Morphology mediation of MoS_2 nanosheets with organic cations for fast sodium ion storage

Ion diffusion kinetics,depending on the size,tortuosity,connectivity of the channels,greatly affects the rate performance of the electrodes.Two-dimensional materials(2DMs) has emerged as promising electrode materials in the past decades.Howeve r,the applications of 2DMs electrodes are limited by the strong restacking problem,which leads to a poor rate capability.In this work,we for the first time mediated the mo rphology of molybdenum disulfide(MoS_2) nanosheets via a facile coagulation method;abundant sheet crumples were induced,which greatly enhance their surface accessibility and thus benefit the ion diffusion kinetics.Consequently,the crumpled-MoS_2 electrodes follow a capacitive Na-ion charge-storage mechanism to a large extent.Importantly,we demonstrate the special role of organic cations in the inter-sheet assembly configuration,in sharp contrast with that of alkali/alkaline-earth ones.We propose that organic cations cause edge/face contact of the sheets,instead of the face/face contact,thus affording a house-of-cards structure.     

Carbon spheres with rational designed surface and secondary particle-piled structures for fast and stable sodium storage

The electrochemical performance of hard carbon in sodium storage is still limited by its poor cycling stability and rate capability because of the sluggish kinetics process.In this study,we use a simple and effective method to accelerate the kinetics process by engineering the structure of the electrode to promote its surface and near-surface reactions.This goal is realized by the use of slightly aggregated ultra-small carbon spheres.The large specific surface area formed by the small spheres can provide abundant active sites for electrochemical reactions.The abundant mesopores and macropores derived from the secondary particle piled structure of the carbon spheres could facilitate the transport of electrolytes,shorten the diffusion distance of Na⁺and accommodate the volume expansion during cycling.Benefiting from these unique structure features,PG700-3(carbon spheres with the diameters of 40-60 nm carbonized at 700℃)exhibits high performance for sodium storage.A high reversible capacity of 163 mAh g^-1 could be delivered at a current density of 1.0 A g^-1 after 100 cycles.Interestingly,at a current density of 10.0 A g^-1,the specific capacity of PG700-3 gradually increases to 140 mAh g^-1 after 10000 cycles,corresponding to a capacity retention of 112%.Given the enhanced kinetics of SIBs reactions,PG700-3 exhibits an excellent rate capability,i.e.,230 and 138 mAh g^-1 at 0.1 and 5.0 A g^-1,respectively.This study provides a facile method to attain high performance anode materials for SIBs.The design strategy and improvement mechanism could be extended to other materials for high rate applications.     

Synthesis of self-assembled 3D flowerlike SnS2 nanostructures with enhanced lithium ion storage property

In this work, we reported a facile ethanol solvothermal approach to fabricate highly dispersive 3D flowerlike SnS₂ architectures. The effects of synthetic conditions, such as the solvent system and the concentration of thiourea, on the morphology of the products were investigated. A possible growth mechanism for the formation of 3D flowerlike architectures was preliminarily propounded on the basis of the evolution of the structure and the morphology with increasing the reaction time. As anode materials of rechargeable Li-ion batteries, the as-prepared flowerlike SnS₂ structures exhibited exceptional good electrochemical properties, which revealed a higher reversible capacity about 502 mA h g^?1 and more stable cyclic retention at 50th cycle than the as-prepared SnS₂ nanoplates. The reasons for the improved electrochemical performance of the flowerlike structures have been proposed. All the results demonstrated that they were potential anode materials in Li-ion batteries.     

Graphene-supported anatase TiO2 nanosheets for fast lithium storage

We have designed a unique hybrid structure by directly growing ultrathin anatase TiO(2) nanosheets onto graphene support for fast lithium storage. With exposed (001) high-energy facets, these TiO(2) nanosheets serve as ideal hosts for fast and efficient lithium storage. On the other hand, the graphene support serves as a highly conductive substrate that is beneficial to the high-rate performance.     

Universal architecture and defect engineering dual strategy for hierarchical antimony phosphate composite toward fast and durable sodium storage

Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume distortion,structural collapse,and ionic conduction interruption upon cycling.Herein,a hierarchical array-like nanofiber structure was designed to address these limitations by combining architecture engineering and anion tuning strategy,in which SbPO_4-x with oxygen vacancy ...     

