Inorganic Polysulfide Chemistries for Better Energy Storage Systems.

ConspectusSulfur-based cathode materials have become a research hot spot as one of the most promising candidates for next-generation, high-energy lithium batteries. However, the insulating nature of elemental sulfur or organosulfides has become the biggest challenge that leads to dramatic degradation and hinders their practical application. The disadvantage is more obvious for all-solid-state battery systems, which require both high electronic and ionic migration at the same sites to realize a complete electrochemical reaction. In addition to adding conductive components into the cathode composites, another effective way to realize high-reversibility sulfur-based cathodes is by optimizing the inherent nature of sulfur-based materials to make them "conductive". Inorganic polysulfide materials including polysulfide molecules, selenium-sulfur solid solutions, and (lithium) metal polysulfides are promising, as they have different structures that can make them intrinsically conductive or becoming conductive during lithiation. They all contain at least one -S-S- bridged bond, which is the intrinsic structural characteristic and the source of the chemical properties of these polysulfide compounds. For example, by balancing the conductivity and reversible capacity, researchers in the US National Aeronautics and Space Administration (NASA) have shown that 500 Wh/kg solid-state Li-Se/S batteries can power cars and even electric aircraft.We have long been focusing on the inorganic polysulfide component, reported the selenium-sulfur solid solutions, the first sulfur-rich phosphorus polysulfide molecules, and followed the research of metal polysulfide components. The proposed Account summarizes our current knowledge of the fundamental aspects of inorganic polysulfides in energy storage systems based on state-of-the-art publications on this topic. Both fast electron and ion migrations within the electrode materials are vital to achieving high-energy batteries. We begin by illustrating effective approaches to enhance the electronic/ionic conductivity of sulfur-based electrode materials. We then present some basic observations and properties (especially the intrinsic high conductivities) of the inorganic polysulfide electrode materials. The key chemical and structural factors dictating their conductive and electrochemical behaviors will be discussed. Finally, we show the advantages and broad applications of inorganic polysulfides in energy storage areas. The proposed Account will provide an insightful perspective on the current knowledge of inorganic polysulfide materials, as well as their future research directions and development potential, serving as a keynote reference for researchers in the field of energy storage.

A Universal Self-Propagating Synthesis of Aluminum-Based Oxyhalide Solid-State Electrolytes.

Inorganic solid-state electrolytes (SSEs) play a vital role in high-energy all-solid-state batteries (ASSBs). However, the current method of SSE preparation usually involves high-energy mechanical ball milling and/or a high-temperature annealing process, which is not suitable for practical application. Here, a facile strategy is developed to realize the scalable synthesis of cost-effective aluminum-based oxyhalide SSEs, which involves a self-propagating method by the exothermic reaction of the raw materials. This strategy enables the synthesis of various aluminum-based oxyhalide SSEs with tunable components and high ionic conductivities (over 10-3 S cm-1 at 25 °C) for different cations (Li+, Na+, Ag+). It is elucidated that the amorphous matrix, which mainly consists of various oxidized chloroaluminate species that provide numerous sites for smooth ion migration, is actually the key factor for the achieved high conductivities. Benefit from their easy synthesis, low cost, and low weight, the aluminum-based oxyhalide SSEs synthesized by our approach could further promote practical application of high-energy-density ASSBs.

Cubic Iodide Lix YI3+x Superionic Conductors through Defect Manipulation for All-Solid-State Li Batteries.

Halide solid electrolytes (SEs) have attracted significant attention due to their competitive ionic conductivity and good electrochemical stability. Among typical halide SEs (chlorides, bromides, and iodides), substantial efforts have been dedicated to chlorides or bromides, with iodide SEs receiving less attention. Nevertheless, compared with chlorides or bromides, iodides have both a softer Li sublattice and lower reduction limit, which enable iodides to possess potentially high ionic conductivity and intrinsic anti-reduction stability, respectively. Herein, we report a new series of iodide SEs: Lix YI3+x (x=2, 3, 4, or 9). Through synchrotron X-ray/neutron diffraction characterizations and theoretical calculations, we revealed that the Lix YI3+x SEs belong to the high-symmetry cubic structure, and can accommodate abundant vacancies. By manipulating the defects in the iodide structure, balanced Li-ion concentration and generated vacancies enables an optimized ionic conductivity of 1.04 × 10-3  S cm-1 at 25 °C for Li4 YI7 . Additionally, the promising Li-metal compatibility of Li4 YI7 is demonstrated via electrochemical characterizations (particularly all-solid-state Li-S batteries) combined with interface molecular dynamics simulations. Our study on iodide SEs provides deep insights into the relation between high-symmetry halide structures and ionic conduction, which can inspire future efforts to revitalize halide SEs.

