What Is the Real Origin of Single-Walled Carbon Nanotubes for the Performance Enhancement of Si-Based Anodes?

A large amount of lithium-ion storage in Si-based anodes promises high energy density yet also results in large volume expansion, causing impaired cyclability and conductivity. Instead of restricting pulverization of Si-based particles, herein, we disclose that single-walled carbon nanotubes (SWNTs) can take advantage of volume expansion and induce interfacial reactions that stabilize the pulverized Si-based clusters in situ. Operando Raman spectroscopy and density functional theory calculations reveal that the volume expansion by the lithiation of Si-based particles generates ∼14% tensile strains in SWNTs, which, in turn, strengthens the chemical interaction between Li and C. This chemomechanical coupling effect facilitates the transformation of sp2-C at the defect of SWNTs to Li-C bonds with sp3 hybridization, which also initiates the formation of new Si-C chemical bonds at the interface. Along with this process, SWNTs can also induce in situ reconstruction of the 3D architecture of the anode, forming mechanically strengthened networks with high electrical and ionic conductivities. As such, with the addition of only 1 wt % of SWNTs, graphite/SiOx composite anodes can deliver practical performance well surpassing that of commercial graphite anodes. These findings enrich our understanding of strain-induced interfacial reactions, providing a general principle for mitigating the degradation of alloying or conversion-reaction-based electrodes.

Bifunctional Potential Structure Design Breaks Electrolyte Limitations of Zinc Ion Battery.

Aqueous zinc-ion batteries (ZIBs) are safe and economical for grid applications. However, current ZIBs have limitations in terms of inferior capacity and low output voltage, which are hampered by the electrolyte applicability of the Zn2+ hosts. In this study, we propose a novel organic cathode design strategy with a bifunctional potential region. This polymeric Zn2+ host combines the conjugated polyaniline backbone to tune the molecular surface pH and [Fe(CN)6]3-/4- redox couple for high output voltage and capacity. The polyaniline doped with ferricyanide (PAF) electrode exhibits two forms of charge storage in ZIBs: proton-assisted Zn2+ doping below 1.2 V (mechanism I), and [Fe(CN)6]3-/4- redox pair above 1.8 V (mechanism II). Density functional theory calculations and in situ pH experiments demonstrated that the H+ doping process of mechanism I forms a localized pH regulation on the molecular chain surface, providing a favorable reaction environment for mechanism II. The Zn-polymer battery delivered an outstanding discharge capacity (405.2 mAh g-1) and high output voltage (1.8 V) in the Zn(CF3SO3)2 electrolyte. This study provides a new route for enhancing the structural stability of electrodes and overcoming the electrolyte limitations of ferricyanide in weakly acidic electrolytes.

Direction of arrival estimation method for ground source based on optimally polarized Rayleigh waves.

This paper points out a critical issue in the study of estimating the azimuth of ground sources by using the polarization characteristics of Rayleigh waves: even if the signal quality is good, the degree of polarization of Rayleigh waves varies across different frequency bands, and the band with the strongest energy is not the one with the lowest azimuth error. A direction of arrival estimation method for ground sources based on optimally polarized Rayleigh waves using a single three-component geophone is presented in this paper. First, the reciprocal ellipse rate, flatness coefficient, and the angle between the semi-minor axes and the horizontal plane are selected as the polarization parameters of this method according to two quantitative principles. Then the frequency band range of the optimal polarization Rayleigh wave is determined by analyzing the sum of the weights of the three polarization parameters in different frequency bands. After filtering and combining with the existing surface wave analysis method, the actual data bearing estimation result with an average error of only 4.95 degrees and a standard deviation of only 1.82 degrees is obtained. It is also found that the signal-to-noise ratio approximates the exponential decay of the direction of arrival error obtained by this method.

An Electrosynthesized 3D Porous Molybdenum Sulfide/Graphene Film with Enhanced Electrochemical Performance for Lithium Storage.

