A Universal Electronic Structure Modulation Strategy: Is Strong Adsorption Always Correlated with High Catalysis?

Unveiling the inherent link between polysulfide adsorption and catalytic activity is key to achieving optimal performance in Lithium-sulfur (Li-S) batteries. Current research on the sulfur reaction process mainly relies on the strong adsorption of catalysts to confine lithium polysulfides (LiPSs) to the cathode side, effectively suppressing the shuttle effect of polysulfides. However, is strong adsorption always correlated with high catalysis? The inherent relationship between adsorption and catalytic activity remains unclear, limiting the in-depth exploration and rational design of catalysts. Herein, the correlation between "d-band center-adsorption strength-catalytic activity" in porous carbon nanofiber catalysts embedded with different transition metals (M-PCNF-3, M = Fe, Co, Ni, Cu) is systematically investigated, combining the d-band center theory and the Sabatier principle. Theoretical calculations and experimental analysis results indicate that Co-PCNF-3 electrocatalyst with appropriate d-band center positions exhibits moderate adsorption capability and the highest catalytic conversion activity for LiPSs, validating the Sabatier relationship in Li-S battery electrocatalysts. These findings provide indispensable guidelines for the rational design of more durable cathode catalysts for Li-S batteries.

Photo-Assisted Rechargeable Metal Batteries: Principles, Progress, and Perspectives.

The utilization of diverse energy storage devices is imperative in the contemporary society. Taking advantage of solar power, a significant environmentally friendly and sustainable energy resource, holds great appeal for future storage of energy because it can solve the dilemma of fossil energy depletion and the resulting environmental problems once and for all. Recently, photo-assisted energy storage devices, especially photo-assisted rechargeable metal batteries, are rapidly developed owing to the ability to efficiently convert and store solar energy and the simple configuration, as well as the fact that conventional Li/Zn-ion batteries are widely commercialized. Considering many puzzles arising from the rapid development of photo-assisted rechargeable metal batteries, this review commences by introducing the fundamental concepts of batteries and photo-electrochemistry, followed by an exploration of the current advancements in photo-assisted rechargeable metal batteries. Specifically, it delves into the elucidation of device components, operating principles, types, and practical applications. Furthermore, this paper categorizes, specifies, and summarizes several detailed examples of photo-assisted energy storage devices. Lastly, it addresses the challenges and bottlenecks faced by these energy storage systems while providing future perspectives to facilitate their transition from laboratory research to industrial implementation.

Multi-functional integrated design of a copper foam-based cathode for high-performance lithium-oxygen batteries.

Lithium-oxygen batteries (LOBs) with extraordinarily high energy density are some of the most captivating energy storage devices. Designing an efficient catalyst system that can minimize the energy barriers and address the oxidant intermediate and side-product issues is the major challenge regarding LOBs. Herein, we have developed a new type of integrated cathode of Cu foam-supported hierarchical nanowires decorated with highly catalytic Au nanoparticles which achieves a good combination of a gas diffusion electrode and a catalyst electrode, contributing to the synchronous multiphase transport of ions, oxygen, and electrons as well as improving the cathode reaction kinetics effectively. Benefiting from such a unique hierarchical architecture, the integrated cathode delivered superior electrochemical performance, including a high discharge capacity of up to 11.5 mA h cm-2 and a small overpotential of 0.49 V at 0.1 mA cm-2, a favorable energy efficiency of 84.3% and exceptional cycling stability with nearly 1200 h at 0.1 mA cm-2 under a fixed capacity of 0.25 mA h cm-2. Furthermore, density functional theory (DFT) calculations further reveal the intrinsic direct catalytic ability to form/decompose Li2O2 during the ORR/OER process. As a consequence, this work provides an insightful investigation on the structural engineering of catalysts and holds great potential for advanced integrated cathode design for LOBs.

Recent Progress of Vertical Graphene: Preparation, Structure Engineering, and Emerging Energy Applications.

Vertical graphene (VG) nanosheets have garnered significant attention in the field of electrochemical energy applications, such as supercapacitors, electro-catalysis, and metal-ion batteries. The distinctive structures of VG, including vertically oriented morphology, exposed, and extended edges, and separated few-layer graphene nanosheets, have endowed VG with superior electrode reaction kinetics and mass/electron transportation compared to other graphene-based nanostructures. Therefore, gaining insight into the structure-activity relationship of VG and VG-based materials is crucial for enhancing device performance and expanding their applications in the energy field. In this review, the authors first summarize the fabrication methods of VG structures, including solution-based, and vacuum-based techniques. The study then focuses on structural modulations through plasma-enhanced chemical vapor deposition (PECVD) to tailor defects and morphology, aiming to obtain desirable architectures. Additionally, a comprehensive overview of the applications of VG and VG-based hybrids d in the energy field is provided, considering the arrangement and optimization of their structures. Finally, the challenges and future prospects of VG-based energy-related applications are discussed.

