Next-generation Electrochemical Energy Storage Devices Research Articles

Recyclable organic radical electrodes for metal-free batteries.

Organic batteries are one of the possible routes for transitioning to sustainable energy storage solutions. However, the recycling of organic batteries, which is a key step toward achieving circularity, is not easily achieved. This work shows the direct recycling of poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl) (PTMA) and poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl acrylamide) (PTAm) based composite electrodes. After charge-discharge cycling, the electrodes are deconstructed using a solubilizing-solvent and then reconstructed using a casting-solvent. The electrochemical properties of the original and recycled electrodes are compared using cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) cycling, from which it is discovered using time-of-flight secondary ion mass spectrometry (ToF-SIMS) that recycling can be challenged by the formation of a solid-electrolyte interphase (SEI). In turn, an additive is proposed to modify the SEI layer and improve the properties after recycling. Last, an anionic rocking chair battery consisting of PTAm electrodes as both positive and negative electrodes is demonstrated, in which the electrodes are recycled to form new battery. This work gives demonstrates the recycling of composite electrodes for organic batteries and provides insights into the challenges and possible solutions for recycling the next-generation electrochemical energy storage devices.

Synthesis of binder-free and highly conducting MoS2 sphere like electrode material for supercapacitor application

Binder free spheres like molybdenum disulfide (MoS2) electrode material (E-M) is synthesized on nickel foam by chemical vapor deposition technique. The interconnected spheres like structures are responsible for maximum electrolyte-ions diffusion and control volume-expansion of MoS2 E-M. The synthesized sphere-based MoS2 E-M is exhibited specific capacitance of 4200 F/g, energy density and power density of 53–145 Wh/kg and 250–3000 W/kg. The absence of charge transfer resistance and binder free synthesis persuaded the MoS2 E-M to reveal the excellent cyclic stability of 98.76 % even after 4000 cycles. The equivalent series resistance before/after 4000 cycles of MoS2 E-M are −3.54/3.22 Ω. The constant b values are 0.721, 0.759, 0.768 and 0.771 which are greater than 0.5 but less than 1 indicating the hybrid-nature of the synthesied E-M. The diffusive and capacitive contributions are 96,78 and 4, 12 % at 5 and 200 mV/s.. The hybrid-nature of the MoS2 E-M makes it usable for the next-generation electrochemical energy storage devices.

Three-dimensional Ti3C2 structure design and in-situ growth of nano-TiO2 crystals to realize high performance lithium-sulfur battery

Lithium–sulfur (Li–S) batteries represent a promising energy storage system with the potential to replace traditional lithium-ion batteries. Recent research has explored the practical applications of Li–S batteries. However, due to the insulation properties of the sulfur components and the shuttle effect of polysulfides, the practical application of Li–S batteries is hindered by poor cycle stability and short life. In this study, we developed a controllable three-dimensional Ti3C2 structure design process, and through in situ growth of TiO2 nanocrystals, we prepared three-dimensional porous materials with TiO2@Ti3C2 heterostructures. These materials constructed using two-dimensional lamellar Ti3C2 function as a conductive skeleton to improve the conductivity of the sulfur cathodes, and through the in-situ growth of nano-TiO2 to introduce more binding sites and provide more chemisorption sites to limit the dissolution and shuttle of polysulfides. In addition, the TiO2@Ti3C2 heterointerface generated in situ on the surface of the lamellar structure can induce an internal electric field and increase active reaction sites, which promotes reaction kinetics, accelerates charge diffusion/transport, and promotes LiPS transformation. The materials designed in this study can effectively restrain the shuttle effect by realising the association process of adsorption, capture, and transformation of polysulfides. Thus, when applied as the sulfur cathode frame, it shows a high specific capacity of 1261.41 mAh g−1 at a rate of 0.1 C. In addition, a specific capacity of 66.5 % is maintained over 500 cycles at a rate of 1 C. This strategy supports the development of Li–S batteries with extraordinary performance and opens up a promising way to design next-generation electrochemical energy storage devices.

