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Wearable power supply devices and systems are important necessities for the emerging textile electronic applications. Current energy supply devices usually need more space than the device they power, and are often based on rigid and bulky materials, making them difficult to wear. Fabric-based batteries without any rigid electrical components are therefore ideal candidates to solve the problem of powering these devices. Printing technologies have greater potential in manufacturing lightweight and low-cost batteries with high areal capacity and generating high voltages which are crucial for electronic textile (e-textile) applications. In this review, we present various printing techniques, and battery chemistries applied for smart fabrics, and give a comparison between them in terms of their potential to power the next generation of electronic textiles. Series combinations of many of these printed and distributed battery cells, using electrically conducting threads, have demonstrated their ability to power different electronic devices with a specific voltage and current requirements. Therefore, the present review summarizes the chemistries and material components of several flexible and textile-based batteries, and provides an outlook for the future development of fabric-based printed batteries for wearable and electronic textile applications with enhanced level of DC voltage and current for long periods of time., GRAPHICAL ABSTRACT

Thick electrode is essential for new-generation, high energy density batteries due to its low active/inactive-component ratio. However, current strategies using external forces for improving ion-transport in electrodes often cause low volumetric density, poor mechanical property or less mass loading. Here, high-performance thick electrodes were fabricated through layer-by-layer assembly of two-dimensional (2D), porous nanosheets. The 2D morphology and in-plane pores enable dense electrode structure but with abundant, penetrated ion-transport channels. Various cathode species (NCMs, LCO and LNMC nanosheets) were synthesized by a simple one-pot process. Typically, the mechanically robust NS-NCM electrode reveals rate and cycling performance far better than the commercial NCM counterparts. In particular, the NS-NCM electrode exhibits thickness-independent capacity and excellent volumetric capacity even when the mass loading is scaled up to 320 mg cm−2. This enables it to deliver a superb areal capacity of 45.4 mAh cm−2, surpassing all the reported cathode species and one order of magnitude higher than commercial cathodes. This strategy provides a significant stride in structural design of electrode toward higher areal and volumetric energy density.

The recent advances in wearable technologies had caused a surge in the demand for stretchable Li-ion microbatteries. Herein, a special design based on micropillar electrodes supported on metallic serpentines has been investigated to achieve the fabrication of a functionning device. Besides achieving high areal capacity values like 2.5 ​mA ​h ​cm−2 at C/10 (i.e. 0.07 ​mA ​cm−2), the micropillars make the system reversibly stretchable. Electrochemical tests revealed excellent performance when the stretchable micropower source was subjected to different mechanical strains. Indeed, 73% of the capacity is retained over 100 cycles under 30% strain and all fatigue tests showed that capacity retention remain higher than 70%.

An ultrathick lithium metal anode (LMA) is a prerequisite for developing practical lithium-sulfur (Li-S) batteries that simultaneously meet the requirements of high areal capacity, lean electrolyte, and limited excess Li. Inspired by the electrochemical process for an organosulfur cathode, herein, we reconfigure such a sulfur cathode by using an overlithiation strategy to enable the formation of a high performance LMA. Specifically, an applicable ultrathick LMA is successfully constructed by overlithiating a well-known organosulfur cathode material, sulfurized polyacrylonitrile (SPAN). SPAN contains a polymeric pyridine structure with an outstanding lithium-ion affinity, so that it can act as a lithiophilic matrix. More importantly, a Li

Practical applications of lithium–sulfur (Li–S) batteries have been severely hindered by their low capacity, poor rate performance, and fast capacity degradation, which mainly originate from the no...

The sluggish redox kinetics of polysulfides and difficult oxidation process of Li2S severely hinder practical application of Li–S batteries under high sulfur loading and a low electrolyte dosage. T...

Redox-active organic compounds have become promising electrode materials for the development of more sustainable, economical, and safer batteries. However, their high electrochemical performance is...

High areal capacity and stable Coulombic efficiency (CE) in lithium metal anodes (LMAs) play pivotal roles in developing high-energy-density rechargeable batteries. However, few reported LMAs delivering high and stable CE (>50 cycles) under ultrahigh areal capacity (>10 mA h cm-2). We demonstrated that the simultaneous homogenization of electric field and Li ion flux by using self-supported and surface-oxidized 3D hollow porous copper fibers (3D-HPCFs) can greatly increase both the areal capacity and reversibility of Li deposition. Li can be easily confined inside the hollow porous fibers and within the interspaces among fibers without uncontrollable Li dendrites. The 3D-HPCF-based anode can be deeply cycled at high capacity of 15 mA h cm-2 with average CE of 98.87% for 53 cycles, enabling a practical cell to realize high capacity retentions at a surplus Li of 10%. This work provides a novel Li deposition-regulation technology in LMAs targeting for next generation high-energy-density batteries.

