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Sulfur-based aqueous batteries (SABs) are promising for safe, low-cost, and high-capacity energy storage. However, the low output voltage of sulfur cannot meet the demands of high-energy cathode applications due to its intrinsic negative potential (E0 = -0.51 V vs SHE) of low-valent polysulfide redox (S2-/S0). Here, instead of relying on traditional aqueous polysulfide redox, for the first time, we demonstrate a high-valent thiosulfate redox (S2O32-/S4O62-) electrochemistry, exhibiting positive redox potential (E0 > 0 V vs SHE) and reversible cation storage in aqueous environment. Operando X-ray absorption fine structure spectroscopy, in situ Raman spectroscopy, and density functional theory calculations reveal the high reversibility and dynamic charge transfer process of high-valent thiosulfate redox. Significantly, the aqueous thiosulfate redox exhibits a high operating voltage of approximately 1.4 V, a reversible capacity of 193 Ah L-1, and a long cycling life of over 1000 cycles (99.6% capacity retention). This work provides new insights into the high-valent S-based electrochemistry and opens a new pathway to achieve energetic aqueous batteries.
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Voltage oscillation at subzero in sodium-ion batteries (SIBs) has been a common but overlooked scenario, almost yet to be understood. For example, the phenomenon seriously deteriorates the performance of Na3V2(PO4)3 (NVP) cathode in PC (propylene carbonate)/EC (ethylene carbonate)-based electrolyte at -20 °C. Here, the correlation between voltage oscillation, structural evolution, and electrolytes has been revealed based on theoretical calculations, in-/ex-situ techniques, and cross-experiments. It is found that the local phase transition of the Na3V2(PO4)3 (NVP) cathode in PC/EC-based electrolyte at -20 °C should be responsible for the oscillatory phenomenon. Furthermore, the low exchange current density originating from the high desolvation energy barrier in NVP-PC/EC system also aggravates the local phase transformation, resulting in severe voltage oscillation. By introducing the diglyme solvent with lower Na-solvent binding energy, the voltage oscillation of the NVP can be eliminated effectively at subzero. As a result, the high capacity retentions of 98.3% at -20 °C and 75.3% at -40 °C are achieved. The finding provides insight into the abnormal SIBs degradation and brings the voltage oscillation behavior of rechargeable batteries into the limelight.
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The intercalation structure of two-dimensional materials with expanded interlayer distance can facilitate mass transport, which is promising in fast-charging lithium-ion batteries (LIBs). However, the designed intercalation structures will be pulverized and destroyed under tough working conditions, causing overall performance deterioration of the batteries. Here, we present that an intercalated heterostructure made of the typical layered material of MoS2 intercalated by N-doped graphene-like carbon monolayer (MoS2/g-CM) through a polymer intercalation strategy exhibits a unique behavior of reversible reconstructability as an LIB anode during cycling. A mechanism of "carbon monolayers-confined topotactic transformation" is proposed, which is evidenced by substantial in/ex situ characterizations. The intercalated heterostructure of MoS2/g-CM featuring a reconstructable property and efficient interlayer electron/ion transport exhibits an unprecedented rate capability up to 50 A g-1 and outstanding long cyclability. Moreover, the proposed strategy based on g-CM intercalation has been extended to the MoSe2 system, also realizing reconstructability of the intercalated heterostructure and improved LIB performance, demonstrating its versatility and great potential in applications.
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Temperature-phased anaerobic digestion (TPAD) and microbial electrolysis cell (MEC) are both able to improve hydrolysis and methane yield during anaerobic digestion (AD) of dewatered sludge. However, the effect of TPAD and MEC integration at different temperatures and different phases is unclear. This study investigated the effect of the integration of intermittent energization MEC in different phases of TPAD on the digestion of dewatered sludge. Thermophilic and MEC hydrolysis could release higher total ammonia nitrogen of 186.0% and 10.3% than control, mesophilic methanogenesis phase integrated with MEC relieved the ammonia inhibition and accelerated the acid utilization leading to the relief of acid accumulation. The ultimate methane yield of the TPAD integrated with MEC was increased by 118.9%, in which the relative abundance of Methanothermobacteria and Methanosarcina was increased. Therefore, intermittent energization MEC integrated TPAD synchronously improved the hydrolysis and methane yield.
