Ag‐Embedded Carbon Nanotube Bucky Papers for Lithium Metal Full Batteries

Lithium (Li) metal anodes have received significant attention owing to their high theoretical capacity and low redox potential. Herein, a 3D bucky paper‐based host is demonstrated, consisting of multi‐walled carbon nanotubes (MWCNT) and Ag nanoparticles, for the uniform and dense Li deposition. The as‐designed Ag‐embedded MWCNT bucky paper (Ag/MCBP) achieves low Li nucleation overpotentials and high coulombic efficiencies (CEs), owing to the high Li affinity of Ag nanoparticles and 3D electronically conductive, porous architecture of MWCNT. Consequently, the optimized sample of Ag/MCBP–10 delivers a high average CE of 99.31% over 150 cycles at 2 mA cm −2 and 4 mAh cm −2 in symmetric cells. The Li metal full batteries are configured pairing Li@Ag/MCBP–10 with lithium iron phosphate (LFP), lithium manganese iron phosphate (LMFP), and nickel‐rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811). The Li@Ag/MCBP–10||LFP full cells retain 95.65% of capacity after 100 cycles at 1C, while the Li@Ag/MCBP–10||LMFP full cells achieve 79.30% of capacity retention after 100 cycles at 0.5C. Moreover, the Li@Ag/MCBP–10||NCM811 full cells, with a high mass loading of NCM811 cathode (22 mg cm −2 , 4.4 mAh cm −2 ) deliver the high specific capacity of 208.74 mAh g −1 at 0.2C rate under harsh condition of ≈0.9 neutron‐to‐proton ratio.