N,O-Doped hierarchical Meso/Microporous carbon frameworks enable efficient Carbon-Based supercapacitor

The precise design of heteroatom-doped carbon with large specific surface area, high conductivity and abundant active sites is profound significance for next-generation electrochemical energy storage devices. Covalent organic frameworks (COFs), emerging as novel crystalline porous polymers, have provided a versatile and powerful platform for complex structural construction and tailor-made functional exploitation. Herein, several kinds of hierarchical porous heteroatom-doped carbons frameworks have been achieved, therein, the topology design furnishes guidance for the structural tiling of extended porous polygons, while the in situ polycondensation reaction provides synthetic procedures to make them true, and then the high-temperature carbonization converts the crystalline COFs into highly conductive heteroatoms-doped meso/microporous carbon frameworks. As the result, the optimal N,O-doped carbon nanosheets demonstrate a high heteroatom content, large specific surface area and superior electrochemical performance with a high energy density of 15.28 Wh kg−1 at 352.5 W kg−1. This strategy not only supplies an efficient approach to obtain heteroatom-doped carbon with a high mass density and high porosity, but also paves the way for the precise design of the structure and activity centers for high-quality energy materials.

Ultrafine Sb2O3 Nanoparticle-Decorated Reduced Graphene Oxide as an Anode Material for Lithium-Ion Batteries

Antimony (Sb)-based materials have shown great potential as anode materials for lithium-ion batteries (LIBs) owing to their high energy density as well as long lifespan. However, the huge volume variation upon cycling will result in severe capacity fading, thus hindering the practical application of Sb-based anode materials. Herein, an ultrafine Sb2O3 nanoparticle-decorated reduced graphene oxide (rGO) composite (denoted as Sb2O3/rGO) was developed through a facile thermal decomposition of antimony 2-ethylhexanoate on rGO in the air at low temperatures, where the ultrafine Sb2O3 nanoparticles are homogeneously anchored on the rGO substrate. Benefiting from the rich mesoporous structure, large specific surface area, moderate mass loading, and uniform dispersion of ultrafine Sb2O3 nanoparticles, the optimized Sb2O3/rGO-100 electrode showed enhanced electrode–electrolyte contact area and ion/electron transferability. When applied as an anode material for LIBs, the Sb2O3/rGO-100 electrode exhibited excellent cycling stability and rate performance, delivering a high reversible capacity of 513 mAh g–1 at 0.5 A g–1 after 300 cycles. Ex situ transmission electron microscopy reveals that the nanoscale configuration of rGO and Sb2O3 nanoparticles of Sb2O3/rGO-100 was well maintained, while the bulk Sb2O3 crushed into pieces after cycling, further confirming the robust structure of the composite. More importantly, the synthetic method may also be commonly applied to other metal oxides, which is promising for the development of high-performance next-generation electrochemical energy storage devices.

Comparative simulation of thin-film and bulk-type all-solid-state batteries under adiabatic and isothermal conditions

As a recently rising cell technology, all-solid-state batteries (ASSBs) have emerged as next-generation electrochemical energy storage devices, which can be classified into two main types: thin-film and bulk-type, according to their structures. Here, we present a comparative simulation of ASSBs employing thin-film and bulk-type structures by using three-dimensional (3-D) and pseudo-3-D electrochemical-thermal coupled models developed on an open-source platform, OpenFOAM. Our results reveal the main differences between two types of ASSBs in terms of voltage-capacity curves, temperature rises, heat generation mechanisms, effect of ambient temperature, and various internal resistance under isothermal and adiabatic conditions, respectively. The thin-film extracts around a third of the capacity of the bulk-type and shows stronger temperature-dependent behaviors at the same C-rate. At the investigated C-rates, the ohm heat always represents a tiny part of the total heat in the thin-film while a decisive role in the bulk-type due to its ohm resistance being nearly-two orders of magnitude higher than the former. Reversely, the charge-transfer resistance of the bulk-type is about an order of magnitude lower than that of the thin-film. Collectively, this work provides a fundamental understanding of thin-film and bulk-type structures.

Three-dimensional binder-free electrodes with high loading of electroactive material for high performance asymmetric supercapacitors

