Structural phase transitions can be used to alter the properties of a material without adding any additional elements and are therefore of significant technological value. It was found that the hexagonal-SnS2 phase can be transformed into the orthorhombic-SnS phase after an annealing step in an argon atmosphere, and the thus transformed SnS shows enhanced sodium-ion storage performance over that of the SnS2, which is attributed to its structural advantages. Here, we provide the first report on a SnS@graphene architecture for application as a sodium-ion battery anode, which is built from two-dimensional SnS and graphene nanosheets as complementary building blocks. The as-prepared SnS@graphene hybrid nanostructured composite delivers an excellent specific capacity of 940 mAh g(-1)and impressive rate capability of 492 and 308 mAh g(-1) after 250 cycles at the current densities of 810 and 7290 mA g(-1), respectively. The performance was found to be much better than those of most reported anode materials for Na-ion batteries. On the basis of combined ex situ Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and ex situ X-ray diffraction, the formation mechanism of SnS@graphene and the synergistic Na-storage reactions of SnS in the anode are discussed in detail. The SnS experienced a two-structural-phase transformation mechanism (orthorhombic-SnS to cubic-Sn to orthorhombic-Na3.75Sn), while the SnS2 experienced a three-structural-phase transformation mechanism (hexagonal-SnS2 to tetragonal-Sn to orthorhombic-Na3.75Sn) during the sodiation process. The lesser structural changes of SnS during the conversion are expected to lead to good structural stability and excellent cycling stability in its sodium-ion battery performance. These results demonstrate that the SnS@graphene architecture offers unique characteristics suitable for high-performance energy storage application.
Constructing heterostructures can endow materials with fascinating performance in high-speed electronics, optoelectronics, and other applications owing to the built-in charge-transfer driving force, which is of benefit to the specific charge-transfer kinetics. Rational design and controllable synthesis of nano-heterostructure anode materials with high-rate performance, however, still remains a great challenge. Herein, ultrafine SnS/SnO2 heterostructures were successfully fabricated and showed enhanced charge-transfer capability. The mobility enhancement is attributed to the interface effect of heterostructures, which induces an electric field within the nanocrystals, giving them much lower ion-diffusion resistance and facilitating interfacial electron transport.
As an emerging electrochemical energy storage device, potassium-ion batteries (PIBs) have drawn growing interest due to the resource-abundance and low cost of potassium. Graphite-based materials, as the most common anodes for commercial Li-ion batteries, have a very low capacity when used an anode for Na-ion batteries, but they show reasonable capacities as anodes for PIBs. The practical application of graphitic materials in PIBs suffers from poor cyclability, however, due to the large interlayer expansion/ shrinkage caused by the intercalation/deintercalation of potassium ions. Here, a highly graphitic carbon nanocage (CNC) is reported as a PIBs anode, which exhibits excellent cyclability and superior depotassiation capacity of 175 mAh g-1at 35 C. The potassium storage mechanism in CNC is revealed by cyclic voltammetry as due to redox reactions (intercalation/deintercalation) and double-layer capacitance (surface adsorption/desorption). The present results give new insights into structural design for graphitic anode materials in PIBs and understanding the double-layer capacitance effect in alkali metal ion batteries.
Potassium-ion batteries (PIBs) are a promising alternative to lithium-ion batteries because potassium is an abundant natural resource. To date, PIBs are in the early stages of exploration and only a few anode materials have been investigated. This study reports a cobalt sulfide and graphene (CoS@G) composite as anode electrode for PIBs for the first time. The composite features interconnect quantum dots of CoS nanoclusters uniformly anchored on graphene nanosheets. The coexistence of CoS quantum dot nanoclusters and graphene nanosheets endows the composite with large surface area, highly conductive network, robust structural stability, and excellent electrochemical energy storage performance. An unprecedented capacity of 310.8 mA h g −1 at 500 mA g −1 is obtained after 100 cycles, with a rate capability better than an equivalent sodium-ion batteries (SIBs). This work provides the evidence that PIBs can be a promising alternative to SIBs, especially at high charge-discharge rates. The development of the CoS@G anode material also provides the basis of expanding the library of suitable anode materials for PIBs.