Alkali metals are ideal anodes for high-energy-density rechargeable batteries, while seriously hampered by limited cycle life and low areal capacities. To this end, rationally designed frameworks f...

Continuum simulations provide a cost-effective approach to analyze the effect of geometric structure and dimension in microscale batteries. This allows us to explore how the introduction of 3D vertical structure into the battery design can be used to increase both areal capacity and power density. As we highlight here, continuum simulations contribute toward new insights into optimized geometric parameters, understanding performance of working 3D microscale batteries, and investigations into different physical processes occurring in microscale batteries.

Lithium–sulfur (Li–S) batteries have garnered a lot of attention in the realm of electrochemical energy storage owing to their high energy and low cost. However, the serious polysulfide shuttle effect of the sulfur cathode poses a critical challenge for the development of Li–S batteries with elevated sulfur loadings. In addition, the poor robustness of traditional blade-casting cathodes greatly impedes the practical applications of flexible Li–S cells that display high areal capacity. To address these concerns, we report herein a freestanding hybrid sulfur host via in situ crafting of flexible carbon cloth (CC), vertically grown graphene nanoflakes over CC (G/CC) and metal–organic-framework derived CoP anchored on vertical graphene (CoP@G/CC). The thus-derived sulfur cathodes (CoP@G/CC-S) with a typical sulfur loading of 2 mg cm−2 exhibit outstanding electrochemical performances, including excellent rate capability (930.1 mA h g−1 at 3.0C) and impressive cycling stability (0.03% capacity decay per cycle after 500 cycles at 2.0C). A high areal capacity of 8.81 mA h cm−2 at 0.05C can also be obtained even at an elevated sulfur loading of 10.83 mg cm−2. Furthermore, flexible pouch cells based on the self-supported CoP@G/CC-S showcase favorable rate and cycling performances with high mechanical robustness.

Stretchable electronics stickers that adhere to the human skin and collect biopotentials are becoming increasingly popular for biomonitoring applications. Such stickers include electrodes, stretchable interconnects, silicon chips for processing and communication, and batteries. Here, we demonstrate a material architecture and fabrication technique for a multilayer, stretchable, low-cost, rapidly deployable, and disposable sticker that integrates skin-interfacing hydrogel electrodes, stretchable interconnects, and a Ag2O–Zn (silver oxide–zinc) battery. In addition, the application of a printed biphasic current collector (AgInGa) for the Ag2O–Zn battery is reported for the first time. Surprisingly, and unlike previously reported batteries, the battery capacity increases after being subjected to strain cycles and reaches a record-breaking areal capacity of 6.88 mAh cm–2 post stretch. As a proof of concept, an application of heart rate monitoring is presented. The disposable patch is interfaced with a miniatu...

We report here highly scalable yet stackable C/Fe3C membranes with fast ion-transport micro-/nanochannels and polysulfide-trapping networks via a facile phase-inversion process for high-areal-capac...

The development of flexible lithium-ion batteries (LIBs) with very high areal capacity becomes extremely important in achieving precision medicine due to the limited area of the involved LIB devices. However, the improvement of areal capacity using well-known conventional strategies unavoidably engenders serious polarization and gravimetric specific capacity fading. Herein, we report an entirely new insight into constructing superhigh areal-specific-capacity LIBs by designing an electron/ion dual-conductive macroporous MoS2/C hybrid film. A four-film stacked electrode even with a high mass loading of ∼12.0 mg cm−2 can deliver an unprecedented high areal specific capacity of 7.21 mA h cm−2, almost double that of best material reported to date (4 mA h cm−2). Such film electrode unexpectedly shows a positive linear increase of areal specific capacity versus layer number, but no gravimetric capacity (high value of ∼600 mA h g−1) change. The electrode kinetics studies reveal that such superhigh areal-specific-capacity lithium storage is mainly attributed to excellent ion transport (10−8–10−9 cm2 s−1) and electron transfer (21.3 S cm−1) of three-dimensional macroporous MoS2/C hybrid film. This work demonstrates a new concept of dual-conductive film electrode for the development and application of LIBs with tailorable areal specific capacity.

