Synchronously Consolidating Li, Se, S, and C for Robust Li-SeS Batteries.

S-redox involving solvated polysulfides is accompanied by volumetric change and structural decay of the S-based cathodes. Here, we propose a synchronous construction strategy for consolidating Li, Se, S, and C elements within a composite cathode via a paradigm reaction of 8Li+2Se+CS2 = 2Li4SeS+C. The obtained composite features crystalline Li4SeS encapsulated in a carbon nanocage (Li4SeS@C), exhibiting ultrahigh electrical conductivity, ultralow activation barrier, and excellent structural integrity, accordingly enabling large specific capacity (615 mAh g-1) and high capacity retention (87.3% after 350 cycles) at 10 A g-1. TOF-SIMS demonstrates its superior volumetric efficiency to a similar derivative SeS@C (2Se+CS2 = 2SeS+C), and DFT reveals its lower activation barrier than Li2S@C and Li2Se@C. This consolidation design significantly improves the electrochemical performance of S-based cathodes, and the paradigm reaction guarantees structural diversity and flexibility. Moreover, employing a synchronous construction mechanism to maximize the synergistic effect between element consolidation and carbon encapsulation opens up a new approach for developing robust S or chalcogenide cathodes.

In-Situ Synthesis of Carbon-Encapsulated Atomic Cobalt as Highly Efficient Polysulfide Electrocatalysts for Highly Stable Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries have been considered as one of the most promising electrochemical energy storage systems because of their high energy density. However, a series of issues severely limit the practical performances of Li-S batteries such as low conductivity, significant volume change, and shuttle effect. The hollow carbon spheres with huge voids and high electrical conductivity are promising as sulfur hosts. Unfortunately, the nonpolar nature of carbon materials cannot prevent the shuttle effect effectively. In this case, the atomic cobalt is introduced to a nitrogen-doped hollow carbon sphere (ACo@HCS) through polymerization and controlled pyrolysis. The atomic cobalt dopants not only act as active sites to restrict the shuttle effect, but also can promote the kinetics of the sulfur redox reactions. ACo@HCS acting as sulfur host exhibits a high discharge capacity (1003 mAh g-1 ) at a 1.0 C rate after 500 cycles, and the corresponding decay rate is as low as 0.002% per cycle. This exciting work paves a new way to design high-performance Li-S batteries.

New Nanoconfined Galvanic Replacement Synthesis of Hollow Sb@C Yolk-Shell Spheres Constituting a Stable Anode for High-Rate Li/Na-Ion Batteries.

In the current research project, we have prepared a novel Sb@C nanosphere anode with biomimetic yolk-shell structure for Li/Na-ion batteries via a nanoconfined galvanic replacement route. The yolk-shell microstructure consists of Sb hollow yolk completely protected by a well-conductive carbon thin shell. The substantial void space in the these hollow Sb@C yolk-shell particles allows for the full volume expansion of inner Sb while maintaining the framework of the Sb@C anode and developing a stable SEI film on the outside carbon shell. As for Li-ion battery anode, they displayed a large specific capacity (634 mAh g-1), high rate capability (specific capabilities of 622, 557, 496, 439, and 384 mAh g-1 at 100, 200, 500, 1000, and 2000 mA g-1, respectively) and stable cycling performance (a specific capacity of 405 mAh g-1 after long 300 cycles at 1000 mA g-1). As for Na-ion storage, these yolk-shell Sb@C particles also maintained a reversible capacity of approximate 280 mAh g-1 at 1000 mA g-1 after 200 cycles.

Air-Stable Porous Fe2N Encapsulated in Carbon Microboxes with High Volumetric Lithium Storage Capacity and a Long Cycle Life.