The exploration of efficient nonprecious metal eletrocatalysis of the hydrogen evolution reaction (HER) is an extraordinary challenge for future applications in sustainable energy conversion. The family of first-row-transition-metal dichalcogenides has received a small amount of research, including the active site and dynamics, relative to their extraordinary potential. In response, we developed a strategy to achieve synergistically active sites and dynamic regulation in first-row-transition-metal dichalcogenides by the heterogeneous spin states incorporated in this work. Specifically, taking the metallic Mn-doped pyrite CoSe2 as a self-adaptived, subtle atomic arrangement distortion to provide additional active edge sites for HER will occur in the CoSe2 atomic layers with Mn incorporated into the primitive lattice, which is visually verified by HRTEM. Synergistically, the density functional theory simulation results reveal that the Mn incorporation lowers the kinetic energy barrier by promoting H-H bond formation on two adjacently adsorbed H atoms, benefiting H2 gas evolution. As a result, the Mn-doped CoSe2 ultrathin nanosheets possess useful HER properties with a low overpotential of 174 mV, an unexpectedly small Tafel slope of 36 mV/dec, and a larger exchange current density of 68.3 μA cm(-2). Moreover, the original concept of coordinated regulation presented in this work can broaden horizons and provide new dimensions in the design of newly highly efficient catalysts for hydrogen evolution.
Ultrathin 2D materials can offer promising opportunities for exploring advanced energy storage systems, with satisfactory electrochemical performance. Engineering atomic interfaces by stacking 2D crystals holds huge potential for tuning material properties at the atomic level, owing to the strong layer-layer interactions, enabling unprecedented physical properties. In this work, atomically thin Bi MoO sheets are acquired that exhibit remarkable high-rate cycling performance in Li-ion batteries, which can be ascribed to the interlayer coupling effect, as well as the 2D configuration and intrinsic structural stability. The unbalanced charge distribution occurs within the crystal and induces built-in electric fields, significantly boosting lithium ion transfer dynamics, while the extra charge transport channels generated on the open surfaces further promote charge transport. The in situ synchrotron X-ray powder diffraction results confirm the material's excellent structural stability. This work provides some insights for designing high-performance electrode materials for energy storage by manipulating the interface interaction and electronic structure.
Nitrate is ar aw ingredient for the production of fertilizer,g unpowder,a nd explosives.D eveloping an alternative approach to activate the NNbond of naturally abundant nitrogen to form nitrate under ambient conditions will be of importance.Herein, pothole-rich WO 3 was used to catalyse the activation of N Nc ovalent triple bonds for the direct nitrate synthesis at room temperature.T he pothole-rich structure endues the WO 3 nanosheet more dangling bonds and more easily excited high momentum electrons,w hicho vercome the two major bottlenecks in NNb ond activation, that is,p oor binding of N 2 to catalytic materials and the high energy involved in this reaction. The average rate of nitrate production is as high as 1.92 mg g À1 h À1 under ambient conditions,without any sacrificial agent or precious-metal co-catalysts.M ore generally,t he concepts will initiate an ew pathwayf or triggering inert catalytic reactions.
The concept of an all-integrated design with multifunctionalization is widely employed in optoelectronic devices, sensors, resonator systems, and microfluidic devices, resulting in benefits for many ongoing research projects. Here, maintaining structural/electrode stability against large volume change by means of an all-integrated design is realized for silicon anodes. An all-integrated silicon anode is achieved via multicomponent interlinking among carbon@void@silica@silicon (CVSS) nanospheres and cross-linked carboxymethyl cellulose and citric acid polymer binder (c-CMC-CA). Due to the additional protection from the silica layer, CVSS is superior to the carbon@void@silicon (CVS) electrode in terms of long-term cyclability. The as-prepared all-integrated CVSS electrode exhibits high mechanical strength, which can be ascribed to the high adhesivity and ductility of c-CMC-CA binder and the strong binding energy between CVSS and c-CMC-CA, as calculated based on density functional theory (DFT). This electrode exhibits a high reversible capacity of 1640 mA h g after 100 cycles at a current density of 1 A g , high rate performance, and long-term cycling stability with 84.6% capacity retention after 1000 cycles at 5 A g .
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