Graphene/hBN Heterostructures as High-Capacity Cathodes with High Voltage for Next-Generation Aluminum Batteries

Abstract

The field of Al batteries immensely demands the development of highly efficient cathode materials which can provide large storage capacities along with maintaining a constant high voltage. In this work, using the firstprinciples calculations, we have proposed the graphene/hexagonal boron nitride heterostructure (G/hBN) as a suitable cathode material for Al batteries. We have systematically investigated the binding, electronic, and electrochemical properties for the AlCl 4 -adsorbed/intercalated G/hBN heterostructure in various possibilities, and a necessary comparison has also been executed with the pristine monolayer of graphene and hBN. It is observed that the binding strength of AlCl 4 has significantly improved on the outer surfaces of graphene and hBN and in interlayer spaces of the G/hBN heterostructure compared to monolayer hBN, besides maintaining a similar strong binding as that of monolayer graphene. The lower diffusion barrier (0.01 eV) ensures a faster charge/discharge rate in the G/hBN heterostructure as the Al battery cathode. On systematically observing the incorporation of AlCl 4 in G/hBN through the voltage profile study, it is determined that the G/hBN heterostructure can deliver both a high voltage of 2.14 V as well as a high storage capacity of 183 mA h/g, whereas monolayers of graphene and hBN are either good at delivering higher storage capacity or better net voltage. All of these results motivate us toward the usage of the G/hBN heterostructure as the potential cathode material for the Al battery and provide valuable insights into the exploration of other 2D heterostructures for the highly efficient Al batteries.

Superior anchoring effect of a Cu-benzenehexathial MOF as an aluminium–sulfur battery cathode host

“…4,5 These ionic liquid based Al batteries are proposed to work in two distinctive reversible energy storage mechanisms depending upon the applicability of the cathode materials, one is intercalation reaction and another is conversion reaction. As the chloroaluminate ionic liquid electrolyte consists of Al ion in the form of both cation and anions, so both Al 3+ and AlCl 4can undergo intercalation in rocking chair type Al batteries [6][7][8][9][10][11][12][13][14][15][16] and Al dual-ion batteries, [17][18][19][20][21][22][23][24][25][26][27][28][29][30] respectively. The rocking chair Al batteries are reported to furnish high capacity (~300 mAh/g) but are limited by their small cycle life (<20 cycles), coulombic efficiency and cell voltage range (~0.6 V), whereas Al dual-ion batteries can deliver higher voltage (~2.0 V) with fast charge/discharge rates, but have low storage capacity (<120 mAh/g) and involve large volume expansion due to the involvement of large sized anion, 31 which can cause irreversible damage to the battery.…”

Identification of Non‐Carbonaceous Cathodes in Al Batteries: Potential Applicability of Black and Blue Phosphorene Monolayers

“…These structural variations have definitely improved the overall performance of Al batteries in terms of increased voltage, higher cycle life and better storage. On the other hand, several theoretical studies have also tried to investigate the involved electrochemistry along with analyzing the feasibility of BC 3 , single‐walled carbon nanotubes, C 3 N, and G/hBN cathodes other than graphite. All of these cathode materials have shown improvement of either voltage or storage capacity compared to graphite and their experimental availability makes them feasible towards practical usage.…”

Recent Trends in Electrode and Electrolyte Design for Aluminum Batteries

“…Various theoretical insights can be gained from our works regarding such reduced dimensional materials. 11f , 16 One such work demonstrated the applicability of single-walled carbon nanotubes as the cathode material. 16a Due to the availability of hollow spaces and porous nature, it can intercalate anions without interlayer expansion unlike 3D graphite.…”