Summary: Nanostructured alloy-type electrode materials and its composites have shown extraordinary promise for lithium-ion batteries (LIBs) with exceptional gravimetric capacity. However, studies to date are usually limited to laboratory cells with too low mass loading (and thus too low areal capacity) to exert significant practical impact. Herein, by impregnating micrometer-sized SnO2/graphene composites into 3D holey graphene frameworks (HGF), we show that a well-designed 3D-HGF/SnO2 composite anode with a high mass loading of 12 mg cm−2 can deliver an ultra-high areal capacity up to 14.5 mAh cm−2 under current density of 0.2 mA cm−2 and stable areal capacity of 9.5 mAh cm−2 under current density of 2.4 mA cm−2, considerably outperforming those in the state-of-art research devices or commercial devices. This robust realization of high areal capacity defines a critical step to capturing the full potential of high-capacity alloy-type electrode materials in practical LIBs. : Energy Storage; Nanomaterials; Energy Materials Subject Areas: Energy Storage, Nanomaterials, Energy Materials

Lithium sulfur (Li–S) batteries have drawn tremendous interest owing to high energy density, low cost, and environmental friendliness. However, the practical application of Li–S batteries is severely restricted by limited cycle life and high self-discharge rate. Here, for the first time, one papermaking waste, calcium lignosulfonate (LSCa), is employed as a novel ecofriendly multifunctional binder for Li–S batteries. The LSCa electrode retains a capacity of 453 mAh g–1 after 500 cycles at 1C (1C = 1675 mA g–1), and it delivers a high capacity of 571 mAh g–1 even at 5C, the performance of which is much better than that of conventional PVDF electrode. Furthermore, a preferable areal capacity of 4.16 mAh cm–2 after 100 cycles at 0.05C is obtained with a high sulfur loading of 7.64 mg cm–2. These achievements are ascribed to the better adsorption ability to polysulfides, more favorable Li+ transportation, and superior adhesion property of the LSCa, compared to PVDF.

Electrochemical performances of lithium-sulfur batteries have received much progress in recent years. However, their practical deployment encounters challenges with respect to optimizing the cell-fabrication parameters (e.g., amounts of the active material and electrolyte). We present here an “ant-nest-like” cathode substrate with unique architecture to synchronously attain high electrochemical performance and necessary cell-fabrication parameters. The cells with a high sulfur loading (11.5 mg cm−2), a high sulfur content (75 wt%), and a low electrolyte/sulfur ratio (9 μL mg−1) display a high areal capacity and energy density of, respectively, 7 mA h cm−2 and 14 mW h cm−2 with a capacity retention of 70% after 150 cycles. Moreover, the cells exhibit a low self-discharge behavior with a low self-discharge constant of 0.0013 per day and a long rest period of one month. These dynamic and static electrochemical stabilities are attributed to the ant-nest-like structure and low surface area of the cathode substrate that allows, respectively, the accommodation and encapsulation of a high amount of active material and reduces the consumption of electrolyte.

In this work, a freestanding layer-structure Se cathode, composed of alternant barrier layers and active layers, is synthesized via a facile syringe-filtration strategy. With employing the barrier layers simultaneously acting as polyselenide-interception barriers and as highly conductive current collectors, the active layers with 3D porous architecture are endowed with strong polyselenide-trapping capability and fast redox-conversion capability. Such novel Se cathode readily achieves a high Se loading up to 13.5 mg cm−2. The optimized Se cathode with a high Se loading of 4.5 mg cm−2 exhibits high specific capacity/areal capacity (794 mA h g−1/3.6 mA h cm−2), excellent cycling stability (508 mA h g−1@300 cycles), and remarkable rate capability (389 mA h g−1@800 mA g−1), which is superior to conventional Se cathodes. Keywords: Lithium-selenium batteries, Se cathode, Alternant layer structure, Syringe-filtration method, Areal capacity

Nanostructured anode materials have attracted significant attention for lithium-ion batteries (LIBs) due to their high specific capacity. However, their practical application is hindered by the rather low areal capacity in the ultrathin electrode (∼1 mg cm-2). Herein, we propose a new strategy of an all-conductive electrode to fabricate a flexible and free-standing vanadium nitride@N-doped carbon/graphene (VN@C/G) thick electrode. Due to the free-standing structure and absence of any nonconductive components in the electrode, the obtained thick electrode displays excellent cycling performances. With the high mass loading of 5 mg cm-2, VN based electrodes achieve a reversible capacity of 2.6 mAh cm-2 after 200 cycles. Moreover, the all-conductive electrode allows an ultrahigh areal capacity of 7 mAh cm-2 with a high mass loading of 18.3 mg cm-2, which is comparable to state-of-the-art graphite anodes (4 mAh cm-2). Theoretical calculations prove the metallic conductivity of VN, which allows fast charge transport in the thick electrode. This strategy of fabricating all-conductive electrodes shows great potentials to achieve high areal capacity in practical lithium-ion batteries.