Hopping Rate and Migration Entropy as the Origin of Superionic Conduction within Solid-State Electrolytes.

Inorganic solid-state electrolytes (SSEs) have gained significant attention for their potential use in high-energy solid-state batteries. However, there is a lack of understanding of the underlying mechanisms of fast ion conduction in SSEs. Here, we clarify the critical parameters that influence ion conductivity in SSEs through a combined analysis approach that examines several representative SSEs (Li3YCl6, Li3HoCl6, and Li6PS5Cl), which are further verified in the xLiCl-InCl3 system. The scaling analysis on conductivity spectra allowed the decoupled influences of mobile carrier concentration and hopping rate on ionic conductivity. Although the carrier concentration varied with temperature, the change alone cannot lead to the several orders of magnitude difference in conductivity. Instead, the hopping rate and the ionic conductivity present the same trend with the temperature change. Migration entropy, which arises from lattice vibrations of the jumping atoms from the initial sites to the saddle sites, is also proven to play a significant role in fast Li+ migration. The findings suggest that the multiple dependent variables such as the Li+ hopping frequency and migration energy are also responsible for the ionic conduction behavior within SSEs.

Superionic Conducting Halide Frameworks Enabled by Interface-Bonded Halides.

The revival of ternary halides Li-M-X (M = Y, In, Zr, etc.; X = F, Cl, Br) as solid-state electrolytes (SSEs) shows promise in realizing practical solid-state batteries due to their direct compatibility toward high-voltage cathodes and favorable room-temperature ionic conductivities. Most of the reported superionic halide SSEs have a structural pattern of [MCl6]x- octahedra and generate a tetrahedron-assisted Li+ ion diffusion pathway. Here, we report a new class of zeolite-like halide frameworks, SmCl3, for example, in which 1-dimensional channels are enclosed by [SmCl9]6- tricapped trigonal prisms to provide a short jumping distance of 2.08 Å between two octahedra for Li+ ion hopping. The fast Li+ diffusion along the channels is verified through ab initio molecular dynamics simulations. Similar to zeolites, the SmCl3 framework can be grafted with halide species to obtain mobile ions without altering the base structure, achieving an ionic conductivity over 10-4 S cm-1 at 30 °C with LiCl as the adsorbent. Moreover, the universality of the interface-bonding behavior and ionic diffusion in a class of framework materials is demonstrated. It is suggested that the ionic conductivity of the MCl3/halide composite (M = La-Gd) is likely in correlation with the ionic conductivity of the grafted halide species, interfacial bonding, and framework composition/dimensions. This work reveals a potential class of halide structures for superionic conductors and opens up a new frontier for constructing zeolite-like frameworks in halide-based materials, which will promote the innovation of superionic conductor design and contribute to a broader selection of halide SSEs.

Three-Dimensional Digital Reconstruction of the Cerebellar Cortex: Lobule Thickness, Surface Area Measurements, and Layer Architecture.

The cerebellum is ontogenetically one of the first structures to develop in the central nervous system; nevertheless, it has been only recently reconsidered for its significant neurobiological, functional, and clinical relevance in humans. Thus, it has been a relatively under-studied compared to the cerebrum. Currently, non-invasive imaging modalities can barely reach the necessary resolution to unfold its entire, convoluted surface, while only histological analyses can reveal local information at the micrometer scale. Herein, we used the BigBrain dataset to generate area and point-wise thickness measurements for all layers of the cerebellar cortex and for each lobule in particular. We found that the overall surface area of the cerebellar granular layer (including Purkinje cells) was 1,732 cm2 and the molecular layer was 1,945 cm2. The average thickness of the granular layer is 0.88 mm (± 0.83) and that of the molecular layer is 0.32 mm (± 0.08). The cerebellum (both granular and molecular layers) is thicker at the depth of the sulci and thinner at the crowns of the gyri. Globally, the granular layer is thicker in the lateral-posterior-inferior region than the medial-superior regions. The characterization of individual layers in the cerebellum achieved herein represents a stepping-stone for investigations interrelating structural and functional connectivity with cerebellar architectonics using neuroimaging, which is a matter of considerable relevance in basic and clinical neuroscience. Furthermore, these data provide templates for the construction of cerebellar topographic maps and the precise localization of structural and functional alterations in diseases affecting the cerebellum.