ZnCo bimetallic LDH is successfully grown on 3D Co 3 O 4 scaffolds on nickel foam as a stable hierarchical core-shell heterostructural electrode. Benefiting from the fine ion/electron transport within Co 3 O 4 @Zn 1 Co 2 -LDH electrode, the prepared Co 3 O 4 @Zn 1 Co 2 -LDH//ZiF-8 DC asymmetric supercapacitor exhibits a high energy density of 1.1 mWh cm -2 at a power density of 4.0 mW cm -2 , which is superior to the values of previous reports. • Three-dimensional binder-free electrodes are constructed with a core-shell heterostructure. • The electrode material can achieve a high quality loading of 13∼15 mg cm -2 . • The electrode achieves high areal capacitance of 10.5 F cm -2 at 5 mA cm -2 and high long durability. • The ASC device delivers a high energy density of 1.1 mWh cm -2 at a power density of 4.0 mW cm -2 . • The ASC device shows 82.0% of capacitance retention after 10000 cycles at 30 mA cm -2 . Rational design of electrode material structure is a key factor to improve high energy density/power density and long lifetime of supercapacitors. Here, a simple two-step hydrothermal strategy was used to synthesize Co 3 O 4 on nickel foam (NF), and a core-shell heterostructure was constructed by growing ZnCo bimetallic layered double hydroxides (LDH) on Co 3 O 4 scaffolds. Because of its unique heterogeneous structure and optimization of different components, the electrochemical performance of the active components was maximized because of the synergistic effect. The electrode material can achieve a high- quality loading of 13∼15 mg cm -2 . The binder-free electrode material Co 3 O 4 @Zn 1 Co 2 -OH grown directly on NF can achieve a high areal capacitance of 10.5 F cm -2 at 5 mA cm -2 and rate performance (82.9% retention at 30 mA cm -2 ) and long durability (62.3% capacitance retention at 30 mA cm -2 ). Additionally, a Co 3 O 4 @Zn 1 Co 2 -LDH//ZiF-8 DC (ZiF-8 Derived Carbon) asymmetric supercapacitor (ASC) is assembled with an operating voltage of 1.5 V. The ASC device delivers a maximum energy density of 1.1 mWh cm -2 (33.7 Wh kg -1 ) at a power density of 4.0 mW cm -2 (19.6 W kg -1 ) and exceptional cycling stability (82.0% of capacitance retention after 10000 cycles at 30 mA cm -2 ). This work demonstrates that hierarchical core-shell heterostructures show great potential in development of next-generation electrochemical energy storage devices.

Design of multifunctional C@Fe3O4–MoO3 binary nanocomposite for applications in triphenylmethane textile dye amelioration via ultrasonic adsorption and electrochemical energy storage

In this paper, we present the synthesis of C@Fe3O4–MoO3 binary composite were prepared through the facile hydrothermal process. The ultrasonic aided adsorption efficacy was evaluated by studying triphenylmethane dye's adsorption potential. The ultrasonic aided adsorption capacity towards crystal violet was 993.6 mg/g, which is remarkably higher and best fitted with the Langmuir isotherm model and followed pseudo-second-order kinetics. The electrochemical studies working electrode have been prepared with 80 wt% active material, 10 wt% carbon black, and 10% polyvinylidene difluoride to evaluate energy storage characteristics. The C@Fe3O4–MoO3 demonstrated an excellent specific capacitance of 40.94 F/g with better retention and stability, making it a potential cathode material for next-generation electrochemical energy storage devices.

Zn–Co-MOF on solution-free CuO nanowires for flexible hybrid energy storage devices

Pouch-type supercapacitor was developed by employing flexible Zn–Co-metal organic framework (MOF)@CuO and porous reduced graphene oxide as active electrodes. The flexible Zn–Co-MOF@CuO was fabricated by a facile two-step strategy. In the first step, Cu mesh was oxidized to cupric oxide (CuO) by a solution-free treatment. In the second step, Zn–Co-MOF was deposited on CuO scaffold through a solvothermal treatment. The as-prepared integrated Zn–Co-MOF@CuO exhibited excellent flexibility at different bending angles. The flexible Zn–Co-MOF@CuO displayed excellent electrochemical activity during three-electrode testing due to the merits of high electrical conductivity and an existence of p-n heterojunction between CuO and Zn–Co-MOF. The as-fabricated pouch supercapacitor yielded a high energy density of 41 W h kg−1 at a current density of 1 A g−1 and an excellent cycling stability of 97% after 20,000 cycles. Structural and superior electronic properties of Zn–Co-MOF@CuO were further verified through first principles calculations based on density functional theory (DFT), which perfectly supported the experimental results. The excellent electrochemical attributes of the flexible pouch supercapacitor show immense promise for next-generation electrochemical energy storage devices.