We report the preparation of thick ceramic electrodes of the olivine LiFePO4 (LFP) with high mass loading. These electrodes are preparated by means of Powder Extrusion Moulding (PEM), which is a technology easily scalable and cheap. These LFP cathodes are additive-free (neither binder nor extra carbon black) with ~0.5 mm thickness, allowing to develop very high areal capacity (13.7 mA h cm−2). By means of a strict control of sintering process, the carbon coating of the commercial LFP powder remains and the decomposition of the active material is prevented. The optimized self-supported LFP cathode presents good cyclability over 20 cycles at C/10 with no capacity loss. The good electrochemical performance of these novel LFP thick electrodes and their non-flammability make them interesting candidates for both mobile and stationary applications. Authors would like to thank financial support received from Spanish Government MICINN (MAT2016-78362-C4-3-R project), and Madrid regional Government (MATERYENER3CM S2013/MIT-2753 program). They also thank the ICTS-Centro Nacional de Microscopía Electrónica (UCM, Madrid) for instrumental facilities and Dr. Esteban Urones for fruitful discussion about carbon coating. J.-Y. Sanchez acknowledges the CONEX Programme, funding received from Universidad Carlos III de Madrid, the European Union's Seventh Framework Programme for research, technological development and demonstration (Grant agreement n. 600371), Spanish Ministry of Economy and Competitiveness (COFUND2013-40258) and Banco Santander. C. de la Torre-Gamarra would like to thank Universidad Carlos III de Madrid for the mobility grant received for her predoctoral stay at Institut de Chimie et des Matériaux Paris Est (Thiais – France). Publicado

We report on the design of a battery electrode architecture in which ion and electronic transport pathways are contiguous and span the entire volume of a thick, nonplanar electrode. It is shown tha...

Lithium-sulfur (Li-S) batteries have caught tremendous attention as next-generation energy storage systems because of their high theoretical energy density. Nevertheless, the inferior cycle stability of Li-S batteries, mainly caused by the polysulfides migration, constrains their practical application. Herein, a honeycomb-like N, P dual-doped carbon (HNPC) modified separator is adopted to restrain the shuttle effect. Particularly, the comparative experiments to systematically explore the reaction mechanisms between HNPC and polysulfides are performed. The results reveal that HNPC coated separator can effectively immobilize the polysulfides via forming strong N-Li and P-S bonds without sacrificing lithium ions diffusion. As results, the Li-S battery employing the HNPC coated separator exhibits the high initial specific capacity of 1387 mA h g−1 and can retain good capacity of 930 mA h g−1 after 200 cycles at 0.2C, as well as outstanding long-term cycle durability even at high current density of 1.0C with only 0.06% capacity attenuation per cycle for over 900cycles. Moreover, stable and high areal capacity (>3 mA h cm−2) is also achieved under high sulfur areal loading conditions (4 mg cm−2).

Realizing stable cycling performance with high areal capacity is a great challenge for metal-ion battery anodes. Achieveing high areal capacity generally requires the electrode in a high active loading with increased electrode thickness, which is not beneficial to the cycling stability. In this work, novel nanosheet-assembled compact CaV4O9 microflowers are firstly synthesized through a facile method, which exhibit both high areal capacity and stable cycling performance at high mass loadings. The compact microflower structure leads to an increased tap density of the electrode materials, benefiting to reduce the anode thickness at high mass loadings. Meanwhile, the assembled nanosheets maintain the nano-effects of the active materials for favorable electrochemical reactions. These merits together with the intrinsic superior electrochemical properties of CaV4O9, result in the outstanding electrochemical performance. When used as Li-ion battery anodes, a high areal capcity of ~2.5 mAh cm−2 at a high mass loading of 4.4 mg cm−2 is obtained, and a stable cycling over 400 cycles with the areal capacity over 1.5 mAh cm−2 is demonstrated. Besides, the superior electrochemical performance at high mass loadings is also observed for Na storage. These achievements may pave the way for constructing applicable high-capacity and stable anode materials in metal-ion batteries.

For the first time, we successfully synthesize a self-supported Na0.7CoO2 nanosheet arrays via the facile “sodiation and post-calcination” method. Different from the traditional high temperature solid-state technique, this facile strategy can easily maintain the novel construction of the precursor. A mass loading as high as 8 mg cm−2 is achieved for the Na0.7CoO2 electrode with an initial capacity of 145.2 mAh g−1 at 1 C. Most importantly, the corresponding areal capacity for the Na0.7CoO2 electrode is calculated to be 1.16 mAh cm−2. This superb areal capacity is higher than that of the previously reported cathode materials. This special “sodiation and post-calcination” protocol mentioned in this article guarantees the high mass loading of Na0.7CoO2 on Ni foam, providing a straightforward direction for engineering high-areal-capacity cathode materials.