Integration of cobalt selenide nanocrystals with interlayer expanded 3D Se/N Co-doped carbon networks for superior sodium-ion storage

Rational electrode structure design is of great significance for realizing superior Na⁺storage performance.Herein,a metal salt-induced polymer blowing-bubble approach followed by selenization procedure is developed to in-situ generate abundant sub-10 nm CoSe₂ nanocrystals on 3D Se/N co-doped carbon networks(CoSe₂@3DSNC).The phase transition from Co to CoSe₂ and the incorporation of Se into the carbon layer are realized simultaneously to establish above configuration,in which the CoSe₂ nanocrystals are anchored on interlayer expanded carbon networks.Such unique configuration endows electrode with lower Na+diffusion energy barrier,higher Na+storage capability and better structural durability.Reflected in SIBs,the optimized CoSe₂@3 DSNC delivers superior rate capability(310 m Ah g^-1 at 10 A g^-1)and excellent longterm cycling stability(409 m Ah g^-1 after 1200 cycles at 5 A g^-1).Moreover,this configuration can also be obtained in other metal selenides-carbon composite through a similar approach.     

Mg-based nanocomposites with high capacity and fast kinetics for hydrogen storage

Magnesium and its alloys have shown a great potential in effective hydrogen storage due to their advantages of high volumetric/gravimetric hydrogen storage capacity and low cost. However, the use of these materials in fuel cells for automotive applications at the present time is limited by high hydrogenation temperature and sluggish sorption kinetics. This paper presents the recent results of design and development of magnesium-based nanocomposites demonstrating the catalytic effects of carbon nanotubes and transition metals on hydrogen adsorption in these materials. The results are promising for the application of magnesium materials for hydrogen storage, with significantly reduced absorption temperatures and enhanced ab/desorption kinetics. High level Density Functional Theory calculations support the analysis of the hydrogenation mechanisms by revealing the detailed atomic and molecular interactions that underpin the catalytic roles of incorporated carbon and titanium, providing clear guidance for further design and development of such materials with better hydrogen storage properties.     

Synergistic effect from coaxially integrated CNTs@MoS2/MoO2 composite enables fast and stable lithium storage

Molybdenum oxide/sulfide materials are extensively evaluated as high-capacity anode candidates for lithium ion batteries.However,they suffer from rapid capacity decay and poor kinetics.Herein,we report on synergistic effect from structurally integrated coaxial CNTs@MoS₂/MoO₂ composite material on lithium storage,in which MoS₂/MoO₂ nanosheets are conformally decorated on carbon nanotubes(CNTs).In-situ synchrotron X-ray diffraction measurement is performed to elucidate synergistic effect among three MoS₂,MoO₂ and CNTs components for lithium storage.Reaction mechanism exploration reveals that the MoO₂ component undergoes reversible Li⁺intercalation via forming a stable Li_0.98 MoO₂ phase over a voltage range of 3.0 to 0.01 V vs.Li⁺/Li,without experiencing the conversion reaction into metallic Mo,which contributes to long-term stability during charge/discharge cycles.Meanwhile,lithium storage of MoS₂ is through lithium and sulfur reversible reaction after the initial conversion reaction of lithiated MoS₂ forming Li₂S and Mo.The CNTs component enhances electronic conductivity and structural stability by minimizing volume change and reaction strains in the CNTs@MoS₂/MoO₂ composite anode.A desired 68.2%capacity retention upon 2000 cycles at 10 A/g has been demonstrated for the CNTs@MoS₂/MoO₂ anode,revealing prominent reaction kinetics and structural stability for fast and stable lithium storage,superior to various Mo-based anode materials previously reported.The findings from this study,with the unique insight into the role of structural integrity in combining MoS₂/MoO₂ materials with the CNTs substrate,offers a strategy for designing composite anode materials for superior lithium storage performance.     

A 2D covalent organic framework with 4.7-nm pores and insight into its interlayer stacking

Two-dimensional layered covalent organic frameworks (2D COFs) organize π-electron systems into ordered structures ideal for exciton and charge transport and exhibit permanent porosity available for subsequent functionalization. A 2D COF with the largest pores reported to date was synthesized by condensing 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) and 4,4'-diphenylbutadiynebis(boronic acid) (DPB). The COF was prepared as both a high surface area microcrystalline powder as well as a vertically oriented thin film on a transparent single-layer graphene/fused silica substrate. Complementary molecular dynamics and density functional theory calculations provide insight into the interlayer spacing of the COF and suggest that adjacent layers are horizontally offset by 1.7-1.8 ?, in contrast to the eclipsed AA stacking typically proposed for these materials.     