The development of inexpensive electrode materials with a high volumetric capacity and long cycle-life is a central issue for large-scale lithium-ion batteries. Here, we report a nanostructured porous Fe2N anode fully encapsulated in carbon microboxes (Fe2N@C) prepared through a facile confined anion conversion from polymer coated Fe2O3 microcubes. The resulting carbon microboxes could not only protect the air-sensitive Fe2N from oxidation but also retain thin and stable SEI layer. The appropriate internal voids in the Fe2N cubes help to release the volume expansion during lithiation/delithiation processes, and Fe2N is kept inside the carbon microboxes without breaking the shell, resulting in a very low electrode volume expansion (the electrode thickness variation upon lithiation is ∼9%). Therefore, the Fe2N@C electrodes maintain high volumetric capacity (1030 mA h cm-3 based on the lithiation-state electrode volume) comparable to silicon anodes, stable cycling performance (a capacity retention of over 91% for 2500 cycles), and excellent rate performance. Kinetic analysis reveals that the Fe2N@C shows an enhanced contribution of capacitive charge mechanism and displays typical pseudocapacitive behavior. This work provides a new direction on designing and constructing nanostructured electrodes and protective layer for air unstable conversion materials for potential applications as a lithium-ion battery/capacitor electrode.

MOF-Derived Hollow Co9 S8 Nanoparticles Embedded in Graphitic Carbon Nanocages with Superior Li-Ion Storage.

Novel electrode materials consisting of hollow cobalt sulfide nanoparticles embedded in graphitic carbon nanocages (HCSP⊂GCC) are facilely synthesized by a top-down route applying room-temperature synthesized Co-based zeolitic imidazolate framework (ZIF-67) as the template. Owing to the good mechanical flexibility and pronounced structure stability of carbon nanocages-encapsulated Co9 S8 , the as-obtained HCSP⊂GCC exhibit superior Li-ion storage. Working in the voltage of 1.0-3.0 V, they display a very high energy density (707 Wh kg(-1) ), superior rate capability (reversible capabilities of 536, 489, 438, 393, 345, and 278 mA h g(-1) at 0.2, 0.5, 1, 2, 5, and 10C, respectively), and stable cycling performance (≈26% capacity loss after long 150 cycles at 1C with a capacity retention of 365 mA h g(-1) ). When the work voltage is extended into 0.01-3.0 V, a higher stable capacity of 1600 mA h g(-1) at a current density of 100 mA g(-1) is still achieved.

Heterostructured MnSe/FeSe nanorods encapsulated by carbon with enhanced Na+ diffusion as anode materials for sodium-ion batteries.

The natural abundance of sodium has fostered the development of sodium-ion batteries for large-scale energy storage. However, the low capacity of the anodes hinders their future application. Herein, carbon-encapsulated MnSe-FeSe nanorods (MnSe-FeSe@C) have been fabricated by the in-situ transformation from polydopamine-coated MnO(OH)-Fe2O3. The heterostructure constructed by MnSe and FeSe nanocrystals induces the formation of built-in electric fields, accelerating electron transfer and ion diffusion, thereby improving reaction kinetics. In addition, carbon enclosure can buffer the volumetric stress and enhance the electrical conductivity. These aspects cooperatively endow the anode with superior cycling stability and distinguished rate performance. Specifically, the discharge capacity of MnSe-FeSe@C reaches 414.3 mA h g-1 at 0.1 A g-1 and 388.8 mA h g-1 even at a high current density of 5.0 A g-1. In addition, it still retains a high reversible capacity of 449.2 mA h g-1 after 700 long cycles at 1.0 A g-1. Further, the ab initio calculation has been employed to authenticate the existence of the built-in electric field by Bader charge, indicating that 0.24 electrons in MnSe were transferred to FeSe. The in-situ XRD has been used to evaluate the phase transition during the charging/discharging process, revealing the sodium ion storage mechanism. The construction of heterostructure material paves a new way to design performance-enhanced anode materials for sodium-ion batteries.

Flame spray pyrolyzed carbon-encapsulated Au/Fe3O4 nanoaggregates enabled efficient photothermal therapy and magnetic hyperthermia of esophageal cancer cells.

Multifunctional magneto-plasmonic nanoparticles with magnetic hyperthermia and photothermal therapy could kill cancer cells efficiently. Herein, carbon-encapsulated Au/Fe3O4 (Au/Fe3O4@C) was fabricated using an enclosed flame spray pyrolysis. The nanostructures, including an Fe3O4 core (51.9-55.2 nm) with a decreasing carbon shell thickness and an Au core (4.68-8.75 nm) coated with 2-4 graphite layers, were tailored by tuning the C2H4 content in the reacting gas mixture. Saturation magnetization (33.7-48.2 emu/g) and optical absorption were determined. The carbon shell facilitated the dispersion of Au/Fe3O4 and restrained their laser-induced and magnetic field-induced coalescence and growth. Au/Fe3O4@C exhibited excellent magnetic resonance imaging capability (91.4 mM-1 s-1) and photothermal performance (65.4°C for 0.8 mg/mL Au/Fe3O4@C at a power density of 1.0 W/cm2 after 300 s near-IR laser irradiation (808 nm)). Moreover, the combined application of photothermal and magnetic-heating properties reduced the required intensity of both laser and magnetic field compared to the intensity of separate situations. Our work provides a unique, intriguing approach to preparing multicomponent core/shell nanoaggregates that are promising candidates for esophageal cancer cell therapy.

