Black phosphorus with a superior theoretical capacity (2596 mAh g-1) and high conductivity is regarded as one of the powerful candidates for lithium-ion battery (LIB) anode materials, whereas the severe volume expansion and sluggish kinetics still impede its applications in LIBs. By contrast, the exfoliated two-dimensional phosphorene owns negligible volume variation, and its intrinsic piezoelectricity is considered to be beneficial to the Li-ion transfer kinetics, while its positive influence has not been discussed yet. Herein, a phosphorene/MXene heterostructure-textured nanopiezocomposite is proposed with even phosphorene distribution and enhanced piezo-electrochemical coupling as an applicable free-standing asymmetric membrane electrode beyond the skin effect for enhanced Li-ion storage. The experimental and simulation analysis reveals that the embedded phosphorene nanosheets not only provide abundant active sites for Li-ions, but also endow the nanocomposite with favorable piezoelectricity, thus promoting the Li-ion transfer kinetics by generating the piezoelectric field serving as an extra accelerator. By waltzing with the MXene framework, the optimized electrode exhibits enhanced kinetics and stability, achieving stable cycling performances for 1,000 cycles at 2 A g-1, and delivering a high reversible capacity of 524 mAh g-1 at - 20 ℃, indicating the positive influence of the structural merits of self-assembled nanopiezocomposites on promoting stability and kinetics.

Tungsten disulfide (WS2) is considered as a promising anode material for high-performance lithium-ion batteries (LIBs) result from its inherent characteristics such as high theoretical capacity, large interlayer spacing and weak interlayer Van der Waals force. Nevertheless, WS2 has the drawbacks of easy agglomeration, severe volume expansion and high Li+ migration barrier, which lead to rapid capacity degradation and imperfect rate ability. In this work, a novel two-dimensional (2D) hierarchical composite (Ti3C2/WS2) consisting of WS2 nanosheets vertically grown on titanium carbide (Ti3C2) nanosheets is prepared. Thanks to this distinctive hierarchical structure and synergy between WS2 and Ti3C2, the Ti3C2/WS2 composite demonstrates exceptional electrochemical performance in LIBs. In addition, we investigate the effect of the mass proportion of WS2 in Ti3C2/WS2 composite on the electrochemical performance, and find that the optimal mass ratio of WS2 is 60%. As expected, the optimal electrode exhibits a high specific capacity (650 mAh/g at 0.1 A/g after 100 cycles) and ultra-long cycle stability (400 mAh/g at 1.0 A/g after 5000 cycles).

The rational design of the heterogeneous interfaces enables precise adjustment of the electronic structure and optimization of the kinetics for electron/ion migration in energy storage materials. In this work, the built-in electric field is introduced to the iron-based anode material (Fe2O3@TiO2) through the well-designed heterostructure. This model serves as an ideal platform for comprehending the atomic-level optimization of electron transfer in advanced lithium-ion batteries (LIBs). As a result, the core-shell Fe2O3@TiO2 delivers a remarkable discharge capacity of 1342 mAh g-1 and an extraordinary capacity retention of 82.7% at 0.1 A g-1 after 300 cycles. Fe2O3@TiO2 shows an excellent rate performance from 0.1 A g-1 to 4.0 A g-1. Further, the discharge capacity of Fe2O3@TiO2 reached 736 mAh g-1 at 1.0 A g-1 after 2000 cycles, and the corresponding capacity retention is 83.62%. The heterostructure forms a conventional p-n junction, successfully constructing the built-in electric field and lithium-ion reservoir. The kinetic analysis demonstrates that Fe2O3@TiO2 displays high pseudocapacitance behavior (77.8%) and fast lithium-ion reaction kinetics. The capability of heterointerface engineering to optimize electrochemical reaction kinetics offers novel insights for constructing high-performance iron-based anodes for LIBs.