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Eletrólise , Metano , Esgotos , Temperatura , Metano/metabolismo , Hidrólise , Esgotos/microbiologia , Anaerobiose , Amônia/metabolismo , Água/química , Reatores BiológicosRESUMO
The gradual increase in cattle farming has led to a huge production of cattle manure (CM), but the conventional treatment methods are less efficient. In this study, the treatment method of anaerobic digestion (AD) of high-solids CM by combining nanobubble water (NBW) with different gases was proposed to present a new idea for the reduction, harmlessness, and resourcefulness of CM. It was found that the performance of the digester with added NBW was better than the control. Among them, the cumulative methane yield T-Air: 227.09 mL g-1 VSadded and T-CO2: 226.12 mL g-1 VSadded increased by 17.72 % and 17.22 %, respectively, compared with the control T: 192.90 mL g-1 VSadded under thermophilic conditions. Under mesophilic conditions, M-Air: 162.39 mL g-1 VSadded increased by 9.68 % compared with control M: 148.05 mL g-1 VSadded. Microbial communities analyzed at the genus level revealed that the relative abundance of bacteria favorable to hydrolysis and acid-producing processes, such as Defluviitalea, Haloplasma, and Bacillus, increased to varying degrees. Moreover, the relative abundance of archaea favorable for methanogenesis, such as Methanoculleus, Methanobrevibacter, and Methanosarcina, also increased to varying degrees. Therefore, the addition of NBW promoted the hydrolysis of high-solids CM, enhanced the stability of the reaction, improved the methanogenic performance, and increased the RA of favorable genera, which ultimately led to a better performance of the AD of high-solids CM.
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Esterco , Metano , Esterco/microbiologia , Animais , Bovinos , Anaerobiose , Metano/metabolismo , Metano/análise , Água/química , Reatores Biológicos , Bactérias/metabolismoRESUMO
The impact of mechanical pretreatment of corn straw (CS), pea straw (PS), and wheat straw (WS), on shape characterization and NO emissions during combustion were investigated in this research. Particle size ranges were obtained and characterized their shape factors using Image J correction. The thermal properties and NO emissions of the different-sized particles were investigated by TG-MS and fixed-bed reactor. Compared with CS and PS, WS is more likely to break into smaller particles due to its moderate strength. Amine-N completely disappeared after pyrolysis, whereas pyrrolic-N and pyridinic-N were the main N functionalities in char-N. During the volatile burning stage, the maximum peak of NO concentration was 270, 354 and 311 ppm for CS, PS and WS, respectively. NO was detected at a steady level during the semicoke combustion stage, and the duration increased with particle size. The NO concentration decreased sharply in a short duration during the fixed carbon combustion stage.
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Poluentes Atmosféricos , Pirólise , Biomassa , Tamanho da Partícula , Agricultura , Carbono/análise , Poluentes Atmosféricos/análiseRESUMO
Developing new cathode materials to avoid shuttle effect of Li-S batteries at source is crucial for practical high-energy applications, which, however, remains a great challenge. Herein, a new class of sulfur-containing ternary covalent inorganic framework (CIF), P4 Se6 S40 , is explored, by simply comelting powders of P, S, and Se. The P4 Se6 S40 CIF with open framework enables all active sites available during electrochemical reactions, giving a high capacity delivery. Moreover, introducing Se atoms can improve intrinsic electronic conductivity of S chains yet without remarkably compromising the capacity because Se is also electrochemical active to lithium storage. More importantly, Se atoms in S-Se chains can serve as a heteroatom barrier to block the bonding of S atoms around, effectively avoiding the formation of long-chain polysulfides during cycling. Besides, stable Li3 PS4 with a tetrahedral configuration formed after lithiation works as not only a good ionic conductor to promote Li ion diffusion, but a three-dimensional spatial barrier and chemical anchor to suppress the dissolution and diffusion of lithium polysulfides (LiPS), further inhibiting the shuttle effect. Consequently, the P4 Se6 S40 cathode delivers high capacity and excellent capacity retention with even a high loading of 10.5 mg cm-2 which far surpasses the requirement for commercial applications.
