Interfacial and Electronic Modulation via Localized Sulfurization for Boosting Lithium Storage Kinetics

Abstract

Structural modulation endows electrochemical hybrids with promising energy storage properties owing to their adjustable interfacial and/or electronic characteristics. For MXene‐based materials, however, the facile but effective strategies for tuning their structural properties at nanoscale are still lacking. Herein, 3D crumpled S‐functionalized Ti3C2Tx substrate is rationally integrated with Fe3O4/FeS heterostructures via coprecipitation and subsequent partial sulfurization to induce a highly active and stable electrode architecture. The unique heterostructures with tuned electronic properties can induce improved kinetics and structural stability. The surface engineering by S terminations on the MXene further unlocks extra (pseudo)capacitive lithium storage. Serving as anode for lithium storage, the optimized electrode delivers an excellent long‐term cycling stability (913.9 mAh g−1 after 1000 cycles at 1 A g−1) and superior rate capability (490.4 mAh g−1 at 10 A g−1). Moreover, the (de)lithiation pathways associated with energy storage mechanisms are further revealed by operando X‐ray diffraction, in situ electroanalytical techniques, and first‐principles calculations. The hybrid electrode is proved to undergo stepwise phase transformations during discharging but a relatively uniform reconversion during charging, suggesting an asymmetric conversion mechanism. This work provides a novel strategy for designing high‐performance hybrids and paves the way for in‐depth understanding of complex lithium intercalation and conversion reactions.

Facile and Scalable Synthesis of Si@void@C Embedded in Interconnected 3D Porous Carbon Architecture for High Performance Lithium‐Ion Batteries

“…Commercial pure silicon particles (purchased from the company of Siping Changchun, China) were chosen as the starting materials. Owing to the positive charge from the Si particles, [ 23,24 ] the synthesis process takes advantage of hydrophilicity of silicon powder (Figure 1a and Figure S1a in the Supporting Information). First, in the water/oil system (Figure 1b), the added (3‐Aminopropyl) triethoxysilane coupling agent is compatible with organic substances (styrene monomer acted as oil phase).…”

Solid Electrolyte Interphases on Sodium Metal Anodes

“…The Na + transmission is fast in the larger ions transport channels because of the small electronegativity and large ionic radius of the sulfur atom. [173][174][175] Additionally, the synthesis of sulfide does not require excessively high temperatures, which can greatly reduce the grain boundary resistance, making it suitable for RT solid-state Na batteries. Reproduced with permission.…”

CoSe2/MoS2 Heterostructures to Couple Polysulfide Adsorption and Catalysis in Lithium‐Sulfur Batteries†

“…However, non‐polar surfaces of carbon‐based materials could not trap polar polysulfides sufficiently. [ 15 ] In view of this, polar materials such as metal oxides, [ 16‐17 ] sulfides, [ 18‐19 ] selenides, [ 20 ] phosphates, [ 21 ] nitrides [ 22 ] and carbides [ 23 ] have been developed as sulfur hosts to take advantages of their strong chemical interactions with polysulfides. Such strategies can effectively suppress the shuttling effect and modestly increase the utilization of active sulfur species.…”