Anode‐Free Aluminum Electrode with Ultralong Cycle Life and High Coulombic Efficiency Exceeding 99.92% Enabled by a Lattice‐Matching Layer

Abstract

Metallic aluminum is an attractive anode owing to its high specific capacity, earth abundance, and low cost. However, the poor reversibility of Al deposition/dissolution and Al dendrites have impeded its deployment. Herein, a strategy for constructing a lattice‐matching layer (LML) to regulate the behavior of Al deposition/dissolution is demonstrated. Various experiments and theoretical calculations validate that gold LML as an example can significantly enhance the nucleation density and reduce average particle size, which achieve highly reversible, dendrite‐free, durable, and anode‐free Al anodes. The metallic Al shows stable Al deposition/dissolution on Au@Ti substrate for more than 4500 h with an average Coulombic efficiency of 99.92%, which is a record‐high reported value. Furthermore, the anode‐free full cell based on Au@Ti anode and expanded graphite cathode exhibits outstanding long‐term stability for 900 cycles with the capacity retention rate of 80%. This study provides an effective strategy to enhance the reversibility and utilization of the Al anode, which provides inspiration for advanced Al batteries.

MXene-Based Mixed Conductor Interphase for Dendrite-Free Flexible Al Organic Battery

“…Figure 3f and Table S1 compare the electrochemical performance of MAl-80 with some previously reported modified Al metal anodes in the literatures. [20][21][22][23][24]28 It can be seen that the electrochemical performance of MAl-80 exhibits significant advances compared with the data reported so far. SEM and surface 3D topography were used to further validate the role of the MXene protective layer in inhibiting dendritic growth.…”

“…22 Au lattice-matching layer can significantly enhance the Al nucleation density, which achieve highly reversible, dendrite-free, durable, and anode-free Al anodes. 23 In addition, designing Al metal anodes with special structures has been proven to be another feasible solution. Yang et al recommended porous aluminum as the anode.…”

“…A 3D-structured MXene paper electrode was fabricated to protect Al deposition/dissolution reactions with improved redox kinetics . Au lattice-matching layer can significantly enhance the Al nucleation density, which achieve highly reversible, dendrite-free, durable, and anode-free Al anodes . In addition, designing Al metal anodes with special structures has been proven to be another feasible solution.…”

Aqueous all-manganese batteries

“…[6][7][8][9] In recent years, a large number of rechargeable aqueous metal ion batteries have been widely reported, including aqueous Li, sodium (Na), potassium (K) and calcium (Ca) ion batteries based on the rocking-chair ion storage, [10][11][12][13] and aqueous copper (Cu), iron (Fe), zinc (Zn), aluminum (Al), and magnesium (Mg) metal batteries based on the anode metal plating/stripping mechanisms. [14][15][16][17][18][19][20][21][22][23][24][25] However, the former showed low actual output voltages and limited energy densities, 6,8 while the latter showed high theoretical capacity with the greatest atomic economy by using plating/stripping of metals as anodes. 6,8,26 Nevertheless, the redox potentials of Cu, Fe, and Zn metal anodes are relatively high, resulting in low battery voltages and unsatisfactory energy densities.…”