2D corrugated magnesium carboxyphosphonate materials: topotactic transformations and interlayer "decoration" with ammonia

In this paper we report the synthesis and structural characterization of the 2D layered coordination polymer Mg(BPMGLY)(H(2)O)(2) (BPMGLY = bis-phosphonomethylglycine, (HO(3)PCH(2))(2)N(H)COO(2-)). The Mg ion is found in a slightly distorted octahedral environment formed by four phosphonate oxygens and two water molecules. The carboxylate group is deprotonated but noncoordinated. This compound is a useful starting material for a number of topotactic transformations. Upon heating at 140 °C one (of the two) Mg-coordinated water molecule is lost, with the archetype 2D structure maintaining itself. However, the octahedral Mg in Mg(BPMGLY)(H(2)O)(2) is now converted to trigonal bipyramidal in Mg(BPMGLY)(H(2)O). Upon exposure of the monohydrate Mg(BPMGLY)(H(2)O) compound to ammonia, one molecule of ammonia is inserted into the interlayer space and stabilized by hydrogen bonding. The 2D layered structure of the product Mg(BPMGLY)(H(2)O)(NH(3)) is still maintained, with Mg now acquiring a pseudo-octahedral environment. All of these topotactic transformations are also accompanied by changes in hydrogen bonding between the layers.     

A mesoporous 3D hybrid material with dual functionality for Hg2+ detection and adsorption

Dual-function hybrid material U1 was designed for simultaneous chromofluorogenic detection and removal of Hg(2+) in an aqueous environment. Mesoporous material UVM-7 (MCM41 type) with homogeneously distributed pores of about 2-3 nm in size, a large specific surface area exceeding 1000 m(2) g(-1), and nanoscale particles was used as an inorganic support. The mesoporous solid is decorated with thiol groups that were treated with squaraine dye III to give a 2,4-bis(4-dialkylaminophenyl)-3-hydroxy-4-alkylsulfanylcyclobut-2-enone (APC) derivative that is covalently anchored to the inorganic silica matrix. The solid was characterised by various techniques including X-ray diffraction, transmission electron microscopy, Raman spectroscopy, and nitrogen adsorption. This hybrid solid is the chemodosimeter for Hg(2+) detection. Hg(2+) reacts with the APC fragment in U1 with release of the squaraine dye into the solution, which turns deep blue and fluoresces strongly. Naked-eye Hg(2+) detection is thus accomplished in an easy-to-use procedure. In contrast, U1 remains silent in the presence of other thiophilic transition metal ions, alkali and alkaline earth metal ions, or anions ubiquitously present in water such as chloride, carbonate, sulfate, and phosphate. Material U1 acts not only as chemodosimeter that signals the presence of Hg(2+) down to parts-per-billion concentrations, but at the same time is also an excellent adsorbent for the removal of mercury cations from aqueous solutions. The amount of adsorbed mercury ranges from 0.7 to 1.7 mmol g(-1), depending on the degree of functionalisation. In addition, hybrid material U1 can be regenerated for both sensing and removal purposes. As far as we know, U1 is the first example of a promising new class of polyfunctional hybrid supports that can be used as both remediation and alarm systems by selective signalling and removal of target species of environmental importance. Model compounds based on silica gel (G1), fumed silica (F1), and micrometre-sized MCM-41 scaffolds (M1) were also prepared and studied for comparative purposes.     

Biomimetic fabrication of lotus-leaf-like structured polyaniline film with stable superhydrophobic and conductive properties

Superhydrophobic surfaces were successfully prepared on Ti/Si substrates via the fabrication of conductive polyaniline (PANI) nanowire film. The PANI nanowire film was synthesized by electrodeposition of aniline into the pores of an anodic aluminum oxide (AAO) template on Ti/Si substrate followed by the removal of the template. The surface showed conductivity and superhydrophobicity, even in many corrosive solutions, such as acidic or basic solutions over a wide pH range. Field emission scanning electron microscopy (FE-SEM) demonstrated that the binary geometric structures at micro- and nanometer scale bestowed the prerequisite roughness on the surfaces. The chemical surface modification made the PANI nanowire film superhydrophobic. The results demonstrated that the PANI nanowire film will have good potential applications in the preparation of conductive superhydrophobic surfaces.     

