Large Spin‐Relaxation Barriers for the Low‐Symmetry Organolanthanide Complexes [Cp*2Ln(BPh4)] (Cp*=pentamethylcyclopentadienyl; Ln=Tb,Dy)

Single‐molecule magnets comprising one spin center represent a fundamental size limit for spin‐based information storage. Such an application hinges upon the realization of molecules possessing substantial barriers to spin inversion. Axially symmetric complexes of lanthanides hold the most promise for this due to their inherently high magnetic anisotropies and low tunneling probabilities. Herein, we demonstrate that strikingly large spin reversal barriers of 216 and 331 cm^?1 can also be realized in low‐symmetry lanthanide tetraphenylborate complexes of the type [Cp*₂Ln(BPh₄)] (Cp*=pentamethylcyclopentadienyl; Ln=Tb ( 1 ) and Dy ( 2 )). The dysprosium congener showed hysteretic magnetization data up to 5.3 K. Further studies of the magnetic relaxation processes of 1 and 2 under applied dc fields and upon dilution within a matrix of [Cp*₂Y(BPh₄)] revealed considerable suppression of the tunneling pathway, emphasizing the strong influence of dipolar interactions on the low‐temperature magnetization dynamics in these systems.     

Solvent-derived Fluorinated Secondary Interphase for Reversible Zn-graphite Dual-ion Batteries

The irreversibility of anion intercalation-deintercalation is a fundamental issue in determining the cycling stability of a dual-ion battery (DIB). In this work, we demonstrate that using a partially fluorinated carbonate solvent can drive a beneficial fluorinated secondary interphase layer formation. Such layer facilitates reversible anion (de−)intercalation processes by impeding solvent molecule co-intercalation and the associated graphite exfoliation. The enhanced reversibility of anion transport contributes to the overall cycling stability for a Zn-graphite DIB—a high Coulombic efficiency of 98.5 % after 800 cycles, with an attractive discharge capacity of 156 mAh g⁻¹ and a mid-point discharge voltage of ≈1.7 V (at 0.1 A g⁻¹). In addition, the formed fluorinated secondary interphase suppresses the self-discharge behavior, preserving 29 times of the capacity retention rate compared to the battery with a commonly used carbonate solvent, after standing for 24 hours. This work provides a simple and effective strategy for addressing the critical challenges in graphite-based DIBs and contributes to fundamental understanding to help accelerate their practical application.