Molybdenum sulfide/graphene composites are promising anode materials for lithium-ion batteries (LIBs). In this work, MoSx /graphene composite film with an ideal 3D porous structure is developed via a facile and straightforward electrochemical route. The MoSx nanoparticles are uniformly anchored on the graphene nanosheets that are randomly arranged, resulting in MoSx /graphene composites with well-developed porous structure. Benefiting from such structure and the synergistic effect from two components, this material shows a high specific capacity over 1200 mA h g-1 , an excellent rate performance, and superior cycling stability. The dominating pseudocapacitive behavior in Li storage contributes to the outstanding rate capacity. Importantly, this kind of novel material can be easily produced as 3D microelectrodes for microscaled LIBs that are highly demanded for autonomous microelectronic systems.

Multiscale Structural Design of 2D Nanomaterials-based Flexible Electrodes for Wearable Energy Storage Applications.

2D nanomaterials play a critical role in realizing high-performance flexible electrodes for wearable energy storge devices, owing to their merits of large surface area, high conductivity and high strength. The electrode is a complex system and the performance is determined by multiple and interrelated factors including the intrinsic properties of materials and the structures at different scales from macroscale to atomic scale. Multiscale design strategies have been developed to engineer the structures to exploit full potential and mitigate drawbacks of 2D materials. Analyzing the design strategies and understanding the working mechanisms are essential to facilitate the integration and harvest the synergistic effects. This review summarizes the multiscale design strategies from macroscale down to micro/nano-scale structures and atomic-scale structures for developing 2D nanomaterials-based flexible electrodes. It starts with brief introduction of 2D nanomaterials, followed by analysis of structural design strategies at different scales focusing on the elucidation of structure-property relationship, and ends with the presentation of challenges and future prospects. This review highlights the importance of integrating multiscale design strategies. Finding from this review may deepen the understanding of electrode performance and provide valuable guidelines for designing 2D nanomaterials-based flexible electrodes.

Encapsulation of Se into Cu-decorated MXene nanosheets with superior electrochemical performance for advanced Na-Se batteries.

Sodium-selenium (Na-Se) batteries are promising energy storage systems with high energy density, high safety, and low cost. However, the huge volume change of selenium, the dissolution shuttle of polyselenides, and low selenium loading need to be solved. Herein, Cu nanoparticles decorated MXene nanosheets composite (MXene/Cu) are synthesized by etching Ti3AlC2 using a molten salt etching strategy. The Se-loaded MXene/Cu (Se@MXene/Cu) electrode delivers superior electrochemical performance even with a high Se loading of ∼74.3 wt%, owing to the synergistic effect of the two-dimensional (2D) confined structure and catalytic role of the unique MXene/Cu host. Specifically, the obtained electrode provides a reversible capacity of 587.3 mAh/g at 0.2 A/g, a discharge capacity as high as 511.3 mAh/g at a high rate of 50 A/g, and still maintains a capacity of 471.9 mAh/g even after 5000 cycles based on the mass of Se@MXene/Cu. With such excellent electrochemical kinetic properties, this study highlights the importance of designing various MXene-based composites with synergistic effects of 2D confined structure and Cu catalytic center for the development of high-performance alkali metal-chalcogen battery systems.

MoP quantum dots based multifunctional efficient electrocatalyst for stable and long-life flexible lithium-sulfur batteries.

The commercialization of lithium-sulfur (Li-S) batteries is challenging, owing to factors like the poor conductivity of S, the 'shuttle effect', and the slow reaction kinetics. To address these challenges, MoP quantum dots were decorated on hollow carbon spheres (MoPQDs/C) in this study and used as an efficient lithium polysulfides (LiPSs) adsorbents and catalysts. In this approach polysulfides are effectively trapped through strong chemisorption and physical adsorption while simultaneously facilitating LiPSs conversion by enhancing the reaction kinetics. MXene serves as a flexible physical barrier (MoPQDs/C@MXene), further enhancing the confinement of LiPSs. Moreover, both materials are conductive, significantly facilitating electron and charge transfer. Additionally, the flexible MoPQDs/C@MXene-S electrode offers a large specific surface area for sulfur loading and withstand volume expansion during electrochemical processes. As a result, the MoPQDs/C@MXene-S electrode exhibits excellent long-term cyclability and maintains a robust specific capacity of 992 mA h g-1 even after 800cycles at a rate of 1.0C (1C = 1675 mA g-1), with a minimal capacity decay rate of 0.034 % per cycle. This work proposes an efficient strategy to fabricate highly efficient electrocatalysts for advanced Li-S batteries.