A generalizable and interpretable model for mortality risk stratification of sepsis patients in intensive care unit.

PURPOSE: This study aimed to construct a mortality model for the risk stratification of intensive care unit (ICU) patients with sepsis by applying a machine learning algorithm. METHODS: Adult patients who were diagnosed with sepsis during admission to ICU were extracted from MIMIC-III, MIMIC-IV, eICU, and Zigong databases. MIMIC-III was used for model development and internal validation. The other three databases were used for external validation. Our proposed model was developed based on the Extreme Gradient Boosting (XGBoost) algorithm. The generalizability, discrimination, and validation of our model were evaluated. The Shapley Additive Explanation values were used to interpret our model and analyze the contribution of individual features. RESULTS: A total of 16,741, 15,532, 22,617, and 1,198 sepsis patients were extracted from the MIMIC-III, MIMIC-IV, eICU, and Zigong databases, respectively. The proposed model had an area under the receiver operating characteristic curve (AUROC) of 0.84 in the internal validation, which outperformed all the traditional scoring systems. In the external validations, the AUROC was 0.87 in the MIMIC-IV database, better than all the traditional scoring systems; the AUROC was 0.83 in the eICU database, higher than the Simplified Acute Physiology Score III and Sequential Organ Failure Assessment (SOFA),equal to 0.83 of the Acute Physiology and Chronic Health Evaluation IV (APACHE-IV), and the AUROC was 0.68 in the Zigong database, higher than those from the systemic inflammatory response syndrome and SOFA. Furthermore, the proposed model showed the best discriminatory and calibrated capabilities and had the best net benefit in each validation. CONCLUSIONS: The proposed algorithm based on XGBoost and SHAP-value feature selection had high performance in predicting the mortality of sepsis patients within 24 h of ICU admission.

A Comprehensive Landscape of Imaging Feature-Associated RNA Expression Profiles in Human Breast Tissue.

The expression abundance of transcripts in nondiseased breast tissue varies among individuals. The association study of genotypes and imaging phenotypes may help us to understand this individual variation. Since existing reports mainly focus on tumors or lesion areas, the heterogeneity of pathological image features and their correlations with RNA expression profiles for nondiseased tissue are not clear. The aim of this study is to discover the association between the nucleus features and the transcriptome-wide RNAs. We analyzed both microscopic histology images and RNA-sequencing data of 456 breast tissues from the Genotype-Tissue Expression (GTEx) project and constructed an automatic computational framework. We classified all samples into four clusters based on their nucleus morphological features and discovered feature-specific gene sets. The biological pathway analysis was performed on each gene set. The proposed framework evaluates the morphological characteristics of the cell nucleus quantitatively and identifies the associated genes. We found image features that capture population variation in breast tissue associated with RNA expressions, suggesting that the variation in expression pattern affects population variation in the morphological traits of breast tissue. This study provides a comprehensive transcriptome-wide view of imaging-feature-specific RNA expression for healthy breast tissue. Such a framework could also be used for understanding the connection between RNA expression and morphology in other tissues and organs. Pathway analysis indicated that the gene sets we identified were involved in specific biological processes, such as immune processes.

Halide Layer Cathodes for Compatible and Fast-Charged Halides-Based All-Solid-State Li Metal Batteries.

Insertion-type compounds based on oxides and sulfides have been widely identified and well-studied as cathode materials in lithium-ion batteries. However, halides have rarely been used due to their high solubility in organic liquid electrolytes. Here, we reveal the insertion electrochemistry of VX3 (X=Cl, Br, I) by introducing a compatible halide solid-state electrolyte with a wide electrochemical stability window. X-ray absorption near-edge structure analyses reveal a two-step lithiation process and the structural transition of typical VCl3 . Fast Li+ insertion/extraction in the layered VX3 active materials and favorable interface guaranteed by the compatible electrode-electrolyte design enables high rate capability and stable operation of all-solid-state Li-VX3 batteries. The findings from this study will contribute to developing intercalation insertion electrochemistry of halide materials and exploring novel electrode materials in viable energy storage systems.