Unraveling the mechanism of non-uniform zinc deposition in rechargeable zinc-based batteries with vertical orientation

• The non-uniform zinc deposition in the vertical direction is investigated. • Optical observations and stripping/platting model are combined in this work. • The non-uniform deposited zinc is started by nucleation site fracture. • The inhomogeneity is exacerbated by the non-uniform current and hydrogen evolution. Secondary zinc-based batteries demonstrate a bright prospect as a candidate for next-generation electrochemical energy storage devices. However, the inhomogeneous zinc deposition with vertical orientation during electrochemical stripping/platting cycles leads to battery failure quickly and thereby limits commercial applications of zinc-based batteries. In this work, the deposited electrochemical reaction is deeply investigated and the mechanism of inhomogeneous electrochemical deposition is proposed via in-situ optical observation and numerical analysis. During the deposited reaction, zinc atoms prefer to deposit on the nucleation sites on the electrode surface, changing the morphology of nucleation sites and leading to possible fractures. The fractural zinc fragments then accumulate at the bottom and connect to the bulk electrode, which initiate the inhomogeneous distribution in the vertical direction where the protrusion appears at the bottom, and the middle and top parts have rare deposited zinc. The inhomogeneity is exacerbated during stripping/platting reaction cycles due to the non-uniform local current density distribution on the emerging protrusion. Besides, the generated bubbles caused by hydrogen evolution exacerbate the inhomogeneous distribution via changing the ion distribution. Based on the conclusions, a uniform deposition behavior is achieved via modulating the ion distribution by the flowing electrolyte as a demonstration. The unraveled mechanisms can serve as a reference for the design of advanced zinc-based batteries with stable electrodes.

Electrode-Electrolyte Interactions in an Aqueous Aluminum-Carbon Rechargeable Battery System.

Being environmentally friendly, safe and easy to handle, aqueous electrolytes are of particular interest for next-generation electrochemical energy storage devices. When coupled with an abundant, recyclable and low-cost electrode material such as aluminum, the promise of a green and economically sustainable battery system has extraordinary appeal. In this work, we study the interaction of an aqueous electrolyte with an aluminum plate anode and various graphitic cathodes. Upon establishing the boundary conditions for optimal electrolyte performance, we find that a mesoporous reduced graphene oxide powder constitutes a better cathode material option than graphite flakes.

Construction of Ti4O7/TiN/carbon microdisk sulfur host with strong polar N–Ti–O bond for ultralong life lithium–sulfur battery

As the desired sulfur host of lithium-sulfur battery, the strong polarity and fast electron migration capability are indispensable for achieving effective adsorption and conversion of lithium polysulfides (LiPSs), that is, restricting the shuttle effect. Herein a porous microdisk Ti4O7/TiN/C heterojunction with strong polar N-Ti-O covalent bonds is precisely constructed. Compared with O-Ti-O or N-Ti-N bond in single Ti4O7 or TiN, the N-Ti-O bond with stronger polarity could adsorb and bond with S and Li atoms in LiPSs, which is beneficial for LiPSs adsorption. Beside, the Ti4O7/TiN heterostructure favors the electron transfer, which could promote the conversion of LiPSs. The design strategy is to construct abundant polar N-Ti-O bonds at Ti4O7/TiN heterogeneous interface that would realize the associative process of LiPSs adsorption, trapping, and conversion, thereby restraining the shuttle effect efficiently. In the current study, as the host of the sulfur cathode, the porous microdisk TiN/Ti4O7/C heterojunction exhibits a high specific capacity of 1204.5 mAh g−1 at 0.2 C, and a high specific capacity of 616.5 mAh g−1 at an ultrahigh current density of 4 C. In addition, 86.4% and 116.9% capacity are retained over 1000 cycles at 1 C and 2 C, respectively. This strategy provides an insight into developing lithium-sulfur battery with extraordinary performance, and opens promising routes to design the next-generation electrochemical energy storage devices.