Electrospinning Photocatalysis Meet In Situ Irradiated XPS: Recent Mechanisms Advances and Challenges.

Producing solar fuels over photocatalysts under light irradiation is a considerable way to alleviate energy crises and environmental pollution. To develop the yields of solar fuels, photocatalysts with broad light absorption, fast charge carrier migration, and abundant reaction sites need to be designed. Electrospun 1D nanofibers with large specific areas and high porosity have been widely used in the efficient production of solar fuels. Nevertheless, it is challenging to do in-depth mechanism research on electrospun nanofiber-based photocatalysts since there are multiple charge transfer routes and various reaction sites in these systems. Here, the basic principles of electrospinning and photocatalysis are systemically discussed. Then, the different roles of electrospun nanofibers played in recent research to boost photocatalytic efficiency are highlighted. It is noteworthy that the working principles and main advantages of in situ irradiated photoelectron spectroscopy (ISI-XPS), a new technique to investigate migration routes of charge carriers and identify active sites in electrospun nanofibers based photocatalysts, are summarized for the first time. At last, a brief summary on the future orientation of photocatalysts based on electrospun nanofibers as well as the perspectives on the development of the ISI-XPS technique are also provided.

Metallic Powder Promotes Nitridation Kinetics for Facile Synthesis of (Oxy)Nitride Photocatalysts.

Nitrogen-containing semiconductors (including metal nitrides, metal oxynitrides, and nitrogen-doped metal oxides) have been widely researched for their application in energy conversion and environmental purification because of their unique characteristics; however, their synthesis generally encounters significant challenges owing to sluggish nitridation kinetics. Herein, a metallic-powder-assisted nitridation method is developed that effectively promotes the kinetics of nitrogen insertion into oxide precursors and exhibits good generality. By employing metallic powders with low work functions as electronic modulators, a series of oxynitrides (i.e., LnTaON2 (Ln = La, Pr, Nd, Sm, and Gd), Zr2 ON2 , and LaTiO2 N) can be prepared at lower nitridation temperatures and shorter nitridation periods to obtain comparable or even lower defect concentrations compared to those of the conventional thermal nitridation method, leading to superior photocatalytic performance. Moreover, some novel nitrogen-doped oxides (i.e., SrTiO3- x Ny and Y2 Zr2 O7- x Ny ) with visible-light responses can be exploited. As revealed by density functional theory (DFT) calculations, the nitridation kinetics are enhanced via the effective electron transfer from the metallic powder to the oxide precursors, reducing the activation energy of nitrogen insertion. The modified nitridation route developed in this work is an alternative method for preparing (oxy)nitride-based materials for energy/environment-related heterogeneous catalysis.

In Situ 1D Carbon Chain-Mail Catalyst Assembly for Stable Lithium-Sulfur Full Batteries.

The main obstacles for the commercial application of Lithium-Sulfur (Li-S) full batteries are the large volume change during charging/discharging process, the shuttle effect of lithium polysulfide (LiPS), sluggish redox kinetics, and the indisciplinable dendritic Li growth. Especially the overused of metal Li leads to the low utilization of active Li, which seriously drags down the actual energy density of Li-S batteries. Herein, an efficient design of dual-functional CoSe electrocatalyst encapsulated in carbon chain-mail (CoSe@CCM) is employed as the host both for the cathode and anode regulation simultaneously. The carbon chain-mail constituted by carbon encapsulated layer cross-linking with carbon nanofibers protects CoSe from the corrosion of chemical reaction environment, ensuring the high activity of CoSe during the long-term cycles. The Li-S full battery using this carbon chain-mail catalyst with a lower negative/positive electrode capacity ratio (N/P < 2) displays a high areal capacity of 9.68 mAh cm-2 over 150 cycles at a higher sulfur loading of 10.67 mg cm-2 . Additionally, a pouch cell is stable for 80 cycles at a sulfur loading of 77.6 mg, showing the practicality feasibility of this design.