Lithium metal has long been regarded as a promising anode for its high energy density and low reduction potential. However, infinite volume change and undesired lithium dendrite and parasitic reactions still block the practical application of lithium-metal anodes, despite persistent research. To address these tough issues, a self-stabilized solid electrolyte interface (SEI) formed in lithium bis(trifluoromethane sulphonyl)imide-vinylene carbonate electrolyte with high ionic conductivity, mechanical strength, and compact structure is reported for the first time, delivering rapid lithium-ion diffusion and suppressed anode/electrolyte interfacial reactions. This excellent SEI contributes to homogeneous lithium plating/stripping and a constant voltage over 4000 h even under harsh conditions. High rate performance with a current density of 20 mA cm–2 and an areal capacity of 40 mA h cm–2 has also been achieved. The self-stabilized SEI provides a promising strategy to tackle the challenges raised by the intrins...

Summary In the pursuit of high-energy-density batteries, there is tremendous appetite for developing the lithium-sulfur technology with high sulfur loading and content while keeping the electrolyte/sulfur (E/S) ratio low to be competitive with or surpass the current lithium-ion technology. However, very limited studies have focused on keeping these parameters at practically desirable ranges. Here, we present a lithium-sulfur cell with a coaxial-graphene-coated cotton-carbon (CGCC) cathode that displays excellent performance with high sulfur loading (57.6 mg cm −2 ), high sulfur content (75 wt %), and low E/S ratio (4.2 μL mg −1 ) simultaneously. The cell exhibits high areal capacity (31 mA hr cm −2 ) and areal energy density (66 mW hr cm −2 ) that exceed the areal capacity (4 mA hr cm −2 ) and areal energy density (10 mW hr cm −2 ) of a commercial LiCoO 2 cathode with a high capacity-retention rate of 68% over 200 cycles.

Despite their potential to provide high energy densities, lithium–oxygen (Li–O2) batteries are not yet widely used in ultrahigh energy density devices like electric vehicles, owing to various challenges, including poor cyclability, low efficiency, and poor rate capability, especially at high areal mass loading. Even the most promising Li–O2 cells are unsuitable for practical applications, owing to a limited areal mass loading below 1 mg cm–2, resulting in low areal capacity. Here, we demonstrate air cathodes of unprecedentedly high areal capacity at a high rate with sufficient cycle life for pragmatic operation of Li–O2 batteries. A separator-carbon nanotube (CNT) monolith-type cathode of massive loading is prepared to achieve high areal capacity, but the cycle life and round-trip efficiency of CNT-only separator monolith cathodes are limited. The reversible and energy-efficient operation at high areal capacity and a high rate is enabled by adopting RuO2/MnO2 solid catalysts on the CNT (RMCNT). RMCNTs sho...

A three-dimensional hierarchical Ni3Se2 nanorod array (NA) grown in situ on foam Ni is the first to act as a carbon/binder-free electrode of SIBs via a one-step reversible conversion reaction. By a special decomposition–fusion process, the morphology and composition of the NA are regulated to obtain ultrahigh areal capacity, which is three times greater than that reported for other metal selenides.

To obtain a satisfactory rate performance of lithium–sulfur (Li–S) batteries with a high sulfur loading, the vapour induced phase inversion (VIPI) process was used to prepare sponge-like porous electrodes. It is suitable for various solvents, binders and materials on account of phase separation principles and produces electrodes with enhanced adhesive properties, high electrolyte uptake and improved capability in electron/ion transport. As a result, batteries assembled with the VIPIE delivered a high initial discharge capacity of 1171 mA h g−1 and presented a capacity retention of 56.6% within 400 cycles at 0.5C. Additionally, a high discharge capacity of 693 mA h g−1 could be also obtained at 2C due to the facilitated electron/ion transport. An electrode with a high sulfur loading of 19 mg cm−2 could be realized. The 10 mg cm−2 sulfur loaded VIPIE delivered a high capacity of 1300 mA h g−1 at 0.05C (equaling to an areal capacity of 13.0 mA h cm−2) and showed a high capacity retention of 90.7% within 60 cycles at 0.1C.

