Structure-Controlled Carbon Hosts for Dendrite-Free Aqueous Zinc Batteries.

The surging demand for environmental-friendly and safe electrochemical energy storage systems has driven the development of aqueous zinc (Zn)-ion batteries (ZIBs). However, metallic Zn anodes suffer from severe dendrite growth and large volume change, resulting in a limited lifetime for aqueous ZIB applications. Here, it is shown that 3D mesoporous carbon (MC) with controlled carbon and defect configurations can function as a highly reversible and dendrite-free Zn host, enabling the stable operation of aqueous ZIBs. The MC host has a structure-controlled architecture that contains optimal sp2 -carbon and defect sites, which results in an improved initial nucleation energy barrier and promotes uniform Zn deposition. As a consequence, the MC host shows outstanding Zn plating/stripping performance over 1000 cycles at 2 mA cm-2 and over 250 cycles at 6 mA cm-2 in asymmetric cells. Density functional theory calculations further reveal the role of the defective sp2 -carbon surface in Zn adsorption energy. Moreover, a full cell based on Zn@MC900 anode and V2 O5 cathode exhibits remarkable rate performance and cycling stability over 3500 cycles. These results establish a structure-mechanism-performance relationship of the carbon host as a highly reversible Zn anode for the reliable operation of ZIBs.

Role of Bicontinuous Structure in Elastomeric Electrolytes for High-Energy Solid-State Lithium-Metal Batteries.

Solid-state lithium (Li)-metal batteries (LMBs) are garnering attention as a next-generation battery technology that can surpass conventional Li-ion batteries in terms of energy density and operational safety under the condition that the issue of uncontrolled Li dendrite is resolved. In this study, various plastic crystal-embedded elastomer electrolytes (PCEEs) are investigated with different phase-separated structures, prepared by systematically adjusting the volume ratio of the phases, to elucidate the structure-property-electrochemical performance relationship of the PCEE in the LMBs. At an optimal volume ratio of elastomer phase to plastic-crystal phase (i.e., 1:1), bicontinuous-structured PCEE, consisting of efficient ion-conducting, plastic-crystal pathways with long-range connectivity within a crosslinked elastomer matrix, exhibits exceptionally high ionic conductivity (≈10-3 S cm-1 ) at 20 °C and excellent mechanical resilience (elongation at break ≈ 300%). A full cell featuring this optimized PCEE, a 35 µm thick Li anode, and a high loading LiNi0.83 Mn0.06 Co0.11 O2 (NMC-83) cathode delivers a high energy density of 437 Wh kganode+cathode+electrolyte -1 . The established structure-property-electrochemical performance relationship of the PCEE for solid-state LMBs is expected to inform the development of the elastomeric electrolytes for various electrochemical energy systems.

Carbon Quantum Dot Modified Reduced Graphene Oxide Framework for Improved Alkali Metal Ion Storage Performance.

Organic materials with redox-active oxygen functional groups are of great interest as electrode materials for alkali-ion storage due to their earth-abundant constituents, structural tunability, and enhanced energy storage properties. Herein, a hybrid carbon framework consisting of reduced graphene oxide and oxygen functionalized carbon quantum dots (CQDs) is developed via the one-pot solvothermal reduction method, and a systematic study is undertaken to investigate its redox mechanism and electrochemical properties with Li-, Na-, and K-ions. Due to the incorporation of CQDs, the hybrid cathode delivers consistent improvements in charge storage performance for the alkali-ions and impressive reversible capacity (257 mAh g-1 at 50 mA g-1 ), rate capability (111 mAh g-1 at 1 A g-1 ), and cycling stability (79% retention after 10 000 cycles) with Li-ion. Furthermore, density functional theory calculations uncover the CQD structure-electrochemical reactivity trends for different alkali-ion. The results provide important insights into adopting CQD species for optimal alkali-ion storage.

A 3D Hierarchical Host with Enhanced Sodiophilicity Enabling Anode-Free Sodium-Metal Batteries.

Sodium-metal batteries (SMBs) are considered as a compliment to lithium-metal batteries for next-generation high-energy batteries because of their low cost and the abundance of sodium (Na). Herein, a 3D nanostructured porous carbon particle containing carbon-shell-coated Fe nanoparticles (PC-CFe) is employed as a highly reversible Na-metal host. PC-CFe has a unique 3D hierarchy based on sub-micrometer-sized carbon particles, ordered open channels, and evenly distributed carbon-coated Fe nanoparticles (CFe) on the surface. PC-CFe achieves high reversibility of Na plating/stripping processes over 500 cycles with a Coulombic efficiency of 99.6% at 10 mA cm-2 with 10 mAh cm-2 in Na//Cu asymmetric cells, as well as over 14 400 cycles at 60 mA cm-2 in Na//Na symmetric cells. Density functional theory calculations reveal that the superior cycling performance of PC-CFe stems from the stronger adsorption of Na on the surface of the CFe, providing initial nucleation sites more favorable to Na deposition. Moreover, the full cell with a PC-CFe host without Na metal and a high-loading Na3 V2 (PO4 )3 cathode (10 mg cm-2 ) maintains a high capacity of 103 mAh g-1 at 1 mA cm-2 even after 100 cycles, demonstrating the operation of anode-free SMBs.

Elastomeric electrolytes for high-energy solid-state lithium batteries.

The use of lithium metal anodes in solid-state batteries has emerged as one of the most promising technologies for replacing conventional lithium-ion batteries1,2. Solid-state electrolytes are a key enabling technology for the safe operation of lithium metal batteries as they suppress the uncontrolled growth of lithium dendrites. However, the mechanical properties and electrochemical performance of current solid-state electrolytes do not meet the requirements for practical applications of lithium metal batteries. Here we report a class of elastomeric solid-state electrolytes with a three-dimensional interconnected plastic crystal phase. The elastomeric electrolytes show a combination of mechanical robustness, high ionic conductivity, low interfacial resistance and high lithium-ion transference number. The in situ-formed elastomer electrolyte on copper foils accommodates volume changes for prolonged lithium plating and stripping processes with a Coulombic efficiency of 100.0 per cent. Moreover, the elastomer electrolytes enable stable operation of the full cells under constrained conditions of a limited lithium source, a thin electrolyte and a high-loading LiNi0.83Mn0.06Co0.11O2 cathode at a high voltage of 4.5 volts at ambient temperature, delivering a high specific energy exceeding 410 watt-hours per kilogram of electrode plus electrolyte. The elastomeric electrolyte system presents a powerful strategy for enabling stable operation of high-energy, solid-state lithium batteries.