Aqueous Zn‐metal batteries are the most promising system for large‐scale energy storage due to their high capacity, high safety, and low cost. The Zn‐metal anode, however, suffers from continuous parasitic reactions, random dendrite growth, and sluggish kinetics in aqueous electrolytes. Herein, a high donor number solvent, tetramethylurea (TMU), is introduced as electrolyte additive to enable highly reversible Zn‐metal anode, where the TMU can 1) preferentially adsorb on the Zn surface to inhibit Zn corrosion and suppress parasitic reaction, 2) solvate with Zn2+ and exclude the H2O from Zn2+ solvation sheath to weaken water activity significantly, and 3) contribute to form an inorganic‐organic bilayer solid electrolyte interphase to enable homogeneous and rapid Zn2+ transport kinetic for dendrite‐free Zn deposition. Benefiting from these three merits, the resulting aqueous electrolyte demonstrates a highly reversible Zn plating/stripping cycling in a Zn||Ti asymmetric cell for over 1200 cycles and in a Zn||Zn symmetric cell for over 4000 h. As a proof‐of‐concept, the aqueous Zn‐metal full cells assembled with various state‐of‐the‐art cathodes also deliver excellent cycling performance even with a 10 µm thin Zn anode, favoring the practical application.
The Li dendrite issue is the major barrier that limits the implement of Li metal anode practically, especially at high current density. From the perspective of the nucleation and growth mechanism of the Li dendrite, we rationally develop a novel Prussian blue analogues (PBA)-derived separator, where tuning the metal ions bestows the PBAs with open metal site to confine anion movement and thereby afford a high Li + transference number (0.78), and PBA with ordered micropores could act as an ionic sieve to selectively extract Li + and thereby homogenize Li + flux. This demonstrates a highly reversible Li plating/stripping cycling for 3000 h at a practically high current density (5.0 mA cm −2 ). Consequently, a high loading Li||LiFeO 4 battery (∼10.0 mg cm −2 ) demonstrates ultralong cycling life at high current densities (∼5.1 mA cm −2 ). This work highlights the prospect of optimizing PBAs in regulating ion transport behavior to enable high-power Li metal batteries.
Si microparticle (SiMP) anodes feature much lower production cost and higher tap density compared to their nanosized counterparts, which hold great promise for high‐energy‐density lithium‐ion batteries, yet they suffer from unavoidable particle pulverization during repeated cycling, thus making their practical application extremely challenging. Herein, a non‐flammable localized high‐concentration electrolyte (LHCE) is rationally formulated using a fluorinated solvent, 2,2,2‐trifluoroethyl methyl carbonate (FEMC), to induce fluorinated solvent‐coupled anion‐derived interfacial chemistry. Unlike other LHCEs, the FEMC‐based LHCE is demonstrated to build a highly robust and stable F‐rich inorganic–organic bilayer solid–electrolyte interphase on SiMP anode, which endows stable cycling of SiMP anode (≈3.4 mAh cm−2) with an ultrahigh Coulombic efficiency of ≈99.7%. Coupled with its high anodic stability, the FEMC‐based LHCE endows unprecedented cycling stability for high‐energy‐density batteries containing high‐capacity SiMP anodes with Ni‐rich LiNi8Mn1Co1O2 or 5 V‐class LiNi0.5Mn1.5O4 cathodes. Remarkably, a 1.0 Ah‐level SiMP||LiNi8Mn1Co1O2 pouch‐cell stably operates for more than 200 cycles, representing the pioneering report in pouch cells containing SiMP anodes.
The practical application of lithium-metal batteries is hindered by insufficient lithium Coulombic efficiency and uncontrolled dendrite growth, bringing a challenge concerning how to create robust solid electrolyte interphases (SEIs) that can regulate Li+ transport and protect reactive lithium-metal. Here, we present the rational construction of a multi-component jigsaw-like artificial SEI by the integration of fluorine-containing silane and polyether-containing silane. The fluorine-donating group prevents the parasitic reaction and yields a dense structure for homogeneous lithium deposition. Additionally, the lithophilicity of ethylene glycol backbone facilitates the rapid transport of Li+ and the cross-linked network increases mechanical robustness of the SEI. With this artificial SEI, we show highly reversible lithium plating and stripping cycling for more than 500 hours. Moreover, we also demonstrate stable operation of high-voltage LiNi0.8Co0.1Mn0.1O2 cathode in both coin and pouch cells under high loading, limiting excess lithium, and lean electrolyte conditions, holding great prospects for the practical application of high-voltage lithium-metal batteries.
Aqueous Zn-metal battery has been regarded as the most scalable system for grid-scale energy storage, yet challenges arise from arbitrary dendrite growth and Zn anode corrosion, thus restricting its practical application. Herein, a strong donor cosolvent (hexamethylphosphoramide, HMPA) is introduced to enable highly reversible Zn anode. It is demonstrated that the HMPA can preferentially adsorb on the surface of Zn as well as regulate the solvation structure of Zn 2+ by excluding H 2 O from the solvation sheath and thus weakens the activity of H 2 O, which contributes to a dense and uniform SEI layer that enables the homogeneous Zn electrodeposition. Owing to the above advantages, the resultant HMPA-containing electrolyte enables highly reversible Zn plating/stripping for thousands of cycles in Zn||Ti and Zn||Zn cells. Consequently, the cycling stability of Zn|| V 2 O 5 full cells is also significantly improved with a high capacity of 155 mAh g −1 maintained after 1500 cycles.
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