Visible-light-responsive Photocatalyst Based on Nitrogen-doped Bulk Oxide YTaO4-x Ny for Z-scheme Overall Water Splitting.

Nitrogen doping into oxide has been proved to be an effective strategy to extend visible-light utilization of oxides with layered or channeled structure, but it is shortage for the bulk oxides free of layered or channeled structure. Here, we report a novel nitrogen-doped bulk oxide (denoted as YTaO4-x Ny ) with good visible light response. As benefited from the strong hybridization of N 2p and O 2p electronic state according to the density functional theory (DFT) calculations, the band gap (3.6 eV) of YTaO4 precursor was sharply narrowed to 2.4 eV on YTaO4-x Ny due to the obvious uplift of the valence band maximum (VBM). After decorated with the platinum cocatalyst, the Pt/YTaO4-x Ny was used as the H2 -evolving photocatalyst for assembly of Z-scheme overall water splitting system by coupling with the PtOx /WO3 as the oxygen evolution photocatalyst and using the I- /IO3- as the shuttle ions. This work enriches the material database of nitrogen-doped oxide with wide visible light absorption and shows its promising application in solar-to-chemical conversion.

Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X-Ray Photoelectron Spectroscopy for Lithium-Sulfur Battery.

The electrocatalysts are widely applied in lithium-sulfur (Li-S) batteries to selectively accelerate the redox kinetics behavior of Li2 S, in which bifunctional active sites are established, thereby improving the electrochemical performance of the battery. Considering that the Li-S battery is a complex closed "black box" system, the internal redox reaction routes and active sites cannot be directly observed and monitored especially due to the distribution of potential active-site structures and their dynamic reconstruction. Empirical evidence demonstrates that traditional electrochemical test methods and theoretical calculations only probe the net result of multi-factors on an average and whole scale. Herein, based on the amorphous TiO2- x @Ni selective bifunctional model catalyst, these limitations are overcome by developing a system that couples the light field and in situ irradiated X-ray photoelectron spectroscopy to synergistically convert the "black box" battery into a "see-through" battery for direct observation of the charge transportation, thus revealing that amorphous TiO2- x and Ni nanoparticle as the oxidation and reduction sites selectively promote the decomposition and nucleation of Li2 S, respectively. This work provides a universal method to achieve a deeper mechanistic understanding of bidirectional sulfur electrochemistry.

Fundamental Understanding of Nonaqueous and Hybrid Na-CO2 Batteries: Challenges and Perspectives.

Alkali metal-CO2 batteries, which combine CO2 recycling with energy conversion and storage, are a promising way to address the energy crisis and global warming. Unfortunately, the limited cycle life, poor reversibility, and low energy efficiency of these batteries have hindered their commercialization. Li-CO2 battery systems have been intensively researched in these aspects over the past few years, however, the exploration of Na-CO2 batteries is still in its infancy. To improve the development of Na-CO2 batteries, one must have a full picture of the chemistry and electrochemistry controlling the operation of Na-CO2 batteries and a full understanding of the correlation between cell configurations and functionality therein. Here, recent advances in CO2 chemical and electrochemical mechanisms on nonaqueous Na-CO2 batteries and hybrid Na-CO2 batteries (including O2 -involved Na-O2 /CO2 batteries) are reviewed in-depth and comprehensively. Following this, the primary issues and challenges in various battery components are identified, and the design strategies for the interfacial structure of Na anodes, electrolyte properties, and cathode materials are explored, along with the correlations between cell configurations, functional materials, and comprehensive performances are established. Finally, the prospects and directions for rationally constructing Na-CO2 battery materials are foreseen.

Detecting and Quantifying Wavelength-Dependent Electrons Transfer in Heterostructure Catalyst via In Situ Irradiation XPS.

The identity of charge transfer process at the heterogeneous interface plays an important role in improving the stability, activity, and selectivity of heterojunction catalysts. And, in situ irradiation X-ray photoelectron spectroscopy (XPS) coupled with UV light optical fiber measurement setup is developed to monitor and observe the photoelectron transfer process between heterojunction. However, the in-depth relationship of binding energy and irradiation light wavelength is missing based on the fact that the incident light is formed by coupling light with different wavelengths. Furthermore, a quantitative understanding of the charge transfer numbers and binding energy remains elusive. Herein, based on the g-C3 N4 /SnO2 model catalyst, a wavelength-dependent Boltzmann function to describe the changes of binding energy and wavelength through utilizing a continuously adjustable monochromatic light irradiation XPS technique is established. Using this method, this study further reveals that the electrons transfer number can be readily calculated forming an asymptotic model. This methodology provides a blueprint for deep understanding of the charge-transfer rules in heterojunction and facilitates the future development of highly active advanced catalysts.