Schottky heterostructures have significant advantages for exciting charge transfer kinetics at material interfaces. In this work, endogenous Nb2CTx/Nb2O5 Schottky heterostructures with a large active surface area were constructed using an in-situ architectural strategy. The semiconductor Nb2O5 has a low work function, and during the construction of Nb2CTx/Nb2O5 Schottky heterostructures, there was an interfacial electron transfer, which resulted in a built-in electric field. The electrochemical reaction kinetics of Nb2CTx/Nb2O5 Schottky heterostructures were enhanced due to the rapid transfer of charge driven by the electric field. The Nb2CTx/Nb2O5 Schottky heterostructures have a large active surface area, which contributes to excellent electrolyte diffusion kinetics. Therefore, Nb2CTx/Nb2O5 Schottky heterostructures have excellent lithium-ion storage capacity with 575 mAh/g after 200 cycles at 0.10 A/g, and 290 mAh/g after 1000 cycles at 2.00 A/g, without capacity fading. Furthermore, in-situ X-ray diffraction and ex-situ X-ray photoelectron spectroscopy analyses reveal the mechanisms for structure evolution and lithium-ion storage optimization of Nb2CTx/Nb2O5 Schottky heterostructures during the electrochemical reaction. The construction of Schottky heterostructures with excited charge transport kinetics provides a novel idea for optimizing the lithium-ion storage activity of MXenes materials.

A two-dimensional (2D) silicene-germanene alloy, siligene (SixGey), a single-phase material, has attracted increased attention due to its two-elemental low-buckled composition and unique physics and chemistry. This 2D material has the potential to address the challenges caused by low electrical conductivity and the environmental instability of corresponding monolayers. Yet, the siligene structure was studied in theory, demonstrating the material\'s great electrochemical potential for energy storage applications. The synthesis of free-standing siligene remains challenging and therefore hinders the research and its application. Herein we demonstrate nonaqueous electrochemical exfoliation of a few-layer siligene from a Ca1.0Si1.0Ge1.0 Zintl phase precursor. The procedure was conducted in an oxygen-free environment applying a -3.8 V potential. The obtained siligene exhibits a high quality, high uniformity, and excellent crystallinity; the individual flake is within the micrometer lateral size. The 2D SixGey was further explored as an anode material for lithium-ion storage. Two types of anode have been fabricated and integrated into lithium-ion battery cells, namely, (1) siligene-graphene oxide sponges and (2) siligene-multiwalled carbon nanotubes. The as-fabricated batteries both with/without siligene exhibit similar behavior; however there is an increase in the electrochemical characteristics of SiGe-integrated batteries by 10%. The corresponding batteries exhibit a 1145.0 mAh·g-1 specific capacity at 0.1 A·g-1. The SiGe-integrated batteries demonstrate a very low polarization, confirmed by their good stability after 50 working cycles and a decrease in the solid electrolyte interphase level that occurs after the first discharge/charge cycle. We anticipate the growing potential of emerging two-component 2D materials and their great promise for energy storage and beyond.

As a holy grail in electrochemistry, both high-power and high-energy electrochemical energy storage system (EES) has always been a pursued dream. To simultaneously achieve the \"both-high\" EES, a rational design of structure and composition for storage materials with characteristics of battery-type and capacitor-type storage is crucial. Herein, fluorine-nitrogen co-implanted carbon tubes (FNCT) have been designed, in which plentiful active sites and expanded interlayer space have been created benefiting from the heteroatom engineering and the fluorine-nitrogen synergistic effect, thus the above two-type storage mechanism can get an optimal balance in the FNCT. The implanted fluorine heteroatoms can not only amplify interlayer spacing, but also induce the transformation of nitrogen configuration from pyrrole nitrogen to pyridine nitrogen, further promoting the activity of the carbon matrix. The extraordinary electrochemical performance as results can be witnessed for FNCT, which exhibit fast lithium-ion storage capability with a high energy density of 119.4 Wh kg-1 at an ultrahigh power density of 107.5 kW kg-1 .