The commercial application of lithium–selenium (Li–Se) batteries is hampered by low areal capacity, inferior cycling stability and low utilization of Se, in particular at a high Se loading. Here, a facile biotemplating method with the assistance of a supercritical CO2 (SC–CO2) technique has been developed to construct a unique 3D porous SiOC/Se cathode with a high Se loading for Li–Se batteries with high areal capacity and a long cycling life. An SiOC/Se cathode derived from rice husks achieved an extremely high initial areal capacity of 8.1 mA h cm−2 at 0.1C at an Se loading of 8 mg cm−2, which is the highest Se loading reported thus far. After 200 cycles, the reversible areal capacity remained at 4.1 mA h cm−2 together with a capacity retention of 90% (vs. 4.8 mA h cm−2 in the 2nd cycle). This excellent performance at a record-breaking Se loading in comparison with earlier Li–Se batteries is attributed to the unique 3D porous conductive network and Si–O–C units set in the porous carbon matrix, which provided continuous electron/ion pathways, enhanced structural stability and strong chemical adsorption for trapping Se and Li2Se, as well as the uniform distribution of Se infiltrated via the SC–CO2 strategy. This cathode with an ultrahigh Se loading is strongly expected to pave the way for the practical implementation of Li–Se batteries with a high energy density in large-scale energy storage systems.

In this work, we developed a renewable wood-derived cathode with well-aligned elongated microchannels for high-performance Li–O2 batteries. The cathode was obtained from natural wood following carbonization, activation, and then loading of RuO2 nanoparticles (4.15 wt%) as catalysts (RuO2/WD-C). The cathode has a three-dimensional, high stability carbon matrix, uniformly anchored catalysts, and well-aligned porous microchannels. As a result, the specific areal capacity of the assembled batteries exceeds 8 mA h cm−2 and the charge terminal potential is lower than 3.8 V at 0.1 mA cm−2. The energy efficiency was improved up to 91.9% and exceeded 87.1% after 100 cycles (curtailed capacity of 0.5 mA h cm−2 at 0.2 mA cm−2). Furthermore, the RuO2/WD-C cathode can be fully regenerated from a deep discharge–charge cycle or 100 curtailed-capacity cycles by simply washing with water. The areal capacity of the regenerated RuO2/WD-C cathode is comparable to the performance of the initial cathode. The cut-off voltage was above 2.6 V following 200 cycles. Even when regenerated for the second time, the RuO2/WD-C cathode still demonstrated almost the same high performance as the initial one, indicating its high stability and excellent renewability.

Constructing high-areal-capacity anodes with high loading for Li-ion batteries is still an enormous challenge, due to the drastic volume change of large-capacity anode materials during cycling. The conventional PVDF binder system fails to withstand the degradation of high-loading electrodes. Therefore, advanced binders are urgently required. Herein, for the first time, the guar gum (GG) biopolymer has been exploited as a robust binder for micro-sized ZnCo2O4 (ZCO) anode materials. Because of its robust mechanical properties and strong interactions with ZCO, the cycling stability of the ZCO anode has been significantly improved with a capacity of 412 mA h g−1 after 600 cycles at 1200 mA g−1. More importantly, the ZCO can act as a “crosslinking agent” to in situ form a robust network with GG, which efficiently maintains the electrode structure stability. Hence, a ZCO anode with an ultrahigh loading of 6.73 mg cm−2 can be achieved and deliver a high areal capacity of 5.6 mA h cm−2. Simultaneously, benefiting from the high tap density of micro-ZCO, the ZCO anode gives a high volumetric capacity of 1179 mA h cm−3. This study will make a significant contribution to accelerating the progress of designing high-areal-capacity anodes.

The rational design of cathode hosts with superior polysulfide (PS) confinement properties, excellent Li+/e− transport and improved cyclability is of the utmost importance for high-areal-capacity lithium–sulfur (Li–S) batteries. Herein, multi-functional nanowall arrays (MNWAs) combining the aforementioned properties are fabricated to improve the electrochemical performance of Li–S batteries with high areal sulfur loadings. The integrated conductive networks and top-down vertically aligned Li+ transport channels are beneficial to Li+/e− transport, resulting in high rate performance with a discharge capacity of 620 mA h g−1 at a high current density of 9.6 mA cm−2 for 4 mg cm−2 sulfur-loaded S/MNWA electrodes. Additionally, the strong PS shuttling suppression via the synergetic effects of physical confinement and chemical adsorption leads to Li–S batteries with a sulfur loading of 10 mg cm−2 capable of delivering a high areal capacity of 12.4 mA h cm−2 with a high capacity retention of nearly 85% for over 100 cycles. What's more, the Li–S batteries assembled with 4 mg cm−2 sulfur-loaded S/MNWA electrodes show an ultra-low capacity decay of 0.07% per cycle over 400 cycles at 3.2 mA cm−2.

