Sodium‐ion batteries (SIBs) have emerged as an alternative technology because of their merits in abundance and cost. Realizing their real applications, however, remains a formidable challenge. One is that among the limitations of anode materials, the alloy‐type candidates tolerate fast capacity fading during cycling. Here, a 3D framework superstructure assembled with carbon nanobelt arrays decorated with a metallic bismuth (Bi) nanospheres coated carbon layer by thermolysis of Bi‐based metal–organic framework nanorods is synthesized as an anode material for SIBs. Due to the unique structural superiority, the anode design promotes excellent sodium‐storage performance in terms of high capacity, excellent cycling stability, and ultrahigh rate capability up to 80 A g−1 with a capacity of 308.8 mAh g−1. The unprecedented sodium‐storage ability is not only attributed to the unique hybrid architecture, but also to the production of a homogeneous and thin solid electrolyte interface layer and the formation of uniform porous nanostructures during cycling in the ether‐based electrolyte. Importantly, deeper understanding of the underlying cause of the performance improvement is illuminated, which is vital to provide the theoretical basis for application of SIBs.

Integrating Bi@C Nanospheres in Porous Hard Carbon Frameworks for Ultrafast Sodium Storage

Pore-structure design with increased ion-diffusion ability is usually regarded as an effective strategy to improve K-storage performance in hard carbon (HC). However, the relationship between porous structure and K+ migration behavior remains unclear and requires further exploration. Herein, a series of chemically activated hard carbon spheres (denoted as AHCSs) with controllable micro/mesopores structure are successfully synthesized to explore intercorrelation between micro/mesopores and K migration behavior. The experimental results indicate AHCSs have two different K+ storage ways, that is, adsorption behavior at high potential region and intercalation process at low potential region. These behaviors are closely related to the pores structure evolution: the micropores afford extra active sites for efficient K-ions adsorption, and therefore positive correlation between micropores and adsorption-contributed capacity is confirmed; the mesopores permit more K-ions intercalation/deintercalation by offering adequate pathways, and as a result positive correlations between mesopores and intercalation-contributed capacity as well as initial Coulombic efficiency are revealed. All these together contribute to achieving excellent reversible capacity, and exceptional rate capability with an ultra-long cycle lifespan in PIBs, and simultaneously exhibit a high energy density as well as considerable cycling stability for potassium-ion full cells. These results promote a fundamental understanding of K+ migration behaviors in hard carbon.

Unraveling the Intercorrelation Between Micro/Mesopores and K Migration Behavior in Hard Carbon.

Free‐standing and foldable electrodes with high energy density and long lifespan have recently elicited attention on the development of lithium‐ion batteries (LIBs) for flexible electronic devices. However, both low energy density and slow kinetics in cycling impede their practical applications. In this work, a free‐standing and binder‐free N, O‐codoped 3D vertical graphene carbon nanofibers electrode with ultra‐high silicon content (VGAs@Si@CNFs) is developed via electrospinning, subsequent thermal treatment, and chemical vapor deposition processes. The as‐prepared VGAs@Si@CNFs electrode exhibits excellent conductivity and flexibility because of the high graphitized carbon nanofiber network and abundant vertical graphene arrays. Such 3D all‐carbon architecture can be fabulous for providing a conductive and mechanically robust network, further improving the kinetics and restraining the volume expansion of Si NPs, especially with an ultra‐high Si content (>90 wt%). As a result, the VGAs@Si@CNFs composite demonstrates a superior specific capacity (3619.5 mAh g−1 at 0.05 A g−1), ultralong lifespan, and outstanding rate capability (1093.1 mAh g−1 after 1500 cycles at 8 A g−1) as a free‐standing anode for LIBs. It is believed that this work offers an exciting method for developing free‐standing and high‐energy‐density electrodes for other energy storage devices.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202104685

Nitrogen, Oxygen‐Codoped Vertical Graphene Arrays Coated 3D Flexible Carbon Nanofibers with High Silicon Content as an Ultrastable Anode for Superior Lithium Storage

