High energy {010} facets are favorable for Li+ transport in a layered Ni-rich LiNi0.6Co0.2Mn0.2O2 cathode through two-dimensional channels that are perpendicular to the c axis. However, those planes can hardly be maintained during the synthesis of layered cathodes. Therefore, we provide a strategy to use appropriate surface active agents which can alter the surface free energy by reducing surface tension directly. Here, a novel self-assembled 3D flower-like hierarchical LiNi0.6Co0.2Mn0.2O2 is formed with the help of sodium dodecyl sulfate (SDS), and those high energy facets are preserved. Due to the unique surface architectures which would lead to the fast ion transport kinetics as current expands to 100 times (from 0.1 to 10 C), the capacity decay only about 23.4%. Furthermore, full cells assembled against Li4Ti5O12 are constructed with a capacity retention of 80.61% at 1 C charge/discharge. This study could show a promising material model for the preferred orientation active planes and higher Li+ transport kinetics

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The introduction of "water-in-salt" electrolyte (WiSE) concept opens an ew horizon to aqueous electrochemistry that is benefited from the formation of as olidelectrolyte interphase (SEI). However,s uch SEI still faces multiple challenges,including dissolution, mechanical damaging, and incessant reforming,w hich result in poor cycling stability.Here,wereport apolymeric additive,polyacrylamide (PAM) that effectively stabilizes the interphase in WiSE. With the addition of 5m olar %P AM to 21 mol kg À1 LiTFSI electrolyte,aLiMn 2 O 4 k L-TiO 2 full cell exhibits enhanced cycling stability with 86 %capacity retention after 100 cycles at 1C.The formation mechanism and evolution of PAM-assisted SEI was investigated using operando small angle neutron scattering and density functional theory (DFT) calculations, which reveal that PAMm inimizes the presence of free water molecules at the anode/electrolyte interface,a ccelerates the TFSI À anion decomposition, and densifies the SEI.

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with CP-131 electrolyte exhibits high energy efficiency (86%, 1 C) and good cycle stability (89% retention after 500 cycles at 5 C), owing to effective SEI and CEI formation during the initial charge/discharge cycles that suppress HER effectively. A flexible LMO||LTO pouch cell with CP-131 electrolyte shows similar cycle capability to the corresponding coin cells even at different bending angles. A capacity retention of 86% is maintained at 0 °C, demonstrating wide range of service temperature. These results highlight that WiETGs electrolytes have the potential to be widely used for high-safety flexible electronic devices.

The formation of solid‐electrolyte interphase (SEI) in “water‐in‐salt” electrolyte (WiSE) expands the electrochemical stability window of aqueous electrolytes beyond 3.0 V. However, the parasitic hydrogen evolution reaction that drives anode corrosion, cracking, and the subsequent reformation of SEI still occurs, compromising long‐term cycling performance of the batteries. To improve cycling stability, an unsaturated monomer acrylamide (AM) is introduced as an electrolyte additive, whose presence in WiSE reduces its viscosity and improves ionic conductivity. Upon charging, AM electropolymerizes into polyacrylamide, as confirmed both experimentally and computationally. The in situ polymer constitutes effective protection layers at both anode and cathode surfaces, and enables LiMn2O4||L‐TiO2 full cells with high specific capacity (157 mAh g−1 at 1 C), long‐term cycling stability (80% capacity retention within 200 cycles at 1 C), and high rate capability (79 mAh g−1 at 30 C). The in situ electropolymerization found in this work provides an alternative and highly effective strategy to design protective interphases at the negative and positive electrodes for high‐voltage aqueous batteries of lithium‐ion or beyond.