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Background: Ankle function impairment is a critical factor impairing normal walking in survivors of stroke. The soft robotic exoskeleton (SRE) is a novel, portable, lightweight assistive device with promising therapeutic potential for gait recovery during post-stroke rehabilitation. However, whether long-term SRE-assisted walking training influences walking function and gait quality in patients following subacute stroke is unknown. Therefore, the primary objective of this study was to assess the therapeutic effects of SRE-assisted walking training on clinical and biomechanical gait outcomes in the rehabilitation of patients with subacute stroke. Methods: A group patients who had experienced subacute stroke received conventional rehabilitation (CR) training combined with 10-session SRE-assisted overground walking training (30 min per session, 5 sessions/week, 2 weeks) (SRE group, n = 15) compared with the control group that received CR training only (CR group, n = 15). Clinical assessments and biomechanical gait quality measures were performed pre-and post-10-session intervention, with the 10-Minute Walk Test (10MWT) and 6-Minute Walk Test (6MWT) used to define the primary clinical outcome measures and the Functional Ambulation Category, Fugl-Meyer Assessment for Lower Extremity (FMA-LE) subscale, and Berg Balance Scale defined the secondary outcome measures. The gait quality outcome measures included spatiotemporal and symmetrical parameters during walking. Results: After the 10-session intervention, the SRE and CR groups exhibited significant within-group improvements in all clinical outcome measures (p < 0.05). Between-comparison using covariance analyses demonstrated that the SRE group showed greater improvement in walking speed during the 10MWT (p < 0.01), distance walked during the 6MWT (p < 0.05), and FMA-LE scores (p < 0.05). Gait analyses showed that the SRE group exhibited significantly improved spatiotemporal symmetry (p < 0.001) after 10-session training, with no significant changes observed in the CR group. Conclusion: Compared with CR training, SRE-assisted walking training led to greater improvements in walking speed, endurance, and motor recovery. Our findings provide preliminary evidence that SRE may be considered for inclusion in intensive gait training clinical rehabilitation programs to further improve walking function in patients who have experienced stroke.
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Partial point cloud registration aims to transform partial scans into a common coordinate system. It is an important preprocessing step to generate complete 3D shapes. Although previous registration methods have made great progress in recent decades, traditional registration methods, such as Iterative Closest Point (ICP) and its variants, all these methods highly depend on the sufficient overlaps between two point clouds, because they cannot distinguish outlier correspondences. Note that the overlap between point clouds could always be small, which limits the application of these methods. To tackle this problem, we present a StrucTure-based OveRlap Matching (STORM) method for partial point cloud registration. In our method, an overlap prediction module with differentiable sampling is designed to detect points in overlap utilizing structure information, and facilitates exact partial correspondence generation, which is based on discriminative pointwise feature similarity. The pointwise features which contain effective structural information are extracted by graph-based methods. Experimental results and comparison with state-of-the-art methods demonstrate that STORM can achieve better performance. Moreover, most registration methods perform worse when the overlap ratio decreases, while STORM can still achieve satisfactory performance when the overlap ratio is small.
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We report here the first implementation of chemically specific imaging in the exhaust plume of a gas turbine typical of those used for propulsion in commercial aircraft. The method used is chemical species tomography (CST) and the target species is CO2, absorbing in the near-infrared at 1999.4 nm. A total of 126 beams propagate transverse to the plume axis, along 7 m paths in a coplanar geometry, to probe a central region of diameter ≈1.5m. The CO2 absorption spectrum is measured using tunable diode laser spectroscopy with wavelength modulation, using the second harmonic to first harmonic (2f/1f) ratio method. The engine is operated over the full range of thrust, while data are recorded in a quasi-simultaneous mode at frame rates of 1.25 and 0.3125 Hz. Various data inversion methodologies are considered and presented for image reconstruction. At all thrust levels a persistent ring structure of high CO2 concentration is observed in the central region of the measurement plane, with a raised region in the middle of the plume assumed to be due to the engine's boat tail. With its potential to target various exhaust species, the CST method outlined here offers a new approach to turbine combustion research, turbine engine development, and aviation fuel research and development.