The Universal Super Cation-Conductivity in Multiple-cation Mixed Chloride Solid-State Electrolytes.

As exciting candidates for next-generation energy storage, all-solid-state lithium batteries (ASSLBs) are highly dependent on advanced solid-state electrolytes (SSEs). Here, using cost-effective LaCl3 and CeCl3 lattice (UCl3 -type structure) as the host and further combined with a multiple-cation mixed strategy, we report a series of UCl3 -type SSEs with high room-temperature ionic conductivities over 10-3  S cm-1 and good compatibility with high-voltage oxide cathodes. The intrinsic large-size hexagonal one-dimensional channels and highly disordered amorphous phase induced by multi-metal cation species are believed to trigger fast multiple ionic conductions of Li+ , Na+ , K+ , Cu+ , and Ag+ . The UCl3 -type SSEs enable a stable prototype ASSLB capable of over 3000 cycles and high reversibility at -30 °C. Further exploration of the brand-new multiple-cation mixed chlorides is likely to lead to the development of advanced halide SSEs suitable for ASSLBs with high energy density.

Metal Halide Superionic Conductors for All-Solid-State Batteries.

ConspectusRechargeable all-solid-state Li batteries (ASSLBs) are considered to be the next generation of electrochemical energy storage systems. The development of solid-state electrolytes (SSEs), which are key materials for ASSLBs, is therefore one of the most important subjects in modern energy storage chemistry. Various types of electrolytes such as polymer-, oxide-, and sulfide-based SSEs have been developed to date and the discovery of new superionic conductors is still ongoing. Metal-halide SSEs (Li-M-X, where M is a metal element and X is a halogen) are emerging as new candidates with a number of attractive properties and advantages such as wide electrochemical stability windows (0.36-6.71 V vs Li/Li+) and better chemical stability toward cathode materials compared to other SSEs. Furthermore, some of the metal-halide SSEs (such as the Li3InCl6 developed by our group) can be directly synthesized at large scales in a water solvent, removing the need for special apparatus or handling in an inert atmosphere. Based on the recent advances, herein we focus on the topic of metal-halide SSEs, aiming to provide a guidance toward further development of novel halide SSEs and push them forward to meet the multiple requirements of energy storage devices.In this Account, we describe our recent progress in developing metal halide SSEs and focus on some newly reported findings based on state-of-the-art publications on this topic. A discussion on the structure of metal-halide SSEs will be first explored. Subsequently, we will illustrate the effective approaches to enhance the ionic conductivities of metal halide SSEs including the effect of anion sublattice framework, the regulation of site occupation and disorder, and defect engineering. Specifically, we demonstrated that proper structural framework, balanced Li+/vacancy concentration, and reduced blocking effect can promote fast Li+ migration for metal halide SSEs. Moreover, humidity stability and degradation chemistry of metal halide SSEs have been summarized for the first time. Some examples of the application of metal halide SSEs with stability toward humidity have been demonstrated. Direct synthesis of halide SSEs on cathode materials by the water-mediated route has been used to eliminate the interfacial challenges of ASSLBs and has been shown to act as an interfacial modifier for high-performance all-solid-state Li-O2 batteries. Taken together, this Account on metal halide SSEs will provide an insightful perspective over the recent development and future research directions that can lead to advanced electrolytes.

Origin of Superionic Li3Y1-xInxCl6 Halide Solid Electrolytes with High Humidity Tolerance.

The high ionic conductivity, air/humidity tolerance, and related chemistry of Li3MX6 solid-state electrolytes (SSEs, M is a metal element, and X is a halogen) has recently gained significant interest. However, most of the halide SSEs suffer from irreversible chemical degradation when exposed to a humid atmosphere, which originates from hydrolysis. Herein, the function of the M atom in Li3MX6 was clarified by a series of Li3Y1-xInxCl6 (0 ≤ x < 1). When the ratio of In3+ was increased, a gradual structural conversion from the hexagonal-closed-packed (hcp) anion arrangement to cubic-closed-packed (ccp) anion arrangement has been traced. Compared to hcp anion sublattice, the Li3MX6 with ccp anion sublattice reveals faster Li+ migration. The tolerance of Li3Y1-xInxCl6 towards humidity is highly improved when the In3+ content is high enough due to the formation of hydrated intermediates. The correlations among composition, structure, Li+ migration, and humidity stability presented in this work provide insights for designing new halide-based SSEs.