Spontaneous knitting behavior of 6.7-nm thin (NH4)0.38V2O5 nano- ribbons for binder-free zinc-ion batteries

Rechargeable, aqueous Zn-ion batteries in a neutral or mildly acidic electrolyte have attracted great attention. The fabrication of binder-free electrodes to boost the Zn2+ transport is extremely desirable for the development of aqueous zinc-ion batteries but remains a big challenge. Herein, we revealed a spontaneous knitting behaviour in 6.7 nm thin, flexible (NH4)0.38V2O5 nanoribbons by a hydrothermal route to form binder-free paper cathode for aqueous zinc-ion batteries. Conductive multi-walled carbon nanotubes (CNTs) was also successfully imbedded into this paper to enhance the electronic conductivity and produce abundant meshes (pore size: 1-3 µm) inside the paper. Taking advantage of the binder-free design and the porous architecture of the paper cathode, it delivered a reversible capacities of 465 mAh·g−1 at 100 mA·g−1. A capacity retention of above 89.3 % after 500 cycles at 100 mA·g−1 has been achieved. Importantly, the resulting paper electrode exhibited a specific energy as high as 343 Wh·kg−1, which remarkably outperforms most of the zinc-ion batteries based on powder form cathode with the presence of polymer binder. Our work reveals a novel self-grown strategy for the binder-free, freestanding electrodes on Zn2+ ion storage from the ultrathin, flexible ammonium vanadates nanostructures, and it might be applicable to the storage of other metal/non-metallic ions (Na+, Mg2+, Ca2+, Al3+, NH4+ etc.) in next-generation electrochemical energy storage devices.

Fabricating low-temperature-tolerant and durable Zn-ion capacitors via modulation of co-solvent molecular interaction and cation solvation

Aqueous Zn-based energy-storage devices have aroused much interest in recent years. However, uncontrollable dendrite growth in the Zn anode significantly limits their cycle life. Moreover, the poor low-temperature performance arising from the freezing of aqueous electrolytes at sub-zero temperatures restricts their practical applications in cold regions. Here, we fabricated low-temperature-tolerant and durable Zn-ion hybrid supercapacitors (ZHSCs) via modulating a co-solvent water/ethylene glycol electrolyte. The interaction of intermolecular hydrogen bonds between water and ethylene glycol as well as cation solvation was systematically investigated by tuning the co-solvent composition. The results illustrate that the ZnSO4/water/ethylene glycol (65%) electrolyte possesses high ionic conductivity at low temperatures and effectively prevents the dendrite formation of the Zn anode. The as-fabricated ZHSCs exhibit long-term cyclability and are capable of working at sub-zero temperatures as low as −40°C. The present ZHSCs are anti-freezing and cost-effective, which may find new applications in the fields of next-generation electrochemical energy storage devices.

Core-shell structured NaTi2(PO4)3@polyaniline as an efficient electrode material for electrochemical energy storage

Sodium-ion batteries are widely suggested as next-generation electrochemical energy storage devices for various applications due to the abundance of sodium resource and environmental friendliness. Advanced anode materials with outstanding Na+ storage performances are crucial for sodium storage. Herein, core-shell NaTi2(PO4)3@polyaniline is synthesized by using a simple sol-gel route and a self-assembly process. In this material, the NaTi2(PO4)3 crystals are uniformly coated by the polyaniline layer. Such polyaniline is benefit to enhance the electronic conductivity and promote the Na+ diffusion of NaTi2(PO4)3 anode. The NaTi2(PO4)3@polyaniline presents the reversible capacities of 128.8 and 115.6 mAh g−1 at 0.1 and 5 C, and it also presents a high capacity retention of 96.9% after 200 cycles at 10 C. The results demonstrate that this new approach can be used to improve other anodes for electrochemical energy conversion and storage.

High-energy aqueous Li-ion hybrid capacitor based on metal-organic-framework-mimicking insertion-type copper hexacyanoferrate and capacitive-type graphitic carbon electrodes

A high-performance aqueous Li-ion hybrid capacitor (LHC) using sonochemically prepared copper hexacyanoferrate (Cu-HCF) and sodium alginate-derived graphitic carbon (GC) nanoparticles are capable of serving as positive and negative electrodes, respectively, is described in this report. The electrode materials were prepared in a cost-effective manner and characterized using X-ray diffraction (XRD) and Fourier transform-infrared spectroscopy (FT-IR). High-resolution transmission electron microscopy (HR-TEM) and surface area measurements revealed the formation of 30- to 60-nm Cu-HCF and 40- to 60-nm GC particles with specific surface areas of 48 and 802 m2g–1, respectively. Electrochemical studies including cyclic voltammetry (CV), galvanostatic charge-discharge (CD) analysis and electrochemical impedance spectroscopy (EIS) using a three-electrode configuration confirmed the presence of intercalative capacitance in the Cu-HCF electrode and double-layer capacitance in the GC electrode. Furthermore, the constructed Cu-HCF‖GC aqueous LHC system operates over a wide voltage window (2.2 V) and delivers a high capacitance (63.64 F g−1) and high energy density (42.78 Wh kg−1) with a good rate capability. These key features make the LHC system an ideal candidate for next-generation electrochemical energy storage devices.

