enhanced mechanism of the porous carbon host on the sulfur cathode is systematically reviewed and revealed. Finally, the combination of porous carbon hosts and high-profile solid-state electrolytes is demonstrated, and the challenges to realize large-scale commercial application of porous carbon-sulfur cathodes is discussed and future trends are proposed.

Porous Carbon Hosts for Lithium-Sulfur Batteries.

Rational design and synthesis of advanced anode materials are extremely important for high-performance lithium-ion and sodium-ion batteries. Herein, a simple one-step hydrothermal method is developed for fabrication of N-C@MoS2 microspheres with the help of polyurethane as carbon and nitrogen sources. The MoS2 microspheres are composed of MoS2 nanoflakes, which are wrapped by an N-doped carbon layer. Owing to its unique structural features, the N-C@MoS2 microspheres exhibit greatly enhanced lithium- and sodium-storage performances including a high specific capacity, high rate capability, and excellent capacity retention. Additionally, the developed polyurethane-assisted hydrothermal method could be useful for the construction of many other high-capacity metal oxide/sulfide composite electrode materials for energy storage.

Wangjia Tang

Papers

Erratum to: Facile fabrication of integrated three-dimensional CMoSe 2 /reduced graphene oxide composite with enhanced performance for sodium storage

Natural biomass-derived carbons for electrochemical energy storage

Hollow metallic 1T MoS2 arrays grown on carbon cloth: a freestanding electrode for sodium ion batteries

Porous Carbon Hosts for Lithium-Sulfur Batteries.

Nitrogen‐Doped Carbon Embedded MoS2 Microspheres as Advanced Anodes for Lithium‐ and Sodium‐Ion Batteries