Site-Occupation-Tuned Superionic LixScCl3+xHalide Solid Electrolytes for All-Solid-State Batteries.

The enabling of high energy density of all-solid-state lithium batteries (ASSLBs) requires the development of highly Li+-conductive solid-state electrolytes (SSEs) with good chemical and electrochemical stability. Recently, halide SSEs based on different material design principles have opened new opportunities for ASSLBs. Here, we discovered a series of LixScCl3+x SSEs (x = 2.5, 3, 3.5, and 4) based on the cubic close-packed anion sublattice with room-temperature ionic conductivities up to 3 × 10-3 S cm-1. Owing to the low eutectic temperature between LiCl and ScCl3, LixScCl3+x SSEs can be synthesized by a simple co-melting strategy. Preferred orientation is observed for all the samples. The influence of the value of x in LixScCl3+x on the structure and Li+ diffusivity were systematically explored. With increasing x value, higher Li+, lower vacancy concentration, and less blocking effects from Sc ions are achieved, enabling the ability to tune the Li+ migration. The electrochemical performance shows that Li3ScCl6 possesses a wide electrochemical window of 0.9-4.3 V vs Li+/Li, stable electrochemical plating/stripping of Li for over 2500 h, as well as good compatibility with LiCoO2. LiCoO2/Li3ScCl6/In ASSLB exhibits a reversible capacity of 104.5 mAh g-1 with good cycle life retention for 160 cycles. The observed changes in the ionic conductivity and tuning of the site occupations provide an additional approach toward the design of better SSEs.

Correction to: Systemic microvascular rarefaction is correlated with dysfunction of late endothelial progenitor cells in mild hypertension: a substudy of EXCAVATION-CHN1.

Upon publication of the original article [1], it was noticed that Jun Tao's affiliation information is not complete. The full affiliation information for Jun Tao can be found below and in the complete affiliation list of this Correction article.

Size-Mediated Recurring Spinel Sub-nanodomains in Li- and Mn-Rich Layered Cathode Materials.

Li- and Mn-rich layered oxides are among the most promising cathode materials for Li-ion batteries with high theoretical energy density. Its practical application is, however, hampered by the capacity and voltage fade after long cycling. Herein, a finite difference method for near-edge structure (FDMNES) code was combined with in situ X-ray absorption spectroscopy (XAS) and transmission electron microscopy/electron energy loss spectroscopy (TEM/EELS) to investigate the evolution of transition metals (TMs) in fresh and heavily cycled electrodes. Theoretical modeling reveals a recurring partially reversible LiMn2 O4 -like sub-nanodomain formation/dissolution process during each charge/discharge, which accumulates gradually and accounts for the Mn phase transition. From the modeling of spectra and maps of the valence state over large regions of the cathodes, it was found that the phase change is size-dependent. After prolonged cycling, the TMs displayed different levels of inactivity.

Systemic microvascular rarefaction is correlated with dysfunction of late endothelial progenitor cells in mild hypertension: a substudy of EXCAVATION-CHN1.