Carbon Dots Mediated In Situ Confined Growth of Bi Clusters on g-C3 N4 Nanomeshes for Boosting Plasma-Assisted Photoreduction of CO2.

Synthesis of high-efficiency, cost-effective, and stable photocatalysts has long been a priority for sustainable photocatalytic CO2 reduction reactions (CRR), given its importance in achieving carbon neutrality goals under the new development philosophy. Fundamentally, the sluggish interface charge transportation and poor selectivity of products remain a challenge in the CRR progress. Herein, this work unveils a synergistic effect between high-density monodispersed Bi/carbon dots (CDs) and ultrathin graphite phase carbon nitride (g-C3 N4 ) nanomeshes for plasma-assisted photocatalytic CRR. The optimal g-C3 N4 /Bi/CDs heterojunction displays a high selectivity of 98% for CO production with a yield up to 22.7 µmol g-1 without any sacrificial agent. The in situ confined growth of plasmonic Bi clusters favors the production of more hot carriers and improves the conductivity of g-C3 N4 . Meanwhile, a built-in electric field driving force modulates the directional injection photogenerated holes from plasmonic Bi clusters and g-C3 N4 photosensitive units to adjacent CDs reservoirs, thus promoting the rapid separation and oriented transfer in the CRR process. This work sheds light on the mechanism of plasma-assisted photocatalytic CRR and provides a pathway for designing highly efficient plasma-involved photocatalysts.

Combined Plant Growth-Promoting Bacteria Inoculants Were More Beneficial than Single Agents for Plant Growth and Cd Phytoextraction of Brassica juncea L. during Field Application.

Single or combined plant growth-promoting bacteria (PGPB) strains were widely applied as microbial agents in cadmium (Cd) phytoextraction since they could promote plant growth and facilitate Cd uptake. However, the distinct functional effects between single and combined inoculants have not yet been elucidated. In this study, a field experiment was conducted with single, double and triple inoculants to clarify their divergent impacts on plant growth, Cd uptake and accumulation at different growth stages of Brassica juncea L. by three different PGPB strains (Cupriavidus SaCR1, Burkholdria SaMR10 and Sphingomonas SaMR12). The results show that SaCR1 + SaMR10 + SaMR12 combined inoculants were more effective for growth promotion at the bud stage, flowering stage, and mature stage. Single/combined PGPB agents of SaMR12 and SaMR10 were more efficient for Cd uptake promotion. In addition, SaMR10 + SaMR12 combined the inoculants greatly facilitated Cd uptake and accumulation in shoots, and enhanced the straw Cd extraction rates by 156%. Therefore, it is concluded that the application of PGPB inoculants elevated Cd phytoextraction efficiency, and the combined inoculants were more conductive than single inoculants. These results enriched the existing understanding of PGPB agents and provided technical support for the further exploration of PGPB interacting mechanisms strains on plant growth and Cd phytoextraction, which helped establish an efficient plant-microbe combined phytoremediation system and augment the phytoextraction efficiency in Cd-contaminated farmlands.

In Situ Monitored (N, O)-Doping of Flexible Vertical Graphene Films with High-Flux Plasma Enhanced Chemical Vapor Deposition for Remarkable Metal-Free Redox Catalysis Essential to Alkaline Zinc-Air Batteries.

Rechargeable zinc-air batteries (ZABs) have attracted great interests for emerging energy applications. Nevertheless, one of the major bottlenecks lies in the fabrication of bifunctional catalysts with high electrochemical activity, high stability, low cost, and free of precious and rare metals. Herein, a high-performance metal-free bifunctional catalyst is synthesized in a single step by regulating radicals within the recently invented high-flux plasma enhanced chemical vapor deposition (HPECVD) system equipped with in situ plasma diagnostics. Thus-derived (N, O)-doped vertical few-layer graphene film (VGNO) is of high areal population with perfect vertical orientation, tunable catalytic states, and configurations, thus enabling significantly enhanced electrochemical kinetic processes of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) with reference to milestone achievements to date. Application of such VGNO to aqueous ZABs (A-ZABs) and flexible solid-state ZABs (S-ZABs) exhibited high discharge power density and excellent cycling stability, which remarkably outperformed ZABs using benchmarked precious-metal based catalysts. The current work provides a solid basis toward developing low-cost, resource-sustainable, and eco-friendly ZABs without using any metals for outstanding OER and ORR catalysis.