A dual heterostructure enables the stabilization of 1T-rich MoSe2 for enhanced storage of sodium ions.

Electron injection effectively induces the formation of a 1T-rich phase to address the low conductivity of MoSe2. Nevertheless, overcoming the inherent metastability of the 1T phase (particularly during the conversion reactions that entail the decomposition-reconstruction of MoSe2 and volume expansion) remains a challenge. Guided by DFT results, we designed a composite with bimetal selenides-based heterostructures anchored on reduced graphene oxide (rGO) nanosheets (G-Cu2Se@MoSe2) to obtain stabilized 1T-rich MoSe2 and enhanced ion transfer. The construction of 1T-rich MoSe2 and built-in electric fields (BiEF) through electron transfer at the heterointerfaces were realized. Moreover, the rGO-metal selenides heterostructures with in situ-formed interfacial bonds could facilitate the reconstruction of the 1T-rich MoSe2-involved heterostructure and interfacial BiEF. Such a dual heterostructure endowed G-Cu2Se@MoSe2 with an excellent rate capability with a capacity of 288 mA h g-1 at 50 A g-1 and superior cycling stability with a capacity retention ratio of 89.6% (291 mA h g-1) after 15 000 cycles at 10 A g-1. Insights into the functional mechanism and structural evolution of the 1T MoSe2-involved dual heterostructure from this work may provide guidelines for the development of MoSe2 and phase-engineering strategies for other polymorphistic materials.

Polyethylene Oxide (PEO) Provides Bridges to Silica Nanoparticles to Form a Shear Thickening Electrolyte for High Performance Impact Resistant Lithium-ion Batteries.

The development of shear thickening electrolytes is proving to be pivotal in the quest for impact resistant lithium-ion batteries (LIBs). However, the high viscosity and poor stability associated with the need for high filler content has to date impeded progress. Here, this work reports a new type of polymer-bridged shear thickening electrolyte that overcomes these shortcomings, by utilizing the interaction between polymer chains and silica nanoparticles. The incorporation of polyethylene oxide (PEO) facilitates hydrocluster formation providing impact resistance with a filler content as low as 2.2 wt%. This low viscosity electrolyte has a high ionic conductivity of ≈5.1 mS cm-1 with excellent long-term stability, over 30 days. The effectiveness of this electrolyte in LIBs is demonstrated by excellent electrochemical performance and high impact resistance.

Application of Inorganic Quantum Dots in Advanced Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries have emerged as one of the most attractive alternatives for post-lithium-ion battery energy storage systems, owing to their ultrahigh theoretical energy density. However, the large-scale application of Li-S batteries remains enormously problematic because of the poor cycling life and safety problems, induced by the low conductivity , severe shuttling effect, poor reaction kinetics, and lithium dendrite formation. In recent studies, catalytic techniques are reported to promote the commercial application of Li-S batteries. Compared with the conventional catalytic sites on host materials, quantum dots (QDs) with ultrafine particle size (<10 nm) can provide large accessible surface area and strong polarity to restrict the shuttling effect, excellent catalytic effect to enhance the kinetics of redox reactions, as well as abundant lithiophilic nucleation sites to regulate Li deposition. In this review, the intrinsic hurdles of S conversion and Li stripping/plating reactions are first summarized. More importantly, a comprehensive overview is provided of inorganic QDs, in improving the efficiency and stability of Li-S batteries, with the strategies including composition optimization, defect and morphological engineering, design of heterostructures, and so forth. Finally, the prospects and challenges of QDs in Li-S batteries are discussed.

A Battery Method to Enhance the Degradation of Iron Stent and Regulating the Effect on Living Cells.

Iron is a promising material for cardiovascular stent applications, however, the low biodegradation rate presents a challenge. Here, a dynamic method to improve the degradation rate of iron and simultaneously deliver electrical energy that could potentially inhibit cell proliferation on the device is reported. It is realized by pairing iron with a biocompatible hydrogel cathode in a cell culture media-based electrolyte forming an iron-air battery. This system does not show cytotoxicity to human adipose-stem cells over a period of 21 days but inhibits cell proliferation. The combination of enhanced iron degradation and inhibited cell proliferation by this dynamic method suggests it might be an approach for restenosis inhibition of biodegradable stents.

