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Numerous efforts are made to improve the reversible capacity and long‐term cycling stability of Li‐S cathodes. However, they are susceptible to irreversible capacity loss during cycling owing to shuttling effects and poor Li+ transport under high sulfur loading. Herein, a physically and chemically enhanced lithium sulfur cathode is proposed to address these challenges. Additive manufacturing is used to construct numerous microchannels within high sulfur loading cathodes, which enables desirable deposition mechanisms of lithium polysulfides and improves Li+ and e‐ transport. Concurrently, cobalt sulfide is incorporated into the cathode composition and demonstrates strong adsorption behavior toward lithium polysulfides during cycling. As a result, excellent electrochemical performance is obtained by the design of a physically and chemically enhanced lithium sulfur cathode. The reported electrode, with a sulfur loading of 8 mg cm‐2, delivers an initial capacity of 1118.8 mA h g‐1 and a reversible capacity of 771.7 mA h g‐1 after 150 cycles at a current density of 3 mA cm‐2. This work demonstrates that a chemically enhanced sulfur cathode, manufactured through additive manufacturing, is a viable pathway to achieve high‐performance Li‐S batteries. [ABSTRACT FROM AUTHOR]

Lithium–sulfur batteries are deemed as optimal energy devices for the next generation of high‐energy‐density energy storage. However, several problems such as low energy density and short cycle life hinder their application in industry. Here, MoS2–MoN heterostructure nanosheets grown on carbon nanotube arrays as free‐standing cathodes are reported. In this heterostructure, MoN works as a promoter to provide coupled electrons to accelerate the redox reaction of polysulfides while the MoS2, with a two‐dimensional layered structure, provides smooth Li+ diffusion pathways. Through their respective advantages, both MoN and MoS2 could mutually boost the process of "adsorption‐diffusion‐conversion" of polysulfides, which have a synergy enhancement effect to restrain the lithium polysulfides from shuttling. The designed cathodes show excellent long‐term cycling performances of 1000 cycles at 1C with a low decay rate of 0.039% per cycle and a high rate capability up to 6C. A high initial areal capacity of 13.3 mAh cm−2 is also achieved under a low electrolyte volume/sulfur loading (E/S) ratio of 6.3 mL g−1. This strategy of promoting polysulfide conversion by heterostructure MoS2–MoN as presented in this work can provide a more structured design strategy for future advanced Li–S energy storage systems. [ABSTRACT FROM AUTHOR]

Although metallic lithium is regarded as the "Holy Grail" for next‐generation rechargeable batteries due to its high theoretical capacity and low overpotential, the uncontrollable Li dendrite growth, especially under high current densities and deep plating/striping, has inhibited its practical application. Herein, a 3D‐printed, vertically aligned Li anode (3DP‐VALi) is shown to efficiently guide Li deposition via a "nucleation within microchannel walls" process, enabling a high‐performance, dendrite‐free Li anode. Moreover, the microchannels within the microwalls are beneficial for promoting fast Li+ diffusion, supplying large space for the accommodation of Li during the plating/stripping process. The high‐surface‐area 3D anode design enables high operating current densities and high areal capacities. As a result, the Li–Li symmetric cells using 3DP‐VALi demonstrate excellent electrochemical performances as high as 10 mA cm−2/10 mAh cm−2 for 1500 h and 5 mA cm−2/20 mAh cm−2 for 400 h, respectively. Additionally, the Li–S and Li–LiFePO4 cells using 3DP‐VALi anodes present excellent cycling stability up to 250 and 800 cycles at a rate of 1 C, respectively. It is believed that these new findings could open a new window for dendrite‐free metal anode design and pave the way toward energy storage devices with high energy/power density. [ABSTRACT FROM AUTHOR]

An aligned and laminated sulfur-absorbed mesoporous carbon/carbon nanotube (CNT) hybrid cathode has been developed for lithium-sulfur batteries with high performance. The mesoporous carbon acts as sulfur host and suppresses the diffusion of polysulfide, while the CNT network anchors the sulfur-absorbed mesoporous carbon particles, providing pathways for rapid electron transport, alleviating polysulfide migration and enabling a high flexibility. The resulting lithium-sulfur battery delivers a high capacity of 1226 mAh g−1 and achieves a capacity retention of 75 % after 100 cycles at 0.1 C. Moreover, a high capacity of nearly 900 mAh g−1 is obtained for 20 mg cm−2, which is the highest sulfur load to the best of our knowledge. More importantly, the aligned and laminated hybrid cathode endows the battery with high flexibility and its electrochemical performances are well maintained under bending and after being folded for 500 times. [ABSTRACT FROM AUTHOR]

The application of Li‐S batteries is hindered by low sulfur utilization and rapid capacity decay originating from slow electrochemical kinetics of polysulfide transformation to Li2S at the second discharge plateau around 2.1 V and harsh shuttling effects for high‐S‐loading cathodes. Herein, a cobalt‐doped SnS2 anchored on N‐doped carbon nanotube (NCNT@Co‐SnS2) substrate is rationally designed as both a polysulfide shield to mitigate the shuttling effects and an electrocatalyst to improve the interconversion kinetics from polysulfides to Li2S. As a result, high‐S‐loading cathodes are demonstrated to achieve good cycling stability with high sulfur utilization. It is shown that Co‐doping plays an important role in realizing high initial capacity and good capacity retention for Li‐S batteries. The S/NCNT@Co‐SnS2 cell (3 mg cm−2 sulfur loading) delivers a high initial specific capacity of 1337.1 mA h g−1 (excluding the Co‐SnS2 capacity contribution) and 1004.3 mA h g−1 after 100 cycles at a current density of 1.3 mA cm−2, while the counterpart cell (S/NCNT@SnS2) only shows an initial capacity of 1074.7 and 843 mA h g−1 at the 100th cycle. The synergy effect of polysulfide confinement and catalyzed polysulfide conversion provides an effective strategy in improving the electrochemical performance for high‐sulfur‐loading Li‐S batteries. The S/NCNT@Co‐SnS2 material acts as not only an effective shuttle‐suppressing shield for polysulfide but also an electrocatalyst in improving sulfur utilization and cycling stability for high‐sulfur‐loading lithium‐sulfur batteries. Therefore, it maintains 1004.3 mA h g−1 after 100 cycles at a current density of 1.3 mA cm−2. [ABSTRACT FROM AUTHOR]