In Situ Conversion of Cu3P Nanowires to Mixed Ion/Electron‐Conducting Skeleton for Homogeneous Lithium Deposition

The introduction of 3D wettable current collectors is one of the practical strategies toward realizing high reversibility of lithium (Li) metal anodes, yet its effect is usually insufficient owing to single electron‐conductive skeleton. Here, homogeneous Li deposition behavior and enhanced Coulombic efficiency is reported for electrochemically lithiated Cu₃P nanowires, owing to the formation of a mixed ion/electron‐conducting skeleton (MIECS). In particular, by evaluating the Gibbs free energy change, the possible chemical reaction between Cu₃P and molten Li is used to construct a MIECS containing Li₃P and Cu–Li alloy phase. The successful conversion of Cu₃P nanowires to Li₃P and Cu–Li alloy nanocomposite not only greatly reduces the surface energy between molten Li and Cu₃P, but also induces uniform Li stripping/plating behavior via balanced ion/electron transport. Thus, the as‐obtained Li@MIECS composite anode displays superior cycling stability in both symmetric cells and full cells. This work provides a promising option for the preparation of high‐performance composite Li anodes containing MIECS by thermally pre‐storing Li.     

Oxygen‐Deficient Blue TiO2 for Ultrastable and Fast Lithium Storage

Developing a titanium dioxide (TiO₂)‐based anode with superior high‐rate capability and long‐term cycling stability is important for efficient energy storage. Herein, a simple one‐step approach for fabricating blue TiO₂ nanoparticles with oxygen vacancies is reported. Oxygen vacancies can enlarge lattice spaces, lower charge transfer resistance, and provide more active sites in TiO₂ lattices. As a result, this blue TiO₂ electrode exhibits a highly reversible capacity of 50 mAh g^?1 at 100 C (16 800 mA g^?1) even after 10 000 cycles, which is attributable to the combination of surface capacitive process and remarkable diffusion‐controlled insertion revealed by the kinetic analysis. The strategy of employing oxygen‐deficient nanoparticles may be extended to the design of other robust semiconductor materials as electrodes for energy storage.     

Superior Oxygen Reduction Reaction on Phosphorus‐Doped Carbon Dot/Graphene Aerogel for All‐Solid‐State Flexible Al–Air Batteries

Carbon dots have been recognized as one of the most promising candidates for the oxygen reduction reaction (ORR) in alkaline media. However, the desired ORR performance in metal–air batteries is often limited by the moderate electrocatalytic activity and the lack of a method to realize good dispersion. To address these issues, herein a biomass‐deriving method is reported to achieve the in situ phosphorus doping (P‐doping) of carbon dots and their simultaneous decoration onto graphene matrix. The resultant product, namely P‐doped carbon dot/graphene (P‐CD/G) nanocomposites, can reach an ultrahigh P‐doping level for carbon nanomaterials. The P‐CD/G nanocomposites are found to exhibit excellent ORR activity, which is highly comparable to the commercial Pt/C catalysts. When used as the cathode materials for a primary liquid Al–air battery, the device shows an impressive power density of 157.3 mW cm^?2 (comparing to 151.5 mW cm^?2 of a similar Pt/C battery). Finally, an all‐solid‐state flexible Al–air battery is designed and fabricated based on our new nanocomposites. The device exhibits a stable discharge voltage of ≈1.2 V upon different bending states. This study introduces a unique biomass‐derived material system to replace the noble metal catalysts for future portable and wearable electronic devices.     

Nonwoven rGO Fiber‐Aramid Separator for High‐Speed Charging and Discharging of Li Metal Anode

Li metal, which has a high theoretical specific capacity and low redox potential, is considered to the most promising anode material for next‐generation Li ion‐based batteries. However, it also exhibits a disadvantageous solid electrolyte interphase (SEI) layer problem that needs to be resolved. Herein, an advanced separator composed of reduced graphene oxide fiber attached to aramid paper (rGOF‐A) is introduced. When rGOF‐A is applied, F^? anions, generated from the decomposition of the LiPF₆ electrolyte during the SEI layer formation process form semi‐ionic C? F bonds along the surface of rGOF. As Li⁺ ions are plated, the “F‐doped” rGO surface induces the formation of LiF, which is known as a component of a chemically stable SEI, therefore it helps the Li metal anode to operate stably at a high current of 20 mA cm^?2 with a high capacity of 20 mAh cm^?2. The proposed rGOF‐A separator successfully achieves a stable SEI layer that could resolve the interfacial issues of the Li metal anode.     

In Situ Electrochemical Synthesis of MXenes without Acid/Alkali Usage in/for an Aqueous Zinc Ion Battery

The traditional method to fabricate a MXene based energy storage device starts from etching MAX phase particles with dangerous acid/alkali etchants to MXenes, followed by device assembly. This is a multistep protocol and is not environmentally friendly. Herein, an all‐in‐one protocol is proposed to integrate synthesis and battery fabrication of MXene. By choosing a special F‐rich electrolyte, MAX V₂AlC is directly exfoliated inside a battery and the obtained V₂CT_X MXene is in situ used to achieve an excellent battery performance. This is a one‐step process with all reactions inside the cell, avoiding any contamination to external environments. Through the lifetime, the device experiences three stages of exfoliation, electrode oxidation, and redox of V₂O₅. While the electrode is changing, the device can always be used as a battery and the performance is continuously enhanced. The resulting aqueous zinc ion battery achieves outstanding cycling stability (4000 cycles) and rate performance (97.5 mAh g^?1 at 64 A g^?1), distinct from all reported aqueous MXene‐based counterparts with pseudo‐capacitive properties, and outperforming most vanadium‐based zinc ion batteries with high capacity. This work sheds light on the green synthesis of MXenes, provides an all‐in‐one protocol for MXene devices, and extends MXenes’ application in the aqueous energy storage field.     

Enabling Deformable and Stretchable Batteries

Deformable energy storage devices are needed to power next‐generation wearable electronics that interface intimately with human skin. Currently, deformable energy storage devices demonstrate poor performance compared to their rigid lithium‐ion counterparts, forcing wearable manufacturers to design their devices around bulky battery compartments. However, technological advances to create deformable batteries at the component and device level have yielded continuous improvement in stretchable batteries over the last five years. In this Essay, the major strategies at the component and device level that have been successfully employed to create stretchable batteries are reviewed. The outstanding challenges facing deformable energy storage are also discussed, namely, energy density, packaging, delamination, device integration, and manufacturing. This Essay will give researchers who are interested in contributing to the development of deformable batteries a cursory understanding of the most successful strategies to date, and provide insights into the most important directions to pursue in the future.     

Redox‐Active Organic Compounds for Future Sustainable Energy Storage System

Utilizing redox‐active organic compounds for future energy storage system (ESS) has attracted great attention owing to potential cost efficiency and environmental sustainability. Beyond enriching the pool of organic electrode materials with molecular tailoring, recent scientific efforts demonstrate the innovations in various cell chemistries and configurations. Herein, recent major strategies to build better organic batteries, are highlighted: diversifying charge‐carrying ions, modifying electrolytes, and utilizing liquid‐type organic electrodes. Each approach is summarized along with their advantages over Li‐ion batteries (LIBs). An outlook is also provided on the practical realization of organic battery systems, which hints at possible solutions for future sustainable ESSs.