BACKGROUND: Hypertension often presents with microvascular rarefaction (MVR), which is closely associated with impaired angiogenesis. Early detection of MVR is essential for systemic assessment in patient with hypertension. We aimed to determine the systemic MVR through both optical coherence tomography angiography (OCTA) and intravital capillaroscopy, and to investigate their respective efficacies and related mechanisms associated with late endothelial progenitor cells (LEPCs) dysfunction. METHODS: Seventy-one hypertensive and sixty-nine age-match normotensive subjects were included in this study. All subjects received intravital capillaroscopy for skin capillary density (SCD) and OCTA for retinal capillary density (RCD) and non-perfused areas (R-NPA). Subsequently, correlation of LEPCs activities and microvascular rarefaction were examined. RESULTS: Compared with normotensive subjects, hypertensive patients had significantly lower RCD [(52.9 ± 2.9)% vs. (57.8 ± 1.6)%, P < 0.01] and higher R-NPA [(0.12 ± 0.07) mm2 vs. (0.053 ± 0.020) mm2, P < 0.01]. SCD correlated positively with RCD but negatively with R-NPA [(RCD: OR = 0.40, 95% CI 0.25-0.67, P < 0.01); (R-NPA: OR = 0.39, 95% CI - 0.0029 to 0.0011, P < 0.01)]. The discriminative powers of RCD performed best (AUC 0.79 versus SCD AUC 0.59, P < 0.001) followed by R-NPA (AUC 0.73 versus SCD AUC 0.59, P < 0.001) for systolic blood pressure. Similar pattern is also found for diastolic blood pressure (RCD AUC 0.80 versus SCD AUC 0.54, P < 0.001; R-NPA AUC 0.77 versus SCD AUC 0.54, P < 0.001). Furthermore, LEPCs tube formation was impaired in hypertensive patients (36.8 ± 2.3 vs. 28 ± 3.7, P < 0.01). After multivariate adjustments, positive correlation existed between RCD or R-NPA with LEPCs tube formation (RCD: ß = 0.64, 95% CI 0.34-0.91, P < 0.01; R-NPA: ß = - 24.67, 95% CI - 43.14 to - 4.63, P < 0.05) but not with SCD (ß = 0.082, 95% CI 0.01-0.18, P = 0.085). CONCLUSION: Compared to intravital capillaroscopy, OCTA is a more precise technique for early detection of hypertensive microvascular rarefaction, which is associated with the fall in LEPC-mediated angiogenesis. Both of OCTA and LEPCs function can help identify hypertension-related capillary abnormality. Trail Registration The trial is a substudy of EXCAVATION-CHN1, registered at clinicaltrials.gov as NCT02817204 (June 26, 2016).

Water-Mediated Synthesis of a Superionic Halide Solid Electrolyte.

To promote the development of solid-state batteries, polymer-, oxide-, and sulfide-based solid-state electrolytes (SSEs) have been extensively investigated. However, the disadvantages of these SSEs, such as high-temperature sintering of oxides, air instability of sulfides, and narrow electrochemical windows of polymers electrolytes, significantly hinder their practical application. Therefore, developing SSEs that have a high ionic conductivity (>10-3  S cm-1 ), good air stability, wide electrochemical window, excellent electrode interface stability, low-cost mass production is required. Herein we report a halide Li+ superionic conductor, Li3 InCl6 , that can be synthesized in water. Most importantly, the as-synthesized Li3 InCl6 shows a high ionic conductivity of 2.04×10-3  S cm-1 at 25 °C. Furthermore, the ionic conductivity can be recovered after dissolution in water. Combined with a LiNi0.8 Co0.1 Mn0.1 O2 cathode, the solid-state Li battery shows good cycling stability.

Optimization of Microporous Carbon Structures for Lithium-Sulfur Battery Applications in Carbonate-Based Electrolyte.

Developing appropriate sulfur cathode materials in carbonate-based electrolyte is an important research subject for lithium-sulfur batteries. Although several microporous carbon materials as host for sulfur reveal the effect, methods for producing microporous carbon are neither easy nor well controllable. Moreover, due to the complexity and limitation of microporous carbon in their fabrication process, there has been rare investigation of influence on electrochemical behavior in the carbonate-based electrolyte for lithium-sulfur batteries by tuning different micropore size(0-2 nm) of carbon host. Here, we demonstrate an immediate carbonization process, self-activation strategy, which can produce microporous carbon for a sulfur host from alkali-complexes. Besides, by changing different alkali-ion in the previous complex, the obtained microporous carbon exhibits a major portion of ultramicropore (<0.7 nm, from 54.9% to 25.8%) and it is demonstrated that the micropore structure of the host material plays a vital role in confining sulfur molecule. When evaluated as cathode materials in a carbonate-based electrolyte for Li-S batteries, such microporous carbon/sulfur composite can provide high reversible capacity, cycling stability and good rate capability.

Sulfur-Rich Phosphorus Sulfide Molecules for Use in Rechargeable Lithium Batteries.

A new family of sulfur-rich phosphorus sulfide molecules (P4 S10+n ) and their electrochemical reaction mechanism with metallic Li has been explored. These P4 S10+n molecules are synthesized by the reaction between P4 S10 and S. For Li batteries, the P4 S40 molecule in the series of P4 S10+n molecules provides the highest capacity, which has a first discharge capacity of 1223 mAh g-1 at 100 mA g-1 and stabilizes at approximately 720 mAh g-1 at 500 mA g-1 after 100 cycles. This new class of sulfur-rich P4 S10+n molecules and its electrochemical behavior for room-temperature Li+ storage could provide novel insights for phosphorus sulfide molecules and high-energy batteries.