Self‐Assembly of Flexible Free‐Standing 3D Porous MoS₂‐Reduced Graphene Oxide Structure for High‐Performance Lithium‐Ion Batteries

Abstract

Flexible freestanding electrodes are highly desired to realize wearable/flexible batteries as required for the design and production of flexible electronic devices. Here, the excellent electrochemical performance and inherent flexibility of atomically thin 2D MoS 2 along with the self-assembly properties of liquid crystalline graphene oxide (LCGO) dispersion are exploited to fabricate a porous anode for high-performance lithium ion batteries. Flexible, free-standing MoS 2 -reduced graphene oxide (MG) film with a 3D porous structure is fabricated via a facile spontaneous self-assembly process and subsequent freeze-drying. This is the first report of a one-pot self-assembly, gelation, and subsequent reduction of MoS 2 /LCGO composite to form a flexible, high performance electrode for charge storage. The gelation process occurs directly in the mixed dispersion of MoS 2 and LCGO nanosheets at a low temperature (70 °C) and normal atmosphere (1 atm). The MG film with 75 wt% of MoS 2 exhibits a high reversible capacity of 800 mAh g −1 at a current density of 100 mA g −1 . It also demonstrates excellent rate capability, and excellent cycling stability with no capacity drop over 500 charge/discharge cycles at a current density of 400 mA g −1 .

Functionalized Hybridization of 2D Nanomaterials

“…[21] As reported, thiol ligand modifications can readily occur on both internal and perimeter edges of MoS 2 nanosheets due to their higher molecular III: Hybridization of protons and semiconductor nanostructures on g-C 3 N 4 nanosheets g-C 3 N 4 Protons Sonication-driven exfoliation of g-C 3 N 4 in 10 m HCl Biosensor New heparin sensing platform with a detection limit of 18 ng mL −1 [163] g-C 3 N 4 Co 2 P nanorods Sonication-driven embedding of Co 2 P nanorods into g-C 3 N 4 nanosheets HER High H 2 production rate at 53.3 µmol g −1 h −1 (no H 2 evolution observed by using g-C 3 N 4 alone) [170] Li + battery Reversible capacity of 800 mA h g −1 at a current density of 100 mA g −1 , and no capacity drop over 500 charge/discharge cycles at a current density of 400 mA g −1 [240] affinities. [21] As reported, thiol ligand modifications can readily occur on both internal and perimeter edges of MoS 2 nanosheets due to their higher molecular III: Hybridization of protons and semiconductor nanostructures on g-C 3 N 4 nanosheets g-C 3 N 4 Protons Sonication-driven exfoliation of g-C 3 N 4 in 10 m HCl Biosensor New heparin sensing platform with a detection limit of 18 ng mL −1 [163] g-C 3 N 4 Co 2 P nanorods Sonication-driven embedding of Co 2 P nanorods into g-C 3 N 4 nanosheets HER High H 2 production rate at 53.3 µmol g −1 h −1 (no H 2 evolution observed by using g-C 3 N 4 alone) [170] Li + battery Reversible capacity of 800 mA h g −1 at a current density of 100 mA g −1 , and no capacity drop over 500 charge/discharge cycles at a current density of 400 mA g −1 [240] affinities.…”

“…[240] With 75 wt% MoS 2 , the resulting hybrids exhibited a high reversible capacity of 800 mA h g −1 at a current density of 100 mA g −1 , and demonstrated a superb rate capability and excellent cycling stability (e.g., no capacity drop was found over 500 charge/discharge cycles at a current density of 400 mA g −1 ). [240] With 75 wt% MoS 2 , the resulting hybrids exhibited a high reversible capacity of 800 mA h g −1 at a current density of 100 mA g −1 , and demonstrated a superb rate capability and excellent cycling stability (e.g., no capacity drop was found over 500 charge/discharge cycles at a current density of 400 mA g −1 ).…”

2D Metal Chalcogenides Incorporated into Carbon and their Assembly for Energy Storage Applications

“…Jalili et al found that liquid crystalline graphene oxide nanosheets (LCGO) possess a high aspect ratio and strong hydrogen bond force, and they can self‐assemble into various 3D porous architectures . When hybridized with other highly active electrode materials, the exceptional characteristics of LCGO can be well‐maintained . Inspired by these features, a flexible free‐standing electrode of a 3D porous MoS 2 /rGO (MG) aerogel‐based membrane was fabricated by the spontaneous self‐assembly of ultrathin MoS 2 nanosheets and LCGO .…”

“…When hybridized with other highly active electrode materials, the exceptional characteristics of LCGO can be well‐maintained . Inspired by these features, a flexible free‐standing electrode of a 3D porous MoS 2 /rGO (MG) aerogel‐based membrane was fabricated by the spontaneous self‐assembly of ultrathin MoS 2 nanosheets and LCGO . It is noted that the MoS 2 /LCGO dispersion with 75% MoS 2 content still exhibits liquid crystal order.…”

Enhanced Li‐Ion‐Storage Performance of MoS2 through Multistage Structural Design

“…[10] This inspires us to consider: whether the multistage structural design concept applicable to the folded proteins can be employed herein to create the advanced electrode materials for LIBs. [13][14][15][16] In recent years, various MoS 2 composites, [17][18][19][20][21][22][23][24][25][26][27] including MoS 2 /C, [19,20,23,24] SnS 2 /MoS 2 /CFC, [21] MoO 2 @MoS 2 [22] and S-MoS 2 @α-Fe 2 O 3 [26] have been widely exploited as important anode materials for lithium ion batteries (see Table S1). [13][14][15][16] In recent years, various MoS 2 composites, [17][18][19][20][21][22][23][24][25][26][27] including MoS 2 /C, [19,20,23,24] SnS 2 /MoS 2 /CFC, [21] MoO 2 @MoS 2 [22] and S-MoS 2 @α-Fe 2 O 3 [26] have been widely exploited as important anode materials for lithium ion batteries...…”