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Study Design: A randomized controlled pilot study. Background: Bimanual therapy (BMT) is an effective neurorehabilitation therapy for the upper limb, but its application to the distal upper limb is limited due to methodological difficulties. Therefore, we applied an exoskeleton hand to perform robot-assisted task-oriented bimanual training (RBMT) in patients with stroke. Objective: To characterize the effectiveness of RBMT in patients with hemiplegic stroke with upper limb motor impairment. Interventions: A total of 19 patients with subacute stroke (1-6 months from onset) were randomized and allocated to RBMT and conventional therapy (CT) groups. The RBMT and CT groups received 90 min of training/day (RBMT: 60 min RBMT + 30 min CT; CT: 60 min CT for hand functional training + 30 min regular CT), 5 days/week, for 4 weeks (20 sessions during the experimental period). Assessments: Clinical assessments, including the Fugl-Meyer assessment of the upper extremity (FMA-UE), action research arm test (ARAT), and wolf motor arm function test (WMFT), were conducted before and after the intervention. Results: Within-group analysis showed a significant improvement in the FMA-UE and WMFT in both the CT and RBMT groups. A significant improvement in the Fugl-Meyer assessment (FMA) of the wrist and hand for the distal part in the RBMT group occurred earlier than that in the CT group. A significant improvement in WMFT time was found in both groups, but the WMFT functional ability assessment was only found in the RBMT group. No significant improvements in ARAT assessment were observed in either the CT or RBMT groups. Compared with CT, significant improvements were found in terms of the proportion of minimally clinically important differences after RBMT in FMA-UE (χ2 = 4.34, p = 0.037). No adverse events were reported by any of the participants across all sessions. Conclusions: This study is the first to apply RBMT to the distal part of the upper limb. Both RBMT and CT are effective in improving the upper limb function in patients with subacute stroke. RBMT shows superior potential efficacy in facilitating recovery of the distal part of upper extremity (UE) motor function in the early stage. Future randomized control studies with a large sample size and follow-up assessments are needed to validate the present conclusions.
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Developing zero-strain electrode materials with high capacity is crucial for lithium-ion batteries (LIBs). Here, a new zero-strain composite material made of ultrasmall Si nanodots (NDs) within metal organic framework-derived nanoreactors (Si NDsâMDN) through a novel space-confined catalytic strategy is reported. The unique Si NDsâMDN anode features a low strain (<3%) and a high theoretical lithium storage capacity (1524 mAh g-1 ) which far surpasses the traditional single-crystal counterparts that suffer from a low capacity delivery. The zero-strain property is evidenced by substantial characterizations including ex/in situ transmission electron microscopy and mechanical simulations. The Si NDsâMDN exhibits superior cycling stability and high reversible capacity (1327 mAh g-1 at 0.1 A g-1 after 100 cycles) in half-cells and high energy density (366 Wh kg-1 after 300 cycles) in a full cell. This study reports a new catalog of zero-strain electrode material with significantly improved capacity beyond the traditional single-crystal zero-strain materials.
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Alcoholism is a severe threat to public health, and there are no adequate treatments for alcoholic liver disease. The aim of this study was to identify bioactive peptides derived from natural proteins that prevent acute alcohol-induced liver injury. We identified a peptide with the sequence Gly-Leu-hydroxyproline-Gly-Glu-Arg (GLpGER) from the hydrolysate of crucian carp swim bladder using size-exclusion chromatography and reversed-phase chromatography. The in vitro EC50 value of GLpGER to activate alcohol dehydrogenase (ADH) was 137.9 ± 9 µM. Molecular docking experiments indicated that the mechanism by which GLpGER activates ADH may be related to the formation of stable complexes with ADH active pockets through hydrogen bonding, and electrostatic and hydrophobic interactions. Oral administration of GLpGER one hour before acute alcohol ingestion significantly increased alcohol metabolism, manifesting as reduced incidence of the loss of righting reflex, increased alcohol tolerance time, shortened sobering time, and decreased blood alcohol concentration level. GLpGER restored liver ADH activity, maintained the typical morphology of hepatocytes, and reduced serum levels of alanine aminotransferase and aspartate aminotransferase. These findings suggest that GLpGER might reduce acute alcohol-induced liver injury and may have the potential to be developed as an anti-inebriation ingredient.