Secondary batteries have been widespread in the daily life causing an ever‐growing demand for long‐cycle lifespan and high‐energy alkali‐ion batteries. As an essential constituent part, electrode materials with superior electrochemical properties play a vital role in the battery systems. Here, an outstanding electrode of yolk–shell ZnS@C nanorods is developed, introducing considerable void space via a self‐sacrificial template method. Such carbon encapsulated nanorods moderate integral electronic conductivity, thus ensuring rapid alkali‐ions/electrons transporting. Furthermore, the porous structure of these nanorods endows enough void space to mitigate volume stress caused by the insertion/extraction of alkali‐ions. Due to the unique structure, these yolk–shell ZnS@C nanorods achieve superior rate performance and cycling performance (740 mAh g−1 at 1.0 A g−1 after 540 cycles) for lithium‐ion batteries. As a potassium‐ion batteries anode, they achieve an ultra‐long lifespan delivering 211.1 mAh g−1 at 1.0 A g−1 after 5700 cycles. The kinetic analysis reveals that these ZnS@C nanorods with considerable pseudocapacitive contribution benefit the fast lithiation/delithiation. Detailed transmission electron microscopy (TEM) and X‐ray diffraction (XRD) analyses indicate that such yolk–shell ZnS@C anode is a typical reversible conversion reaction mechanism accomplished by alloying processes. This rational design strategy opens a window for the development of superior energy storage materials.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202200247

Self‐Sacrifice Template Construction of Uniform Yolk–Shell ZnS@C for Superior Alkali‐Ion Storage

Potassium‐ion batteries (KIBs) are considered as the potential energy storage devices due to the abundant reserves and low cost of potassium. In the past decade, research on KIBs has generally focused on electrode materials. However, since electrolytes also play a key role in determining the cell performance, this review summarizes recent advances in KIB electrolytes and design strategies. Specifically, the review includes five parts. First, the organic liquid electrolyte is the most widely used type for KIBs. Its two major components, salts and solvents, have a huge impact on the formation of the solid electrolyte interphase and the performance of KIBs. Changes in salts/solvents, the introduction of additives, and the concentration increase all have a positive effect on organic liquid electrolytes. Second, the design of water‐in‐salt electrolytes can effectively widen the narrow electrochemical stability window of aqueous electrolytes. Third, despite the appealing properties, the ionic liquid electrolytes have not been widely applied due to its high cost. Fourth, the solid‐state electrolytes have drawn much attention due to high safety, and current research has been working on improving their ionic conductivity at room temperature. Lastly, perspectives are provided to support the future development of suitable electrolytes for high‐performance KIBs.

Recent Advances in Electrolytes for Potassium‐Ion Batteries

SnS has been extensively investigated as a potential anode material in potassium-ion batteries (PIBs) for its high theoretical capacity. Nonetheless, it suffers a limited cyclic lifespan owing to its poor electronic conductivity and huge volume expansion. This work proposed a facile approach where SnS nanocrystals are confined in the walls of hollow multichannel carbon nanofibers (denoted SnS@HMCFs) to tackle the issues above. In contrast to previous studies, impregnated ultrafine SnS nanocrystals in HMCFs compactly can increase the SnS loading number per unit area of the carbon matrix. Furthermore, the unique hollow multichannel carbon nanofibers are used as a robust carrier to uniformly distribute the SnS nanocrystals. This can significantly accelerate K+/electron transport, resulting in large specific capacity, outstanding rate performance, and steady cycling property for PIBs. High reversible capacities of 415.5 mAh g−1 at 0.1 A g−1 after 300 cycles and 245.5 mAh g−1 at 1 A g−1 after 1000 cycles are retained, suggesting great potential of SnS@HMCFs as a negative electrode material for PIBs. Additionally, when the SnS@HMCF anode is assembled with the KVPO4F cathode, the obtained full cell shows a large discharge capacity of 165.3 mAh g−1 after 200 cycles at 0.1 A g−1.

Confining ultrafine SnS nanoparticles in hollow multichannel carbon nanofibers for boosting potassium storage properties

Sn4P3 nanoparticles confined in multilayer graphene sheets as a high-performance anode material for potassium-ion batteries

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Confining ultrafine SnS nanoparticles in hollow multichannel carbon nanofibers for boosting potassium storage properties

Sn4P3 nanoparticles confined in multilayer graphene sheets as a high-performance anode material for potassium-ion batteries