Self-aligned stitching growth of centimeter-scale quasi-single-crystalline hexagonal boron nitride monolayers on liquid copper.

Two-dimensional hexagonal boron nitride (hBN) atomic crystals are excellent charge scattering screening interlayers for advanced electronic devices. Although wafer-scale single crystalline hBN monolayer films have been demonstrated on liquid Au and solid Cu (110) and (111) vicinal surfaces, their reproducible growth still remains challenging. Here, we report the facile self-aligned stitching growth of centimeter-scale quasi-single-crystalline hBN monolayer films through synergistic chemical vapor deposition growth kinetics and liquid Cu rheological kinetics control. The sublimation temperature of the ammonia borane precursor, H2 content and melting temperature of the Cu substrate are revealed to be the dominant factors that regulate hBN nucleation, growth and alignment. The flowing liquid Cu catalytic surface promotes efficient rotation of floating triangular hBN domains and provokes uniform self-alignment upon merging at a critical high temperature of 1105 °C. Identical aligned grains are constantly observed at multiple regions, which corroborate the homogeneous in-plane orientation and uniform stitching over the whole growth area. Continuous quasi-single-crystalline hBN monolayer films are produced by seamless stitching of aligned domains with the same polarity. The quasi-single-crystalline hBN monolayers are successfully included as charge scattering and trap site screening interlayers in the hBN/SiO2 gate insulator stack to build high performance InGaZnO field-effect transistors (FETs). Full suppression of hysteresis and twofold enhancement of field-effect mobility are realized for InGaZnO FETs built with hBN as the interface dielectric. The facile growth of large quasi-single-crystalline hBN monolayers on liquid Cu paves the way for future high-performance electronics.

Lithium-Sulfur Batteries Meet Electrospinning: Recent Advances and the Key Parameters for High Gravimetric and Volume Energy Density.

Lithium-sulfur (Li-S) batteries have been regarded as a promising next-generation energy storage technology for their ultrahigh theoretical energy density compared with those of the traditional lithium-ion batteries. However, the practical applications of Li-S batteries are still blocked by notorious problems such as the shuttle effect and the uncontrollable growth of lithium dendrites. Recently, the rapid development of electrospinning technology provides reliable methods in preparing flexible nanofibers materials and is widely applied to Li-S batteries serving as hosts, interlayers, and separators, which are considered as a promising strategy to achieve high energy density flexible Li-S batteries. In this review, a fundamental introduction of electrospinning technology and multifarious electrospinning-based nanofibers used in flexible Li-S batteries are presented. More importantly, crucial parameters of specific capacity, electrolyte/sulfur (E/S) ratio, sulfur loading, and cathode tap density are emphasized based on the proposed mathematic model, in which the electrospinning-based nanofibers are used as important components in Li-S batteries to achieve high gravimetric (WG ) and volume (WV ) energy density of 500 Wh kg-1 and 700 Wh L-1 , respectively. These systematic summaries not only provide the principles in nanofiber-based electrode design but also propose enlightening directions for the commercialized Li-S batteries with high WG and WV .

Array-Structured Double-Ion Cooperative Adsorption Sites as Multifunctional Sulfur Hosts for Lithium-Sulfur Batteries with Low Electrolyte/Sulfur Ratio.

Low electrolyte/sulfur ratio (E/S) is a crucial factor that promotes the development of lithium-sulfur batteries (LSBs) with desired energy density. However, it causes multiple problems, including a strong "shuttle effect" during both the cycle and storage process, and limited sulfur utilization. Herein, we develop a Na2Ti6O13 (NTO) nanowire array as a multifunctional sulfur host to simultaneously tackle both the above problems. The synergistic coordination between Na and Ti cations in NTO can accelerate the conversion of soluble polysulfides (PSs) to insoluble sulfides and significantly enhance their adsorption. Therefore, accumulation of PSs, which is the primary cause of the "shuttle effect", can be avoided in two ways. One is fast conversion kinetics during cycles; another is strong PS adsorption, which can suppress the disproportionation of PSs during storage. The as-prepared array represents an easy-to-infiltrate structure with efficient electron transport that allows good wetting ability of the conductive surface toward the electrolyte. Therefore, it helps improve sulfur utilization that is mainly limited by the presence of unwetted conductive surface. Consequently, NTO/sulfur array cathodes exhibit high sulfur utilization and extended cycle- and shelf-lives at a low E/S (5:1). Our work suggests that array materials featuring cooperative multi-ion adsorption sites are promising hosts for LSBs.