A non-polarity flexible asymmetric supercapacitor with nickel nanoparticle@ carbon nanotube three-dimensional network electrodes

Asymmetric supercapacitors are one of the promising next-generation electrochemical energy storage devices. However, the necessity to distinguish the polarity of asymmetric supercapacitors makes it more like rechargeable batteries and affects the convenience of practical applications. We herein report a novel flexible asymmetric supercapacitor (FASC) that can be charged without distinguishing the electrode polarity based on CVD-grown nickel nanoparticle@carbon nanotube (Ni@CNT) network films. The FASC is assembled by using the binder-free Ni@CNT as both the negative and positive electrodes but aqueous alkaline solution as the electrolyte. In such a design, one electrode side is involved with the Faradaic redox reactions between nickel nanoparticles and OH-, while the other side works via electric double layer charge accumulation at the interface of CNTs/electrolyte, enabling the device with an asymmetric feature and a high voltage of 1.8V. Exactly because of the above, the FASC demonstrates almost the same charge/discharge profiles, stable cycling and comparable efficiency for powering small electronics even with frequently alternating the charging direction. With the integration of hydrogel electrolyte of PVA-KOH, our flexible quasi-solid-state FASC device delivers high volumetric energy density of 1.39 mWh cm−3 and power density of 440mWcm−3, as well as excellent cycleability up to 10,000 times (100% capacitance retention). The volumetric performance is even much better than previous reported FASC devices that were designed with complicated electrode architectures. Our work presents a pioneering strategy for developing non-polarity asymmetric electrochemical energy storage systems.

Interfacial Processes and Influence of Composite Cathode Microstructure Controlling the Performance of All-Solid-State Lithium Batteries.

All-solid-state lithium-ion batteries have the potential to become an important class of next-generation electrochemical energy storage devices. However, for achieving competitive performance, a better understanding of the interfacial processes at the electrodes is necessary for optimized electrode compositions to be developed. In this work, the interfacial processes between the solid electrolyte (Li10GeP2S12) and the electrode materials (In/InLi and LixCoO2) are monitored using impedance spectroscopy and galvanostatic cycling, showing a large resistance contribution and kinetic hindrance at the metal anode. The effect of different fractions of the solid electrolyte in the composite cathodes on the rate performance is tested. The results demonstrate the necessity of a carefully designed composite microstructure depending on the desired applications of an all-solid-state battery. While a relatively low mass fraction of solid electrolyte is sufficient for high energy density, a higher fraction of solid electrolyte is required for high power density.

Effects of Solute-Solvent Hydrogen Bonding on Nonaqueous Electrolyte Structure.

We investigate the source of Raman background signal commonly misidentified as fluorescence in nonaqueous electrolytes via a variety of spectroscopies (Raman, fluorescence, NMR) and find evidence of hydrogen-bonding interactions. This hydrogen bonding gives rise to broadband anharmonic vibrational modes and suggests that anions play an important and underappreciated role in the structure of nonaqueous electrolytes. Controlling electrolyte structure has important applications in advancing in operando spectroscopy measurements as well as understanding the stability of high concentration electrolytes for next-generation electrochemical energy storage devices.

Evaluating the performance of nanostructured materials as lithium-ion battery electrodes

The performance of the lithium-ion cell is heavily dependent on the ability of the host electrodes to accommodate and release Li+ ions from the local structure. While the choice of electrode materials may define parameters such as cell potential and capacity, the process of intercalation may be physically limited by the rate of solid-state Li+ diffusion. Increased diffusion rates in lithium-ion electrodes may be achieved through a reduction in the diffusion path, accomplished by a scaling of the respective electrode dimensions. In addition, some electrodes may undergo large volume changes associated with charging and discharging, the strain of which, may be better accommodated through nanostructuring. Failure of the host to accommodate such volume changes may lead to pulverisation of the local structure and a rapid loss of capacity. In this review article, we seek to highlight a number of significant gains in the development of nanostructured lithium-ion battery architectures (both anode and cathode), as drivers of potential next-generation electrochemical energy storage devices.