Efficient Metal-Oriented Electrodeposition of a Co-Based Metal-Organic Framework with Superior Capacitive Performance.

An efficient cathodic electrodeposition method is developed for coating Co-based metal-organic frameworks (Co-MOF) on carbon fiber cloth (CFC), a widely used substrate in energy fields. The use of a highly active Co metal surface enables nucleation and growth of Co-MOF in 3D rodlike crystal bundles. When used as a binder-free electrode (Co-MOF/CFC) for supercapacitors, it shows a high areal capacitance of 1784 mF cm-2 at 1 mA cm-2 , good cycling stability and excellent rate capability. The assembled asymmetric all-solid-state supercapacitor device (Co-MOF/CFC//AC) delivers a high energy density and power density. This work may open up an effective approach to realize the electrosynthesis of MOF films, promoting use in energy storage and conversion fields.

Abuse-Tolerant Electrolytes for Lithium-Ion Batteries.

Safety issues currently limit the development of advanced lithium-ion batteries (LIBs) and this is exacerbated when they are misused or abused. The addition of small amounts of fillers or additives into common liquid electrolytes can greatly improve resistance to abuse without impairing electrochemical performance. This review discusses the recent progress in such abuse-tolerant electrolytes. It covers electrolytes with shear thickening properties for tolerating mechanical abuse, electrolytes with redox shuttle additives for suppressing electrochemical abuse, and electrolytes with flame-retardant additives for resisting thermal abuse. It aims to provide insights into the functioning of such electrolytes and the understanding of electrolyte composition-property relationship. Future perspectives, challenges, and opportunities towards practical applications are also presented.

One-Pot Hydrothermal Synthesis of Solution-Processable MoS2/PEDOT:PSS Composites for High-Performance Supercapacitors.

It is challenging to hydrothermally synthesize solution-processable MoS2, as the strong van der Waals force between MoS2 nanosheets induces self-assembly of agglomerates. Here, we introduce poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) into the precursor to impede aggregate formation in the hydrothermal process. A hybrid MoS2/PEDOT:PSS (MP) hydrogel is formed due to the electrostatic interactions between the negatively charged MoS2 and positively charged PEDOT chains. This hydrogel can be easily dispersed in water for subsequent solution processing such as vacuum filtration to form free-standing flexible films or extrusion 3D printing to create novel patterns. The MP film with a fracture strength of 18.59 MPa displays excellent electrochemical performance in both aqueous Na2SO4 electrolyte (474 mF cm-2) and solid-state PVA-H3PO4 electrolyte (360 mF cm-2). Flexibility and robustness can be evidenced by high capacitance retention rates of 94 and 89% after being repeatedly bent to 180° for 5000 cycles in aqueous and solid-state electrolytes, respectively.

Data on the bipolar electroactive conducting polymers for wireless cell stimulation.

Data in this article is associated with our research article "Bipolar Electroactive Conducting Polymers for Wireless Cell Stimulation" [1]. Primarily, the present article shows the data of PPy-pTS, PPy-DS and PPy-DS/collagen in conventional electrochemical process and bipolar electrochemical process for comprehensive supplement and comparison to help with better understanding and developing conducting polymers based bipolar electrochemistry. Secondly, the presented data of bipolar electrostimulation (BPES) protocol development constitute the complete dataset useful for modeling the bipolar electroactive conducting polymers focusing on wireless cell stimulation, which are reported in the main article. All data reported were analysed using Origin 2018b 64Bit.

Scalable Solution Processing MoS2 Powders with Liquid Crystalline Graphene Oxide for Flexible Freestanding Films with High Areal Lithium Storage Capacity.