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Carpas , Doença Hepática Crônica Induzida por Substâncias e Drogas , Álcool Desidrogenase , Animais , Concentração Alcoólica no Sangue , Etanol , Fígado , Camundongos , Simulação de Acoplamento Molecular , Peptídeos , Bexiga UrináriaRESUMO
We use a model to investigate both the temporal and spectral characteristics of a signal lightwave which has been spectrally broadened through phase modulation with a maximal-length sequence (MLS), which is a common type of pseudo-random bit sequence. The enhancement of the stimulated Brillouin scattering (SBS) threshold of the modulated lightwave in a fiber system is evaluated by numerically simulating the coupled three-wave SBS interaction equations. We find that SBS can build up on a nanosecond-level time scale in a short fiber, which can reduce the SBS suppressing capability of MLS modulation waveforms with GHz-level clock rate, if the sub-sequence ("run") lengths with the same symbol (zero or one) of the MLS extend over several nanoseconds. To ensure the SBS buildup is perturbed and thus suppressed also during these long sub-sequences, we introduce a low-pass filter to average the signal over several bits so that the modulation waveform changes gradually even during long runs and amplify the RF modulation waveforms to the level required for sufficient spectral broadening and carrier suppression of the optical signal. We find that the SBS suppression depends non-monotonically on the parameters of the filtered and amplified MLS waveform such as pattern length, modulation depth, and the ratio of low-pass filter cutoff frequency to clock rate for maximum SBS mitigation. We optimize the SBS suppression through numerical simulations and discuss it in terms of the temporal and spectral characteristics of the lightwave and modulation waveform using derived analytical expressions and numerical simulations. The simulations indicate that the normalized SBS threshold reaches a maximum for a RMS modulation depth of 0.56π and a ratio of filter cutoff frequency to clock rate of 0.54 and that MLS9 is superior to other investigated patterns.
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Potassium-ion capacitors (KICs) are promising for sustainable and eco-friendly energy storage technologies, yet their slow reaction kinetics and poor cyclability induced by large K-ion size are a major obstacle toward practical applications. Herein, by employing black phosphorus nanosheets (BPNSs) as a typical high-capacity anode material, we report that BPNS anodes armored with an ultrathin oriented-grown metal-organic-framework (MOF) interphase layer (BPNS@MOF) exhibit regulated potassium storage behavior for high-performance KICs. The MOF interphase layers as protective layer with ordered pores and high chemical/mechanical stability facilitate K ion diffusion and accommodate the volume change of electrode, beneficial for improved reaction kinetics and enhanced cyclability, as evidenced by substantial characterizations, kinetics analysis and DFT calculations. Consequently, the BPNS@MOF electrode as KIC anodes exhibits outstanding cycle performance outperforming most of the reported state-of-art KICs so far.
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The exploration of ideal electrode materials overcoming the critical problems of large electrode volume changes and sluggish redox kinetics induced by large ionic radius of Na+ /K+ ions is highly desirable for sodium/potassium-ion batteries (SIBs/PIBs) toward large-scale applications. The present work demonstrates that single-phase ternary cobalt phosphoselenide (CoPSe) in the form of nanoparticles embedded in a layered metal-organic framework (MOF)-derived N-doped carbon matrix (CoPSe/NC) represents an ultrastable and high-rate anode material for SIBs/PIBs. The CoPSe/NC is fabricated by using the MOF as both a template and precursor, coupled with in situ synchronous phosphorization/selenization reactions. The CoPSe anode holds a set of intrinsic merits such as lower mechanical stress, enhanced reaction kinetics, as well as higher theoretical capacity and lower discharge voltage relative to its counterpart of CoSe2 , and suppressed shuttle effect with higher intrinsic electrical conductivity relative to CoPS. The involved mechanisms are evidenced by substantial characterizations and density functional theory (DFT) calculations. Consequently, the CoPSe/NC anode shows an outstanding long-cycle stability and rate performance for SIBs and PIBs. Moreover, the CoPSe/NC-based Na-ion full cell can achieve a higher energy density of 274 Wh kg-1 , surpassing that based on CoSe2 /NC and most state-of-the-art Na-ion full cells based on P-, Se-, or S-containing binary/ternary anodes to date.
