A 3D Lithiophilic Mo₂N‐Modified Carbon Nanofiber Architecture for Dendrite‐Free Lithium‐Metal Anodes in a Full Cell

Abstract

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 3dimensional (3D) framework configured with Mo 2 N-mofidied carbon nanofiber (CNF) architecture is established as a Li host via a facile fabrication method. The lithiophilic Mo 2 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 the Li-dendrite formation. As a result, the 3D hybrid Mo 2 N@CNF structure facilitates 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 Mo 2 N@CNF substrates stably operate over 1,500 h at 6 mA cm-2 for 6 mA h cm-2. Furthermore, full cells paired with LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NMC811) cathodes in conventional carbonate electrolytes achieve a remarkable capacity retention of 90% over 150 cycles. This

Rational Design of Multifunctional Integrated Host Configuration with Lithiophilicity‐Sulfiphilicity toward High‐Performance Li–S Full Batteries

“…Luo et al. [ 20 ] demonstrated that a 3D framework configured with lithiophilic Mo 2 N‐mofidied carbon nanofiber as a Li host can not only effectively guide a uniform Li nucleation and deposition, but also suppress the Li‐dendrite formation. On the S cathode side, restricting shuttle effect, providing enough space for the Li 2 S deposition, and improving the conductivity of S cathode leads to high‐performance Li–S batteries.…”

A Dual‐Functional Conductive Framework Embedded with TiN‐VN Heterostructures for Highly Efficient Polysulfide and Lithium Regulation toward Stable Li–S Full Batteries

“…The nucleation overpotential could reflect the energy barrier of Li nucleation, indicating the lithiophilicity of the substrate . Therefore, to further evaluate the lithiophilic feature of the TiN‐VN@CNF, nucleation overpotentials of Li on different substrates were measured at a current density of 1 mA cm −2 (Figure k).…”

“…Especially the electrode with Li excess only 100%, it displayed unstable cycling, low Coulombic efficiency and fast capacity decay. This may be ascribed to the controlled less Li excess, which inadequately compensate the Li loss by side reactions …”

Interconnected Two‐dimensional Arrays of Niobium Nitride Nanocrystals as Stable Lithium Host

“…This is followed by the rapid Li + diffusion in vertical direction within the host, facilitated by the presence of abundant pores between interconnected nanocrystals and spaces between nanosheets (Figure1b). Such a Li + redistribution process, combined with the naturally strong lithiophilicity of metal nitrides [31] and high electron conductivity of NbN‐based host (674 S cm −1 ) that lower the Li nucleation energy, [36] could lead to the fast and uniform Li + ion flux, and eventually smooth Li deposition. During the following cycling, fresh Li may migrate into 2D arrays of NbN nanocrystals and compensate for the depletion due to the “self‐filling” effect of mesopores [18] .…”