Faradaic reactions including charge transfer are often accompanied with diffusion limitation inside the bulk. Conductive two-dimensional frameworks (2D MOFs) with a fast ion transport can combine both-charge transfer and fast diffusion inside their porous structure. To study remaining diffusion limitations caused by particle morphology, different synthesis routes of Cu-2,3,6,7,10,11-hexahydroxytriphenylene (Cu3 (HHTP)2 ), a copper-based 2D MOF, are used to obtain flake- and rod-like MOF particles. Both morphologies are systematically characterized and evaluated for redox-active Li+ ion storage. The redox mechanism is investigated by means of X-ray absorption spectroscopy, FTIR spectroscopy and in situ XRD. Both types are compared regarding kinetic properties for Li+ ion storage via cyclic voltammetry and impedance spectroscopy. A significant influence of particle morphology for 2D MOFs on kinetic aspects of electrochemical Li+ ion storage can be observed. This study opens the path for optimization of redox active porous structures to overcome diffusion limitations of Faradaic processes.

With high theoretical specific capacity, the low-cost MoO3 is known to be a promising anode for lithium-ion batteries. However, low electronic conductivity and sluggish reaction kinetics have limited its ability for lithium ion storage. To improve this, the phase engineering approach is used to fabricate orthorhombic/monoclinic MoO3 (α/h-MoO3) homojunctions. The α/h-MoO3 is found to have excessive hetero-phase interface. This not only creates more active sites in the MoO3 for Li+ storage, it regulates local coordination environment and electronic structure, thus inducing a built-in electric field for boosting electron/ion transport. In using α/h-MoO3, higher capacity (1094 mAh g-1 at 0.1 A g-1) and rate performance (406 mAh g-1 at 5.0 A g-1) are obtained than when using only the single phase h-MoO3 or α-MoO3. This work provides an option to use α/h-MoO3 hetero-phase homojunction in LIBs.

Ni-containing heteropolyvanadate, Na6[NiV14O40], was synthesized for the first time to be applied in high-energy lithium storage applications as a negative electrode material. Na6[NiV14O40] can be prepared via a facile solution process that is suitable for low-cost mass production. The as-prepared electrode provided a high capacity of approximately 700 mAh g-1 without degradation for 400 cycles, indicating excellent cycling stability. The mechanism of charge storage was investigated using operando X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), transition X-ray microscopy (TXM), and density functional theory (DFT) calculations. The results showed that V5+ was reduced to V2+ during lithiation, indicating that Na6[NiV14O40] is an insertion-type material. In addition, Na6[NiV14O40] maintained its amorphous structure with negligible volume expansion/contraction during cycling. Employed as the negative electrode in a lithium-ion battery (LIB), the Na6[NiV14O40]//LiFePO4 full cell had a high energy density of 300 W h kg-1. When applied in a lithium-ion capacitor, the Na6[NiV14O40]//expanded mesocarbon microbead full cell displayed energy densities of 218.5 and 47.9 W h kg-1 at power densities of 175.7 and 7774.2 W kg-1, respectively. These findings reveal that the negative electrode material Na6[NiV14O40] is a promising candidate for Li-ion storage applications.

Heterostructures with the electric field effect can excite the charge transfer kinetics of materials due to the driving force of the electric field. Herein, we report a new ReS2/Nb2O5 heterostructure of rhenium disulfide coupled to niobium oxide with a mutually compatible band structure and enriched oxygen vacancies. The unique heterostructure can facilitate the redistribution of charges to induce built-in electric fields and microlocalized electric fields. As expected, the ReS2/Nb2O5 heterostructure shows a superior lithium-ion reversible capacity of 805 mAh g-1 after 2400 h at 0.10 A g-1, and 414 mAh g-1 at 2.00 A g-1. In addition, in situ X-ray diffraction and ex situ X-ray photoelectron spectroscopy analysis reveal the phase transition process of the ReS2/Nb2O5 heterostructure during the electrochemical reaction. This provides deeper insights into the construction of high-performance lithium-ion storage materials based on heterostructures with dual-electric field-driven charge transfer.