A 3D Lithiophilic Mo2 N-Modified Carbon Nanofiber Architecture for Dendrite-Free Lithium-Metal Anodes in a Full Cell.

The pursuit for high-energy-density batteries has inspired the resurgence of metallic lithium (Li) as a promising anode, yet its practical viability is restricted by the uncontrollable Li dendrite growth and huge volume changes during repeated cycling. Herein, a new 3D framework configured with Mo2 N-mofidied carbon nanofiber (CNF) architecture is established as a Li host via a facile fabrication method. The lithiophilic Mo2 N acts as a homogeneously pre-planted seed with ultralow Li nucleation overpotential, thus spatially guiding a uniform Li nucleation and deposition in the matrix. The conductive CNF skeleton effectively homogenizes the current distribution and Li-ion flux, further suppressing Li-dendrite formation. As a result, the 3D hybrid Mo2 N@CNF structure facilitates a dendrite-free morphology with greatly alleviated volume expansion, delivering a significantly improved Coulombic efficiency of ≈99.2% over 150 cycles at 4 mA cm-2 . Symmetric cells with Mo2 N@CNF substrates stably operate over 1500 h at 6 mA cm-2 for 6 mA h cm-2 . Furthermore, full cells paired with LiNi0.8 Co0.1 Mn0.1 O2 (NMC811) cathodes in conventional carbonate electrolytes achieve a remarkable capacity retention of 90% over 150 cycles. This work sheds new light on the facile design of 3D lithiophilic hosts for dendrite-free lithium-metal anodes.