Dispersion–Assembly Approach to Synthesize Three-Dimensional Graphene/Polymer Composite Aerogel as a Powerful Organic Cathode for Rechargeable Li and Na Batteries

Abstract

Polymer cathode materials are promising alternatives to inorganic counterparts for both lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs) due to their high theoretical capacity, adjustable molecular structure, and strong adaptability to different counterions in batteries, etc. However, they suffer from poor practical capacity and low rate capability because of their intrinsically poor conductivity. Herein, we report the synthesis of self-assembled graphene/poly(anthraquinonyl sufide) (PAQS) composite aerogel (GPA) with efficient integration of a three-dimensional (3D) graphene framework with electroactive PAQS particles via a novel dispersion-assembly strategy which can be used as a free-standing flexible cathode upon mechanical pressing. The entire GPA cathode can deliver the highest capacity of 156 mAh g at 0.1 C (1 C = 225 mAh g) with an ultrahigh utilization (94.9%) of PAQS and exhibits an excellent rate performance with 102 mAh g at 20 C in LIBs. Furthermore, the flexible GPA film was also tested as cathode for SIBs and demonstrated a high-rate capability with 72 mAh g at 5 C and an ultralong cycling stability (71.4% capacity retention after 1000 cycles at 0.5 C) which has rarely been achieved before. Such excellent electrochemical performance of GPA as cathode for both LIBs and SIBs could be ascribed to the fast redox kinetics and electron transportation within GPA, resulting from the interconnected conductive framework of graphene and the intimate interaction between graphene and PAQS through an efficient wrapping structure. This approach opens a universal way to develop cathode materials for powerful batteries with different metal-based counter electrodes.

Aromatic Polyimide/Graphene Composite Organic Cathodes for Fast and Sustainable Lithium‐Ion Batteries

“…Electronically conducting additives such as carbon, metals, and conductive polymers have shown to be effective for improving the high‐rate capability of polymeric‐cathode‐based batteries . So far, the main avenues of incorporating electron‐conducting additives include coating, fillers, composites, and matrix skeleton .…”

“…[25,26] Electronicallyc onducting additives such as carbon, metals, and conductive polymers have shown to be effective for improvingt he high-rate capability of polymeric-cathode-based batteries. [27][28][29][30][31][32][33][34][35] So far,t he main avenues of incorporating electron-conducting additives include coating, fillers, composites, and matrixs keleton. [33,[36][37][38] Amongt hem, conductive carbon fillers such as carbon nanotubes (CNTs) and graphene have been commonly used as electronically conductive additives for organic electrodes owing to their highe lectronic conductivity.…”

Recent advances on flexible electrodes for Na-ion batteries and Li–S batteries

“…80 2.0-0.01 ∼555 at 1600 620 (100) [43] 2 D -conjugated aromatic Polymer 2.5-0.005 105 at 10,0 0 0 ∼79(770 0)50 0 0 [44] http://engine.scichina.com/doi/10.1016/j.jechem.2018.06.011 Table 3. Working potential range, capacity, and cycling stability of recently reported several types of flexible cathode materials for SIBs [38,[86][87][88][89][90][91][92][93][94][95][96][97] .…”

“…Capacity retention in mAh g -1 (cycles) current density in mA g -1 Refs. [97] NF: nano-fiber; FWCNTs: few-walled carbon nano-tubes; NTs: nanotubes; CC: carbon cloth; MWCNTs: multi-walled carbon nano-tubes; NW: nanowire; CFC: carbon fiber cloth; PAQS: poly(anthraquinonyl sufide); GO: graphene oxide.…”

“…Hybridizing the potential cathode materials with carbonaceous materials such as carbon nano-fiber, carbon nano-tubes, graphene, cotton textiles, carbon cloth, and carbon fiber cloth is the useful strategy for the fabrication of flexible cathode materials for SIBs, which can also enhance high electronic/ionic conductivity and that enhance the electrochemical properties. Table 3 shows the working potential range, capacity, and cycling stability of recently reported several types of flexible cathode materials for SIBs [38,[86][87][88][89][90][91][92][93][94][95][96][97] . Carbon-nano-fibers matrix can provide high flexibility while their electrospinning synthesis process is a versatile technology.…”