How to simultaneously restrain the loss of active species and facilitate the conversion reaction under high S loading condition is the key to solve the commercialization of Li–S batteries. For this system, the availability of raw materials and simplicity (high efficiency) of synthetic strategies are also important factors. Herein, we propose an interlaced two-dimensional (2D) carbon material as advanced Li–S cathode host characterized by corrugated monolithic morphology and Co/N dopants as dual lithiophilic–sulfiphilic sites. This 2D structure is derived from a cheap biomass precursor, adenine, with bonding interaction with a MgCl2 hydrate template via a facile ionothermal method. It allows a homogeneous spatial distribution of S/Li2S deposits and strong adsorbability and enhanced conversion kinetics for polysulfides. Benefiting from the synergistic effects of corrugated 2D conductive matrix and embedded heteroatom/nanodot catalyst, the resultant sulfur cathode releases a high specific capacity of 1290.4 mA h g–1 at 0.2 C, small capacity fading rate of 0.029% per cycle over 600 cycles at 2 C, superior rate performance up to 20 C, and considerable areal capacity retention of 6.0 mA h cm–2 even under an ultrahigh sulfur loading up to 9.7 mg cm–2.

A cathode host with strong sulfur/polysulfide confinement and fast redox kinetics is a challenging demand for high-loading lithium−sulfur batteries. Recently, porous carbon hosts derived from metal−organic frameworks (MOFs) have attracted wide attention due to their unique spatial structure and customizable reaction sites. However, the loading and rate performance of Li−S cells are still restricted by the disordered pore distribution and surface catalysis in these hosts.Here, we propose a concept of built-in catalysis to accelerate lithium polysulfide (LiPSs) conversion in confined nanoreactors, i.e., laterally stacked ordered crevice pores encompassed by MoS 2 -decorated carbon thin layers. The functions of Sfixability and LiPS catalysis in these mesoporous cavity reactors benefit from the 2D interface contact between ultrathin catalytic MoS 2 and conductive C pyrolyzed from Al-MOF. The integrated function of adsorption−catalysis−conversion endows the sulfur-infused C@MoS 2 electrode with a high initial capacity of 1240 mAh g −1 at 0.2 C, long life cycle stability of at least 1000 cycles at 2 C, and high rate endurance up to 20 C. This electrode also exhibits commercial potential in view of considerable capacity release and reversibility under high sulfur loading (6 mg cm −2 and ∼80 wt %) and lean electrolyte (E/S ratio of 5 μL mg −1 ). This study provides a promising design solution of a catalysis−conduction 2D interface in a 3D skeleton for high-loading Li−S batteries.

Herein, we propose the construction of asandwichstructured host filled with continuous 2D catalysis-conduction interfaces.T his MoN-C-MoN trilayer architecture causes the strong conformal adsorption of S/Li 2 S x and its high-efficiency conversion on the two-sided nitride polar surfaces,w hich are supplied with high-flux electron transfer from the buried carbon interlayer.The 3D self-assembly of these 2D sandwich structures further reinforces the interconnection of conductive and catalytic networks.The maximized exposure of adsorptive/ catalytic planes endows the MoN-C@S electrode with excellent cycling stability and high rate performance even under high S loading and lowhost surface area. The high conductivity of this trilayer texture does not compromise the capacity retention after the Sc ontent is increased. Suchajob-synergistic mode between catalytic and conductive functions guarantees the homogeneous deposition of S/Li 2 S x ,a nd avoids thicka nd devitalized accumulation (electrode passivation) even after high-rate and long-term cycling.

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A vulnerable solid–electrolyte interphase (SEI) layer cannot retard Li dendrite growth, electrolyte consumption, and anode volumetric expansion, which seriously hinders the development of high‐safety Li‐metal batteries (LMBs). Herein, a dynamical SEI reinforced by an open‐architecture metal–organic framework (OA‐MOF) film characterized by elastic expansion and contraction of the volume of stereoscopic lithiophilic sites, is designed. The self‐adjustment distribution of lithiophilic sites on vertically grown Cu2(BDC)2 nanosheets enables the homogenization of Li‐ion flux, smart control of Li mass transport, and compaction of Li deposition. The trapped N, N‐dimethylformamide molecules in the open framework structure are favorable for the better wetting and dissolution effect of Li‐ions accessing to Cu2(BDC)2. Combining these advantages, the featured OA‐MOF/Cu@Li anode enables a high coulombic efficiency and low voltage hysteresis in Li||Cu cells even at an ultrahigh current density of 15 mA cm−2.

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All-solid-state batteries are appealing electrochemical energy storage devices because of their high energy content and safety. However, their practical development is hindered by inadequate cycling performances due to poor reaction reversibility, electrolyte thickening and electrode passivation. Here, to circumvent these issues, we propose a fluorination strategy for the positive electrode and solid polymeric electrolyte. We develop thin laminated all-solid-state Li||FeF3 lab-scale cells capable of delivering an initial specific discharge capacity of about 600 mAh/g at 700 mA/g and a final capacity of about 200 mAh/g after 900 cycles at 60 °C. We demonstrate that the polymer electrolyte containing AlF3 particles enables a Li-ion transference number of 0.67 at 60 °C. The fluorinated polymeric solid electrolyte favours the formation of ionically conductive components in the Li metal electrode’s solid electrolyte interphase, also hindering dendritic growth. Furthermore, the F-rich solid electrolyte facilitates the Li-ion storage reversibility of the FeF3-based positive electrode and decreases the interfacial resistances and polarizations at both electrodes.