Thermodynamic simulation of performance of a dual cycle with stroke length and volumetric efficiency

This article presents finite-time thermodynamics analysis of an irreversible air standard dual cycle. An irreversible dual cycle model which is more close to practice is established. In this model, the effects of stroke length and volume efficiency by considering the nonlinear relation between the specific heats of working fluid and its temperature, the frictional loss, the internal irreversibility, and heat transfer loss are analyzed. The results show that if compression ratio is less than certain value, the power output increases with increasing stroke length, while if compression ratio exceeds certain value, the power output first increases and then starts to decrease with increasing stroke length. With further increase in compression ratio, the increase of stroke length results in decreasing the power output. The results also show that, throughout the compression ratio range, the power output increases with the increasing volumetric efficiency. The results obtained in this study are of importance to provide good guidance for performance evaluation and improvement of practical internal combustion engines.     

Water-processable nanocomposite based on polyaniline and 2D molybdenum disulfide for NIR-transparent ambipolar transport layers

Polymer nanocomposite based on stable water-dispersible polyaniline complex with poly(2-acrylamido-2-methyl-1-propanesulfonic acid) (PANI–PAMPSA) and 2D molybdenum disulphide (MoS₂) was developed. The nanocomposite layers obtained by drop-casting were characterized by Vis–NIR- and FTIR spectroscopies, as well as by atomic force, transmission electron, and Kelvin-probe microscopies, X-ray diffraction, cyclic voltammetry, Hall effect, and DC-conductivity measurements. It was shown that the preparation procedure allows easy adjusting of MoS₂ content in the nanocomposite resulting in the growth of DC conductivity by up to six times in the case of 20 wt% MoS₂ as compared with the additive-free PANI–PAMPSA complex. FTIR spectroscopy revealed the existence of hydrophobic interactions between PANI–PAMPSA and 2D MoS₂ nanophase, which facilitate interchain electron transfer. Hall effect studies showed that while increasing MoS₂ content in the nanocomposite, a transition occurs from monopolar hole transport, characteristic of PANI–PAMPSA, to ambipolar transport. This feature makes the obtained PANI–PAMPSA/MoS₂ composite a promising material for different optoelectronic devices, in particular tandem solar cells.     

Formamidinium-incorporated Dion-Jacobson phase 2D perovskites for highly efficient and stable photovoltaics

Dion-Jacobson phase two-dimensional (DJ 2D) perovskites,recently attracting considerable interests,exhibit excellent environmental stability and structural tuna...     

Nitrogen-doped carbon encapsulated in mesoporous TiO_2 nanotubes for fast capacitive sodium storage

Controllable synthesis of insertion-type anode materials with beneficial micro-and nanostructures is a promising approach for the synthesis of sodium-ion storage devices with high-reactivity and excellent electrochemical performance.In this study,we developed a sacrificial-templating route to synthesize TiO₂@N-doped carbon nanotubes(TiO₂@NC-NTs)with excellent electrochemical performance.The asprepared mesoporous TiO₂@NC-NTs with tiny nanocrystals of anatase TiO₂ wrapped in N-doped carbon layers showed a well-defined tube structure with a large specific surface area of 198 m² g^-1 and a large pore size of~5 nm.The TiO₂@NC-NTs delivered high reversible capacities of 158 m A h g^-1 at 2 C(1 C=335 m A g^-1)for 2200 cycles and 146 m A h g^-1 at 5 C for 4000 cycles,as well as an ultrahigh rate capability of up to 40 C with a capacity of 98 m A h g^-1.Even at a high current density of 10 C,a capacity of 138 m A h g^-1 could be delivered over 10,000 cycles.Thus,the synthesis of mesoporous TiO₂@NC-NTs was demonstrated to be an efficient approach for developing electrode materials with high sodium storage and long cycle life.     

Chemical interaction motivated structure design of layered metal carbonate hydroxide/MXene composites for fast and durable lithium ion storage

Rational architecture design has turned out to be an effective strategy in improving the electrochemical performance of electrode materials for batteries.Howeve...     

A pillared-bilayer porous coordination polymer with a 1D channel and a 2D interlayer space, showing unique gas and vapor sorption

A new 2D pillared-bilayer porous coordination polymer (PCP) has been synthesized and structurally characterized that shows selective adsorption of CO(2) over other gases (N(2), O(2), Ar, H(2), CH(4)) and guest selective single/double-step adsorption of vapor correlated to the successive confinement of adsorbates in a 1D channel and a 2D interlayer space.