Addressing adsorption and catalysis of lithium polysulfide via electronic distribution of molybdenum carbide host.

Heterostructure engineering is considered a crucial strategy to modulate the intrinsic charge transfer behavior of materials, enhance catalytic activity, and optimize sulfur electrochemical processes. However, parsing the role of heterogeneous interface-structure-property relationships in heterostructures is still a key scientific issue to realize the efficient catalytic conversion of polysulfides. Based on this, molybdenum carbide (Mo2C) was successfully partial reduced to molybdenum metal (Mo) via a thermal reduction at high-temperature and the typical Mo-Mo2C-based Mott-Schottky heterostructures were simultaneously constructed, which realized the modulation of the electronic structure of Mo2C and optimized the conversion process of lithium polysulfides (LPS). Compared with single molybdenum carbide, the modulated molybdenum carbide acts as an electron donor with stronger Mo-S bonding strength as well as higher polysulfide adsorption energy, faster Li2S conversion kinetics, and greatly facilitates the adsorption → catalysis process of LPS. As a result, yolk-shell Mo-Mo2C heterostructure (C@Mo-Mo2C) exhibits excellent cycling performance as a sulfur host, with a discharge specific capacity of 488.41 mAh g-1 for C@Mo-Mo2C/S at 4 C and present an excellent high-rate cyclic performance accompanied by capacity decay rate of 0.08 % per cycle after 400 cycles at 2 C. Heterostructure-acting Mo2C electron distribution modulation engineering may contributes to the understanding of the structure-interface-property interaction law in heterostructures and further enables the efficient modulation of the chemical behavior of sulfur.

Manipulating Charge-Transfer Kinetics of Lithium-Rich Layered Oxide Cathodes in Halide All-Solid-State Batteries.

Employing lithium-rich layered oxide (LLO) as the cathode of all-solid-state batteries (ASSBs) is highly desired for realizing high energy density. However, the poor kinetics of LLO, caused by its low electronic conductivity and significant oxygen-redox-induced structural degradation, has impeded its application in ASSBs. Here, the charge transfer kinetics of LLO is enhanced by constructing high-efficiency electron transport networks within solid-state electrodes, which considerably minimizes electron transfer resistance. In addition, an infusion-plus-coating strategy is introduced to stabilize the lattice oxygen of LLO, successfully suppressing the interfacial oxidation of solid electrolyte (Li3 InCl6 ) and structural degradation of LLO. As a result, LLO-based ASSBs exhibit a high discharge capacity of 230.7 mAh g-1 at 0.1 C and ultra-long cycle stability over 400 cycles. This work provides an in-depth understanding of the kinetics of LLO in solid-state electrodes, and affords a practically feasible strategy to obtain high-energy-density ASSBs.

Emerging carbon-based flexible anodes for potassium-ion batteries: Progress and opportunities.

In recent years, carbon-based flexible anodes for potassium-ion batteries are increasingly investigated owing to the low reduction potential and abundant reserve of K and the simple preparation process of flexible electrodes. In this review, three main problems on pristine carbon-based flexible anodes are summarized: excessive volume change, repeated SEI growth, and low affinity with K+, which thus leads to severe capacity fade, sluggish K+ diffusion dynamics, and limited active sites. In this regard, the recent progress on the various modification strategies is introduced in detail, which are categorized as heteroatom-doping, coupling with metal and chalcogenide nanoparticles, and coupling with other carbonaceous materials. It is found that the doping of heteroatoms can bring the five enhancement effects of increasing active sites, improving electrical conductivity, expediting K+ diffusion, strengthening structural stability, and enlarging interlayer spacing. The coupling of metal and chalcogenide nanoparticles can largely offset the weakness of the scarcity of K+ storage sites and the poor wettability of pristine carbon-based flexible electrodes. The alloy nanoparticles consisting of the electrochemically active and inactive metals can concurrently gain a stable structure and high capacity in comparison to mono-metal nanoparticles. The coupling of the carbonaceous materials with different characteristics can coordinate the advantages of the nanostructure from graphite carbon, the defects and vacancies from amorphous carbon, and the independent structure from support carbon. Finally, the emerging challenges and opportunities for the development of carbon-based flexible anodes are presented.