Lithium−sulfur (Li−S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithium sulfide (Li 2 S) oxidation reactions during discharge− charge processes hinder their practical applications. Herein, under the guidance of density functional theory calculations, we have successfully synthesized large-scale single atom vanadium catalysts seeded on graphene to achieve high sulfur content (80 wt % sulfur), fast kinetic (a capacity of 645 mAh g −1 at 3 C rate), and long-life Li−S batteries. Both forward (sulfur reduction) and reverse reactions (Li 2 S oxidation) are significantly improved by the single atom catalysts. This finding is confirmed by experimental results and consistent with theoretical calculations. The ability of single metal atoms to effectively trap the dissolved lithium polysulfides (LiPSs) and catalytically convert the LiPSs/Li 2 S during cycling significantly improved sulfur utilization, rate capability, and cycling life. Our work demonstrates an efficient design pathway for single atom catalysts and provides solutions for the development of high energy/power density Li−S batteries.

Single-atom catalysts (SACs) are the smallest entities for catalytic reactions with projected high atomic efficiency, superior activity, and selectivity; however, practical applications of SACs suffer from a very low metal loading of 1-2 wt%. Here, a class of SACs based on atomically dispersed transition metals on nitrogen-doped carbon nanotubes (MSA-N-CNTs, where M = Ni, Co, NiCo, CoFe, and NiPt) is synthesized with an extraordinarily high metal loading, e.g., 20 wt% in the case of NiSA-N-CNTs, using a new multistep pyrolysis process. Among these materials, NiSA-N-CNTs show an excellent selectivity and activity for the electrochemical reduction of CO to CO, achieving a turnover frequency (TOF) of 11.7 s at -0.55 V (vs reversible hydrogen electrode (RHE)), two orders of magnitude higher than Ni nanoparticles supported on CNTs.

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Vacancy engineering is a promising approach for optimizing the energy storage performance of transition metal dichalcogenides (TMDs) due to the unique properties of vacancies in manipulating the electronic structure and active sites. Nevertheless, achieving effective introduction of anion vacancies with adjustable vacancy concentration on a large scale is still a big challenge. Herein, MoS 2(1−x) Se 2x alloys with anion vacancies introduced in situ have been achieved by a simple alloying reaction, and the vacancy concentration has been optimized through adjusting the chemical composition. Experimental and density functional theory calculation results suggest that the anion vacancies in MoS 2(1−x) Se 2x alloys could enhance the electronic conductivity, induce more active sites, and alleviate structural variation in the alloys during the potassium storage process. When applied as potassium ion battery anodes, the most optimized vacancy-rich MoSSe alloy delivered high reversible capacities of 517.4 and 362.4 mAh g −1 at 100 and 1000 mA g −1 , respectively. Moreover, a reversible capacity of 220.5 mAh g −1 could be maintained at 2000 mA g −1 after 1000 cycles. This work demonstrates a practical approach to modifying the electronic and defect properties of TMDs, providing an effective strategy for constructing advanced electrode materials for battery systems.

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