A Computational Study of a Single‐Walled Carbon‐Nanotube‐Based Ultrafast High‐Capacity Aluminum Battery

Abstract

Exploring suitable electrode materials is a fundamental step toward developing Al batteries with enhanced performance. In this work, we explore using density functional theory calculations the feasibility of single-walled carbon nanotubes (SWNTs) as a cathode material for Al batteries. Carbon nanotubes with hollow structures and large surface area are able to overcome the difficulty of activating the opening of interlayer spaces as observed in graphite electrode during the first intercalation cycle. Our results show that AlCl binds strongly with the SWNT to result in an energetically and thermally stable AlCl -adsorbed SWNT system. Diffusion calculations show that the SWNT system allows ultrafast diffusion of AlCl with a more favorable inner surface diffusion than outer surface diffusion. Our charge-density difference and Bader atomic charge analysis confirm the oxidation of SWNT upon adsorption of AlCl , which shows a similar behavior to the previously studied graphite cathode. The average open-circuit voltage and AlCl storage capacity increases with increasing SWNT diameter and can be as high as 1.96 V and 275 mA h g in (25,25) SWNT relative to graphite (70 mA h g ). All of these properties show that SWNTs are a potential cathode material for high-performance Al batteries and should be explored further.

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

“…From previously studied Al batteries, [9][10][11][12][13][15][16][17][18] it is now clear that the carbon based cathodesp referentially stabilize the tetrahedral geometry of AlCl 4 and not planar, however it is also important to check the geometrical preference of AlCl 4 in monolayer of black and blue phosphorene. Therefore, both tetrahedral and planar geometries of AlCl 4 are examineda nd we observe that phosphorenem onolayers follow the same trend as that of carbon based cathodes by stabilizing tetrahedral geometry of AlCl 4 .N ext, to investigate the adsorption behavior of AlCl 4 on black and blue phosphorene monolayers,d ifferent sites have been considered in 4 4 1a nd 5 5 1s upercells, respectively as showni nF igure 1.…”

“…[4][5][6][7][8][9][10] Now,w hen we talk about cathodes, numerous cathode materials have been examined for Al batteries, which can reversibly intercalate and deintercalate AlCl 4 À during charging and discharging reactions, respectively. [11][12][13][14][15][16][17][18][19] Experimentally,different studies have been executed for Al batteriesc athode by diversifying the graphite at structural level, such as naturalg raphite, [1,9] graphite foam, [20] graphitic carbon paper, [8] few layered graphene sheets, [21,22] polypyren [23] etc. These structural variations have definitely improved the overall performance of Al batteries in terms of increased voltage, higherc yclel ife and better storage.…”

“…However,t ill now both experimental and theoretical studies have proposed only the carbon based materials as cathodes for Al batteries, and amongst these speciallyt he low dimensionalm aterials (2D ad 1D) have shown improved performance (in terms of storage capacity,c ycle stability,r ate performance, coulombic efficiencies and wide operation temperature range) over experimentally observed graphite. [13,18,[25][26][27][28] Therefore, it will be interesting to examineo ther low dimensionalm aterial which could be equally or more advantageous than graphite as Al battery electrode. More precisely,the monolayer materials have been considered as potential electrode materials with high-performance rechargeableb atteriesb ecause of their high surface-volume ratio and unique electronic properties compared to their bulk counterparts.…”

A New Anode for Lithium‐Ion Batteries Based on Single‐Walled Carbon Nanotubes and Graphene: Improved Performance through a Binary Network Design

“…[7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22] For example, single-walled carbon nanotube "paper" that is prepared by using vacuum filtration has been used as anodes in LIBs, thereby showingareversible dischargec apacity of about 400 mA hg À1 at ac urrent density of 0.08 mA cm À2 . [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22] For example, single-walled carbon nanotube "paper" that is prepared by using vacuum filtration has been used as anodes in LIBs, thereby showingareversible dischargec apacity of about 400 mA hg À1 at ac urrent density of 0.08 mA cm À2 .…”

“…Carbon nanomaterials, especially graphene and carbon nanotubes, are considered to be favorable alternatives to graphite anodes in lithium-ion batteries, owing to their high specific surfacea rea, electrical conductivity,a nd excellent mechanicalf lexibility. [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22] For example, single-walled carbon nanotube "paper" that is prepared by using vacuum filtration has been used as anodes in LIBs, thereby showingareversible dischargec apacity of about 400 mA hg À1 at ac urrent density of 0.08 mA cm À2 . [23] Despite its low capacity,t his flexible paper can be used directly as binder-free electrodes and holds great potentialf or applicationsi nf lexible batteries.…”