Freestanding flexible electrodes with high areal mass loading are required for the development of flexible high-performance lithium-ion batteries (LIBs). Currently they face the challenge of low mass loading due to the limited concentrations attainable in processable dispersions. Here, we report a simple low-temperature hydrothermal route to fabricate flexible layered molybdenum disulfide (MoS2)/reduced graphene oxide (MSG) films offering high areal capacity and good lithium storage performance. This is achieved using a self-assembly process facilitated by the use of liquid crystalline graphene oxide (LCGO) and commercial MoS2 powders at a low temperature of 70 °C. The amphiphilic properties of ultralarge LCGO nanosheets facilitates the processability of large-size MoS2 powders, which is otherwise nondispersible in water. The resultant film with an areal mass of 8.2 mg cm-2 delivers a high areal capacity of 5.80 mAh cm-2 (706 mAh g-1) at 0.1 A g-1. This simple method can be adapted to similar nondispersible commercial battery materials for films fabrication or production of more complicated constructs via advanced fabrication technologies.

A "Tandem" Strategy to Fabricate Flexible Graphene/Polypyrrole Nanofiber Film Using the Surfactant-Exfoliated Graphene for Supercapacitors.

The surfactant-assisted liquid-phase exfoliation of expanded graphite can produce graphene sheets in large quantities with minimal defects. However, it is difficult to completely remove the surfactant from the final product, thus affecting the electrochemical properties of the produced graphene. In this article, a novel approach to fabricate flexible graphene/polypyrrole film was developed: using surfactant cetyltrimethylammonium bromide as a template for growth of polypyrrole nanofibers (PPyNFs) instead of removal after the exfoliation process; followed by a simple filtration method. The introduction of PPyNF not only increases the electrochemical performance, but also ensures flexibility. This composite film electrode offers a capacitance up to 161 F g-1 along with a capacitance retention rate of over 80% after 5000 cycles.

Silicon as a ubiquitous contaminant in graphene derivatives with significant impact on device performance.

Silicon-based impurities are ubiquitous in natural graphite. However, their role as a contaminant in exfoliated graphene and their influence on devices have been overlooked. Herein atomic resolution microscopy is used to highlight the existence of silicon-based contamination on various solution-processed graphene. We found these impurities are extremely persistent and thus utilising high purity graphite as a precursor is the only route to produce silicon-free graphene. These impurities are found to hamper the effective utilisation of graphene in whereby surface area is of paramount importance. When non-contaminated graphene is used to fabricate supercapacitor microelectrodes, a capacitance value closest to the predicted theoretical capacitance for graphene is obtained. We also demonstrate a versatile humidity sensor made from pure graphene oxide which achieves the highest sensitivity and the lowest limit of detection ever reported. Our findings constitute a vital milestone to achieve commercially viable and high performance graphene-based devices.

High-performance hybrid carbon nanotube fibers for wearable energy storage.

Wearable energy storage devices are of practical interest, but few have been commercially exploited. Production of electrodes with extended cycle life, as well as high energy and power densities, coupled with flexibility, remains a challenge. Herein, we have demonstrated the development of a high-performance hybrid carbon nanotube (CNT) fiber-based supercapacitor for the first time using conventional wet-spinning processes. Manganese dioxide (MnO2) nanoflakes were deposited onto the as-prepared CNT fibers by electrodeposition to form highly flexible nanocomposites fibers. As-prepared fibers were characterized by electron microscopy, electrical, mechanical, and electrochemical measurements. It was found that the specific capacitance was over 152 F g-1 (156 F cm-3), which is about 500% higher than the multi-walled carbon nanotube/MnO2 yarn-based supercapacitors. The measured energy density was 14.1 Wh kg-1 at a power density of 202 W kg-1. These values are 232% and 32% higher than the energy density and power density of MWNT/MnO2 yarn-based supercapacitor, respectively. It was found that the cyclic retention ability was more stable, revealing a 16% increase after 10 000 cycles. Such substantial enhancements of key properties of the hybrid material can be associated with the synergy of CNT and MnO2 nanoparticles in the fiber structure. The use of wet-spun hybrid CNT for fiber-based supercapacitors has been demonstrated.

Processable 2D materials beyond graphene: MoS2 liquid crystals and fibres.

Herein, we show properly engineered MoS2 crystals can readily form liquid crystalline dispersions in water making them ideal candidates for large-scale manufacturing processes. The guideline provided here can serve as the basis to develop practical protocols to address the long-standing goal of large-scale manufacturing of 2D materials.