Rational design and scalable construction of sulfur cathodes with high areal capacity and suppressed shuttle effect are challenging for real Li-S application. Herein, laser-induced micro-explosive techniques were firstly demonstrated as high-efficient polysulfide mediator for Li-S batteries, in which unique hierarchical structure (nitrogen-doped porous carbon (LNPCs) skeletons uniformly decorated with metal oxide nanoparticles) were designed and constructed. The as-assembled nitrogen-doped porous carbons decorated with ZnO nanoparticles (LNPCs-ZnO) hybrids cathode perform exceptionally high discharge capacity of 1184.9 mAh g−1 at 0.5C and excellent rate discharge capacity of 716.1 mA h g−1 at 3C, as well as a remarkable cycling performance (a low-capacity decay rate of 0.31% per cycle at 0.5C upon 1000 cycles). Moreover, impressive areal sulfur loading up to 6.7 mg cm−2 leads to a high initial areal capacity of 6.36 mAh cm−2 and excellent cycling stability at 0.2C. The DFT calculations propose that the intrinsic interaction and the rapid catalytical effects play the key role in suppressing the shuttling effect of LiPSs. This work provides new insights for novel structure design and opens up a potential route to construct Li-S batteries with high areal sulfur loadings for their practical applications.

Nanoarchitectures of ternary NiCo2S4 are desirable for the development of advanced high-performance supercapacitors. Herein, we demonstrate a simple solvothermal synthesis procedure for a fern-like nanoarchitecture of NiCo2S4 on Ni foam. The electrode exhibits a good areal capacity of approximately 1.55F cm−2 at a current density of 10 mA cm−2, while the ASC device exhibits an areal capacity of approximately 1.02 F cm−2 at 12 mA cm−2 and retention of 75.3% over 8000 charge–discharge cycles.

In this work, we report a simple method to fabricate the hierarchical three-dimensional CuCo2O4@Ni(OH)2 hybrid nanostructures on Ni foam for supercapacitors. The highly mesoporous and interconnected CuCo2O4 nanoflakes are ideal scaffolds for loading electroactive Ni(OH)2 shell nanosheets, which significantly boost the energy storage efficiency of the integrated system. The optimized CuCo2O4@Ni(OH)2 hybrid electrode delivers a high areal capacity of 439 μAh/cm2 at 2 mA/cm2 and a good rate capability of 82.7% at 80 mA/cm2. In light of these merits, a hybrid supercapacitor (HSC) has been further assembled. The HSC device displays simultaneously high energy and power densities (48 Wh/kg at 468 W/kg, and 34 Wh/kg at 9145 W/kg), as well as good long-term cycling stability. After charging for a short time, two HSC devices connected in series can drive LEDs with different colors efficiently, suggesting the great potential of this hybrid material toward practical applications as advanced electrodes for high-performance HSC devices.

To meet the increasing demand of flexible and wearable electronic devices, a novel injection molding method is established to prepare flexible electrodes with controllable shapes such as film, bowl, wire, etc. It overcomes the materials limitation for traditional methods and could easily create flexible and shapeable electrodes based on 0-D active materials, even with ultra-high loadings and excellent electrochemical performance. Taking flexible and shapeable S/C electrodes as a model, sulfur loadings 24 mg cm−2 based on 30 nm S/C particles are, for the first time, successfully achieved. It can deliver ultra-high an areal capacity of 27.1 mA h cm−2 and a capacity retention of 64.1% after 100 cycles with low electrolyte to sulfur ratio (E/S) of 5.3 µL mg−1. In addition, flexible and shapeable Li-ion battery electrodes based on 17 mg cm−2 0-D Li3V2(PO4)3 (LVP) electrode could also be obtained, achieving excellent C-rate performance and cycling stability, which is 94 mA h g−1 at 5C and nearly 100% capacity retention at 1C during 100 cycles. The results provided a versatile and universal way to create flexible and shapeable electrodes for a variety of energy storage devices.

The search for an appropriate flexible cathode is pivotal to expediting the development of flexible and foldable lithium-ion batteries (LIBs). Herein, we demonstrate a simple and scalable synthesis of hierarchical V2O5 nanosheet arrays on polydopamine (PDA)-decorated carbon cloth with strong combination between them, which then directly applied as flexible cathode for LIBs. We found this flexible cathode with a loading mass of 2.1 mg cm−2 can deliver a high specific capacity of 120 mAh g−1 even at 15C (1C = 300 mA g−1) and maintain a long-term cycling stability, i.e. simply 0.30% capacity loss per cycle at 2C for 100 cycles without morphology change. More importantly, the corresponding areal capacity can reach as high as 560 μAh cm−2 at 210 μA cm−2, favorably comparing with the-state-of-art flexible cathode reported to date. Additionally, a flexible LIBs full cell has been assembled, exhibiting high mechanical strength and superior electrochemical performances.