High-Performance Lithium-Ion Batteries with High Stability Derived from Titanium-Oxide- and Sulfur-Loaded Carbon Spherogels.

This study presents a novel approach to developing high-performance lithium-ion battery electrodes by loading titania-carbon hybrid spherogels with sulfur. The resulting hybrid materials combine high charge storage capacity, electrical conductivity, and core-shell morphology, enabling the development of next-generation battery electrodes. We obtained homogeneous carbon spheres caging crystalline titania particles and sulfur using a template-assisted sol-gel route and carefully treated the titania-loaded carbon spherogels with hydrogen sulfide. The carbon shells maintain their microporous hollow sphere morphology, allowing for efficient sulfur deposition while protecting the titania crystals. By adjusting the sulfur impregnation of the carbon sphere and varying the titania loading, we achieved excellent lithium storage properties by successfully cycling encapsulated sulfur in the sphere while benefiting from the lithiation of titania particles. Without adding a conductive component, the optimized material provided after 150 cycles at a specific current of 250 mA g-1 a specific capacity of 825 mAh g-1 with a Coulombic efficiency of 98%.

Rational Design of N-Doped Carbon-Coated Cobalt Nanoparticles for Highly Efficient and Durable Photothermal CO2 Conversion.

Photothermal CO2 hydrogenation to high-value-added chemicals and fuels is an appealing approach to alleviate energy and environmental concerns. However, it still relies on the development of earth-abundant, efficient, and durable catalysts. Here, the design of N-doped carbon-coated Co nanoparticles (NPs), as a photothermal catalyst, synthesized through a two-step pyrolysis of Co-based ZIF-67 precursor, is reported. Consequently, the catalyst exhibits remarkable activity and stability for photothermal CO2 hydrogenation to CO with a 0.75 mol gcat -1 h-1 CO production rate under the full spectrum of light illumination. The high activity and durability of these Co NPs are mainly attributed to the synergy of the attuned size of Co NPs, the thickness of carbon layers, and the N doping species. Impressively, the experimental characterizations and theoretical simulations show that such a simple N-doped carbon coating strategy can effectively facilitate the desorption of generated CO and activation of reactants due to the strong photothermal effect. This work provides a simple and efficient route for the preparation of highly active and durable nonprecious metal catalysts for promising photothermal catalytic reactions.

Fe-Co Alloy Nanoparticles Dispersed in Polymer-Derived Carbon Support: Effect of Initial Polymer Nature on the Size, Structure and Magnetic Properties.

Fe-Co alloy nanoparticles with different sizes, supported by carbon derived from several polymers, namely polyacrylonitrile, polyvinyl alcohol and chitosan, have been synthesized by a one-pot method involving simultaneous metal nanoparticle formation and polymer carbonization. The method involves the joint dissolution of metal salts and a polymer, followed by annealing of the resulting dried film. Detailed XRD analysis confirmed the formation of Fe-Co alloy nanoparticles in each sample, regardless of the initial polymer used. Transmission electron microscopy images showed that the Fe-Co nanoparticles were all spherical, were homogeneously distributed within the carbon support and varied by size depending on the initial polymer nature and synthesis temperature. Fe-Co nanoparticles supported by polyacrylonitrile-derived carbon exhibited the smallest size (6-12 nm), whereas nanoparticles on chitosan-derived carbon support were characterized by the largest particle size (13-38 nm). The size dependence of magnetic properties were studied by a vibrating sample magnetometer at room temperature. For the first time, the critical particle size of Fe-Co alloy nanoparticles with equiatomic composition has been experimentally determined as 13 nm, indicating the transition of magnetic properties from ferromagnetic to superparamagnetic.