Universal in Situ Crafted MO_x-MXene Heterostructures as Heavy and Multifunctional Hosts for 3D-Printed Li–S Batteries

Abstract

The Li–S battery has emerged as a promising next-generation system for advanced energy storage. Notwithstanding the recent progress, the problematic polysulfide shuttling, retarded sulfur redox, and low output of volumetric capacity remain daunting challenges toward its practicability. In response, this work demonstrates herein a universal approach to in situ craft MO x -MXene (M: Ti, V, and Nb) heterostructures as heavy and multifunctional hosts to harvest good battery performances with synchronous polysulfide immobilization and conversion. Theoretical calculations indicate that the in situ implanted oxides boost the reaction kinetics of polysulfide transformation without affecting the intrinsic conductivity of MXene. As a result, the representative VO x -V2C/S electrode enables a high volumetric capacity (offering 1645.98 mAh cm–3 at 0.2 C) and cycling stability (retaining 631.17 mAh cm–3 after 1500 cycles at 2.0 C with a capacity decay of 0.03% per cycle). More encouragingly, 3D-printed sulfur electrodes harnessing VO x -V2C hosts readily harvest an areal capacity of 9.74 mAh cm–2 at 0.05 C under an elevated sulfur loading of 10.78 mg cm–2, holding promise for the development of practically viable Li–S batteries.

Universal‐Descriptors‐Guided Design of Single Atom Catalysts toward Oxidation of Li2S in Lithium–Sulfur Batteries

“…We revealed that Δ E , Δ E (*LiS), and ICOHP can serve as distinguished descriptors for rationally designing potential catalysts of MN 4 @G catalyzing Li 2 S decomposition and next we extended this strategy to predict the catalytic performance of various types of 2D materials with dispersed atomic metals for Li 2 S decomposition. Recently, various strategies have been proposed to enhance the catalytic performances of SACs toward electrochemical reactions, which involve heterostructures [ 51 , 52 , 53 ] and heteroatoms dopants other than N to tailor the local atomic environments. [ 54 ] Therefore, we used Δ E , Δ E (*LiS), and ICOHP to search for enhanced catalytic performance compared to WN 4 @G and MoN 4 @G by introducing interface effect and S dopant to modulate electronic properties of active metal center.…”

Designing principles of advanced sulfur cathodes toward practical lithium‐sulfur batteries

“…218 Though the poor performance was attained due to the low electric conductivity of sulfur copolymer, this work indeed motivated tremendous efforts on regulating the employed ink and architecture for realizing sulfur loading cathodes with 3D printing. Subsequent works such as improving the conductivity of ink 217 or tailoring thickness and pores 219 were also reported. Impressively, a versatile 3D printed N-doped porous Ti 3 C 2 MXene framework was fabricated by Sun and coworkers.…”

Additive Manufacturing of Electrochemical Energy Storage Systems Electrodes

“…Recently, Wei et al introduced a metal oxide/MXene heterostructure for 3D-printed Li-S batteries. [153] Using a hydrothermal approach, they synthesized in situ MO x /MXene (M: Ti, V, Nb) heterostructures as S host. The heterostructure acted as a multifunctional host providing abundant active sites for Li 2 S n adsorption and catalytic activity.…”