Synthesis of a Visible-Light-Responsive Perovskite SmTiO2 N Bifunctional Photocatalyst via an Evaporation-Assisted Layered-Precursor Strategy.

Development of visible-light-responsive oxynitride photocatalysts has been highly inspired for promising solar-to-chemical conversion, but the number of Ti-based oxynitrides is scarce because of the relatively low thermal stability of Ti4+ ions under ammonia flow. Here, the feasible synthesis of a novel perovskite SmTiO2 N from the layered NaSmTiO4 precursor is demonstrated to exhibit wide visible-light response with a bandgap of ≈2.1 eV and to show effective water reduction and oxidation functionalities under visible-light irradiation. The successful preparation mainly results from the synergistic effect of the layered structure of NaSmTiO4 and the evaporation spillover of Na+ ions, both of which are favorable for ammonia diffusion to accelerate the substitution of nitrogen to oxygen atoms and to shorten the nitridation time. The thermodynamic and kinetic feasibility of SmTiO2 N for water splitting are investigated in detail, and its optimal apparent quantum efficiency (AQE) of water oxidation reaches 16.7% at 420 ± 10 nm, higher by far than that of most previous visible-light-responsive photocatalysts. Interestingly, a series of oxynitrides RTiO2 N (R = La, Pr, Nd) are similarly synthesized by the alkali-metal evaporation-assisted layered-precursor strategy, demonstrating its generality to prepare visible-light-responsive (oxy)nitride photocatalysts containing reducible metals for solar energy conversion.

Dynamic Reaction Mechanism of P-N-Switched H2-Sensing Performance on a Pt-Decorated TiO2 Surface.

Pt decoration is known to be one of the most promising strategies to enhance the performance of TiO2 hydrogen gas sensors, while the effect of Pt-decorating concentration on the sensing performance of TiO2 and the specific interaction between Pt and TiO2 have not been fully investigated. Here, a series of TiO2 nanoarray thin films with differing amounts of Pt decorated (Pt/TiO2) is fabricated, and the H2-sensing performance is evaluated. A switch in the response from P-type to N-type is observed with increasing Pt decoration. The response additionally depends on the H2 concentration: resistance increases in low H2 concentrations and decreases in hydrogen concentrations higher than 40 ppm. This is explained by the competitive adsorption of hydrogen between the Pt nanoparticles (Pt NPs) and the exposed TiO2 surface. The preference for H2 adsorption and splitting between Pt and TiO2 is established by DFT calculations. Humidity brings preferential adsorption of H2O on the surface of Pt, which affects the following adsorption and splitting of H2, thus resulting in a P-N switch of the sensing performance. The detailed dynamic reaction process is described according to the findings.

In Situ Electrochemical Intercalation-Induced Phase Transition to Enhance Catalytic Performance for Lithium-Sulfur Battery.

Accelerating the conversion of polysulfide to inhibit shutting effect is a promising approach to improve the performance of lithium-sulfur batteries. Herein, the hollow titanium nitride (TiN)/1T-MoS2 heterostructure nanospheres are designed with efficient electrocatalysis properties serving as a sulfur host, which is formed by in situ electrochemical intercalation from TiN/2H-MoS2 . Metallic, few-layered 1T-MoS2 nanosheets with abundant active sites decorated on TiN nanospheres enable fast electron transfer, high adsorption ability toward polysulfides, and favorable catalytic activity contributing to the conversion kinetics of polysulfides. Benefiting from the synergistic effects of these favorable features, the as-developed hollow TiN/1T-MoS2 nanospheres with advanced architecture design can achieve a high discharge capacity of 1273 mAh g-1 at 0.1 C, good rate performance with a capacity retention of 689 mAh g-1 at 2 C, and long cycling stability with a low-capacity fading rate of 0.051% per cycle at 1 C for 800 cycles. Notably, the TiN/1T-MoS2 /S cathode with a high sulfur loading of up to 7 mg cm-2 can also deliver a high capacity of 875 mAh g-1 for 50 cycles at 0.1 C. This work promotes the prospect application for TiN/1T-MoS2 in lithium-sulfur batteries.