We report the highly stable galvanostatic cycling of lithium metal (Li) electrodes in a symmetrical Li|electrolyte solution|Li coin-cell configuration at a high rate and high areal capacity using fluoroethylene carbonate (FEC)-based electrolyte solutions [1 M LiPF6 in FEC/dimethyl carbonate (DMC)]. The FEC-based electrolyte solution shows cycling behavior that is markedly better than that observed for the cells cycled with an ethylene carbonate (EC)-based electrolyte solution (1 M LiPF6 in EC/DMC). With FEC-based electrolyte solution, Li|Li cells can be cycled at 2 mA cm–2 with an areal capacity of 3.3 mAh cm–2 for more than 1100 cycles, and full Li|LiNi0.6Co0.2Mn0.2O2 (NMC) cells with high areal loading cathode demonstrate stable cycling with the same capacity during 90 cycles. An increase in areal capacity up to 6 mA h cm–2 does not affect the shape of the voltage profile of the symmetric Li|Li cells. The reason for this high performance is the formation of a stable and efficient solid electrolyte inter...

peer-reviewed The full text of this article will not be available in ULIR until the embargo expires on the 23/07/2021 Silicon nanowires (Si NWs) have been identified as an excellent candidate material for the replacement of graphite in anodes, allowing for a significant boost in the capacity of lithium‐ion batteries (LIBs). Herein, high‐density Si NWs are grown on a novel 3D interconnected network of binary‐phase Cu‐silicide nanofoam (3D CuxSiy NF) substrate. The nanofoam facilitates the uniform distribution of well‐segregated and small‐sized catalyst seeds, leading to high‐density/single‐phase Si NW growth with an areal‐loading in excess of 1.0 mg cm−2 and a stable areal capacity of ≈2.0 mAh cm−2 after 550 cycles. The use of the 3D CuxSiy NF as a substrate is further extended for Al, Bi, Cu, In, Mn, Ni, Sb, Sn, and Zn mediated Si NW growth, demonstrating the general applicability of the anode architecture.

Three dimensional (3D) hedgehog-like Ge nanoelectrodes coated on patterned Si substrate are successfully fabricated through the facile chemical vapor deposition (CVD) process. The 3D Si substrate with enlarged surface area and the abundant Ge shell electrode configuration are together favorable to enhance the lithiation/delithiation kinetics during cycling. Impressively, the optimized 3D Si@hedgehog-like Ge (Si@H-Ge) NRs composites anodes embrace high reversible areal capacity and superior rate capability when employed as anode material for 3D Si based lithium ion microbatteries (LIMBs). Keywords: 3D, Ge, Anode, Cyclability, Lithium ion microbattery

Self-supported electrodes represent a novel architecture for better performing lithium ion batteries. However, lower areal capacity restricts their commercial application. Here, we explore a facial strategy to increase the areal capacity without sacrificing the lithium storage performance. A hierarchical CuO–Ge hybrid film electrode will not only provide high areal capacity but also outstanding lithium storage performance for lithium ion battery anode. Benefiting from the favorable structural advance as well as the synergic effect of the Ge film and CuO NWs array, the hybrid electrode exhibits a high areal capacity up to 3.81 mA h cm−2, good cycling stability (a capacity retention of 90.5% after 150 cycles), and superior rate performance (77.4% capacity remains even when the current density increased to 10 times higher). Published version

ZnO is considered to be one of the promising anode materials for lithium-ion batteries, but the poor electronic conductivity and large volume variation during lithium-ion extraction and insertion process of ZnO seriously hinders its commercial application in lithium-ion batteries (LIBs). In this study, we synthesized a novel self-supporting porous ZnO nanobelt (PZB) arrays on Zn foils, in which Zn foils can be directly used as current collectors to promote electrically connection between the active materials and the current collectors. Furthermore, the well-aligned ZnO nanobelts have a thin thickness and uniform porous structure, which endue it well improved electrochemical performance. The PZB anodes display a high areal capacity of 5.91 mAh cm-2 at current density of 0.5 mA cm-2 at room temperature, and deliver an areal capacity of 1.73 mAh cm-2 at -20 °C, indicating its excellent application potential especially at low temperatures, and it makes the porous ZnO nanobelts a practical anode material for lithium-ion batteries.

Li–S batteries with a high theoretical capacity are considered as the most promising candidate to satisfy the increasing demand for batteries with a high areal capacity. However, the low sulfur loading (

A Li–S battery based on a novel device structure was proposed, which showed a very high areal capacity of ∼60 mA h cm−2. The high-capacity Li–S battery was also found to retain 75.7% initial capacity after 140 cycles at 90 mA g−1.