Li‐ion Capacitor via Solvent‐Co‐Intercalation Process from Spent Li‐ion Batteries

Abstract

Li‐intercalation into graphite is the key underlying mechanism in the energy storage process. However, the intercalation of solvated Li‐ion/co‐intercalation of Li‐ion into graphite is considered unfitting, as it can initiate exfoliation of graphene layers. But later, it is revealed that co‐intercalation of Li does not destroy graphene layers and the compatibility of graphite host; moreover, the type of lithiated solvent molecule decides the reversibility of co‐intercalation process. Here, we report the fabrication of glyme‐based Li‐ion capacitors (LIC). The battery‐type electrode, graphite, is recovered from a spent Li‐ion battery (LIB) and serves as an anode, active along with a commercial activated carbon cathode. The assembled LIC with a co‐intercalation mechanism could deliver a maximum energy density of ∼46.40 Wh kg−1 at ambient temperature conditions. In addition, the performance of LIC is studied at various temperature conditions to ensure compatibility at different environmental conditions. The developed dual‐carbon LICs with low cost and high performance using recovered graphite as the anode can be considered as a real solution for recycling spent LIBs in an effective way by incorporating the waste‐to‐wealth approach.

Solvent Co-intercalation: An Emerging Mechanism in Li-, Na-, and K-Ion Capacitors

“…10,12,13,15,65 Considering the previous reports on solvated Li-ion intercalation in graphite lattice, our group recently established the assembly of a dual carbon cointercalation-based LIC. 58 The device used 1 M LiPF 6 in G 4 electrolyte, a spent LIB recovered graphite (RG) anode, and a commercial AC cathode. RG acts as a co-intercalation-type battery electrode to intercalate glyme-solvated Li-ions; AC serves as an EDLC-type electrode that undergoes adsorption− desorption of anions on the electrode surface.…”

“…21,66−69 Graphite, the state-of-art anode material for LICs, was considered unsuitable for NIC application as Na can hardly intercalate into graphite host lattices. Amazingly, Adelhelm's and Kang's research groups 28,53 58 Na + -ion 1.73 × 10 −7 cm 2 s −1 (anodic) Na + -ion 10 −13 −10 −14 cm 2 s −1 1.16 × 10 −7 cm 2 s −1 (cathodic) (PITT method) 63 (Randles−Sevsik equation) 59 (1−6) × 10 −10 cm 2 s −1 (GITT method) 62 K + -ion 3.0 × 10 −8 cm 2 s −1 K + -ion 6.1 × 10 −10 cm 2 s −1 (Randles−Sevsik equation) 56 (Randles−Sevsik equation) 56 ∼5 × 10 −8 cm 2 s −1 ∼10 −10 cm 2 s −1 (GITT method) 56 (GITT method) 56 diversity of chemistry high low explored whether sodium could reversibly insert into a graphite host using the idea of the co-intercalation phenomenon. By considering the reported works on co-intercalation-based graphite anodes, Han et al 70 established a NIC with a sodium-inserted graphitic meso-carbon microbead (MCMB) anode and an AC cathode in a G 2 -based electrolyte.…”

“…LICs are assembled to accomplish higher energy storage capacity than typical EDLC and higher power storage capability than LIBs. They employ a pre-lithiated battery-type anode and a capacitor-type cathode. ,,,, Considering the previous reports on solvated Li-ion intercalation in graphite lattice, our group recently established the assembly of a dual carbon co-intercalation-based LIC . The device used 1 M LiPF 6 in G 4 electrolyte, a spent LIB recovered graphite (RG) anode, and a commercial AC cathode.…”

MnCO3 Cuboids from Spent LIBs: A New Age Displacement Anode to Build High‐Performance Li‐Ion Capacitors

“…A similar performance was observed for the solvation-interaction process of Li-into the graphite, in which the graphite electrode exhibits better compatibility with the AC electrode than metallic Li. [41,42] Furthermore, the capacity fading issues can be efficiently eased by introducing conductive networks like graphene (regenerated from the spent battery graphite anode), which is our next target to improve the recycling process to build low-cost LIC without compromising energy and durability.…”

Pencil Scripted Ultrathin Graphene Nanostructure as Binder‐Free Battery‐Type Electrode for Li‐Ion Micro‐Capacitors with Excellent Performance

“…This clearly indicates that the 10B PG sample contains a significant amount of sp 2 carbon. The deconvoluted O 1 s spectra showed Lorentzian peaks at 532.28, 533.6, and 531 eV, which are associated with C–O, COO‐, and C = O functionalities, respectively, [ 28,29 ] as shown in Figure 1d. Deconvolution of Si 2 p spectra shows two main components at 99.92 and 102.87 eV corresponding to SiO x and SiO x /Si–O–C, respectively, [ 30 ] as shown in Figure 1e.…”