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We experimentally demonstrate Raman amplification of signal pulses in a high-order Bessel mode (LP06) at a wavelength of 1121 nm in a 335-m step-index fiber with a 70-µm diameter, 0.227-NA pure-silica core. This was pumped by 5-ns multimode pulses at 1065 nm from a Yb-doped fiber master oscillation power amplifier. The mode purity of the amplified pulses is well preserved to 23 dB of average-power gain, to 774 W of peak power in 2 ns pulses at a 20 kHz repetition rate, when pumped with a peak power of 942 W. The pump depletion as averaged over the signal pulses reaches 59%. We believe, to the best of our knowledge, that this is the first demonstration of stable mode propagation and Raman amplification of a single Bessel-like higher-order mode in a fiber of hundreds of meters. This shows the potential for efficient power scaling of a single signal mode with low-brightness pumping, comparable with that from continuous-wave multimode diode lasers.
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Structured light, with spatially varying phase or polarization distributions, has given rise to many novel applications in fields ranging from optical communication to laser-based material processing. However the efficient and flexible generation of such beams from a compact laser source at practical output powers still remains a great challenge. Here we describe an approach capable of addressing this need based on the coherent combination of multiple tailored Gaussian beams emitted from a multicore fibre (MCF) amplifier. We report a proof-of-concept structured light generation experiment, using a cladding-pumped 7-core MCF amplifier as an integrated parallel amplifier array and a spatial light modulator (SLM) to actively control the amplitude, polarization and phase of the signal light input to each fibre core. We report the successful generation of various structured light beams including high-order linearly polarized spatial fibre modes, cylindrical vector (CV) beams and helical phase front optical vortex (OV) beams.
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We demonstrate efficient pulse-energy extraction from a partly quenched erbium-doped aluminosilicate fiber amplifier. This has a high erbium concentration that allows for short devices with reduced nonlinear distortions but also results in partial quenching and thus significant unsaturable absorption, even though the fiber is still able to amplify. Although the quenching degrades the average-power efficiency, the pulse energy remains high, and our results point to an increasingly promising outcome for short pulses. Furthermore, unlike unquenched fibers, the conversion efficiency improves at low repetition rates, which we attribute to smaller relative energy loss to quenched ions at higher pulse energy. A short (2.6 m) cladding-pumped partly quenched Er-doped fiber with 95-dB/m 1530-nm peak absorption and saturation energy estimated to 85 µJ reached 0.8 mJ of output energy when seeded by 0.2-µs, 23-µJ pulses. Thus, according to our results, pulses can be amplified to high energy in short highly Er-doped fibers designed to reduce nonlinear distortions at the expense of average-power efficiency.
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Weak van der Waals interactions between interlayers of two-dimensional layered materials result in disabled across-interlayer electron transfer and poor layered structural stability, seriously deteriorating their performance in energy applications. Herein, we propose a novel covalent assembly strategy for MoS2 nanosheets to realize unique MoS2 /SnS hollow superassemblies (HSs) by using SnS nanodots as covalent linkages. The covalent assembly based on all-inorganic and carbon-free concept enables effective across-interlayer electron transfer, facilitated ion diffusion kinetics, and outstanding mechanical stability, which are evidenced by experimental characterization, DFT calculations, and mechanical simulations. Consequently, the MoS2 /SnS HSs exhibit superb rate performance and long cycling stability in lithium-ion batteries, representing the best comprehensive performance in carbon-free MoS2 -based anodes to date. Moreover, the MoS2 /SnS HSs also show excellent sodium storage performance in sodium-ion batteries.