Halide Ordering Enables Superior Charge Transport in 3D (NMPDA)Pb2 I4 Br2 Perovskitoid Single Crystal.

Halide composition engineering has been demonstrated as an effective strategy for optical and electronic properties modulation in 3D perovskites. While the impact of halide mixing on the structural and charge transport properties of 3D perovskitoids remains largely unexplored. Herein, it is demonstrated that bromine (Br) mixing in 3D (NMPDA)Pb2 I6 (NMPDA = N-methyl-1,3-propane diammonium) perovskitoid yields stabilized (NMPDA)Pb2 I4 Br2 with specific ordered halide sites, where Br ions locate at the edge-sharing sites. The halide ordered structure enables stronger H-bonds, shorter interlayer distance, and lower octahedra distortion in (NMPDA)Pb2 I4 Br2 with respect to the pristine (NMPDA)Pb2 I6 . These attributes further result in high ion migration activation energy, low defect states density, and enhanced carrier mobility-lifetime product (µτ), as underpinned by the electrical properties investigation and DFT calculations. Remarkably, the parallel configured photodetector based on (NMPDA)Pb2 I4 Br2 single crystal delivers a high on/off current ratio of 3.92 × 103 , a satisfying photoresponsivity and detectivity of 0.28 A W-1 and 3.05 × 1012 Jones under 10.94 µW cm-2 irradiation, superior to that of (NMPDA)Pb2 I6 and the reported 3D perovskitoids. This work sheds novel insight on exploring 3D mixed halide perovskitoids toward advanced and stable optoelectronic devices.

Large Interlayer Distance and Heteroatom-Doping of Graphite Provide New Insights into the Dual-Ion Storage Mechanism in Dual-Carbon Batteries.

Dual-ion batteries (DIBs) is a promising technology for large-scale energy storage. However, it is still questionable how material structures affect the anion storage behavior. In this paper, we synthesis graphite with an ultra-large interlayer distance and heteroatomic doping to systematically investigate the combined effects on DIBs. The large interlayer distance of 0.51 nm provides more space for anion storage, while the doping of the heteroatoms reduces the energy barriers for anion intercalation and migration and enhances rapid ionic storage at interfaces simultaneously. Based on the synergistic effects, the DIBs composed of carbon cathode and lithium anode afford ultra-high capacity of 240 mAh g-1 at current density of 100 mA g-1 . Dual-carbon batteries (DCBs) using the graphite as both of cathode and anode steadily cycle 2400 times at current density of 1 A g-1 . Hence, this work provides a reference to the strategy of material designs of DIBs and DCBs.

Edge-Nitrogen Enriched Porous Carbon Nanosheets Anodes with Enlarged Interlayer Distance for Fast Charging Sodium-Ion Batteries.

The application of nitrogen-doped porous carbon for sodium-ion batteries (SIBs) has attracted tremendous attention. Herein, a series of edge-nitrogen enriched porous carbon nanosheets (ENPCNs) are synthesized by annealing g-C3 N4 and glucose in a sealed graphite crucible at different temperatures (T = 700, 800, and 900 °C). Surprisingly, under the closed thermal treatment condition, the ENPCNs-T possess a high N-doping level (>12.62 at%) and different carbon interlayer distance ranging from 0.429 to 0.487 nm. By correlating the carbon interlayer distance with the N configurations of ENPCNs-T materials, a reasonable perception of the important influence of pyrrolic N on the increase of carbon interlayer distance is proposed. When applied as anode materials for SIBs, the ENPCNs-800 exhibits a remarkable capacity (294.1 mAh g-1 at 0.1 A g-1 ), excellent rate performance (132.8 mAh g-1 at 10 A g-1 ), and outstanding cycle life (180.6 mAh g-1 at 1 A g-1 after 1000 cycles with a capacity retention of 104.7%). Meanwhile, the characterizations of cyclic voltammetry, galvanostatic intermittent titration technique, and electrochemical impedance spectroscopy demonstrate that the edge-nitrogen doping and enlarged carbon interlayer distance improve the capacity and fast charging performance of ENPCNs-800. Considering the detailed investigation of the Na+ storage mechanism and excellent electrochemical performance of ENPCNs-800, this work can pave a new avenue for the research of SIBs.

Atomic-Scale Laminated Structure of O-Doped WS2 and Carbon Layers with Highly Enhanced Ion Transfer for Fast-Charging Lithium-Ion Batteries.

WS2 anode materials show huge potential for fast-charging lithium-ion batteries (LIBs) due to the naturally good 2D diffusion pathways but suffer from large Li+ diffusion barrier energy and poor intrinsic electrical conductivity. Here, a defect-rich atomic-scale laminated structure of WS2 and C (D-WS2 -C) with O doping and enlarged interlayer distance from 0.62 to 1.06 nm of WS2 is first fabricated, which is assembled into micron-sized spheres to prepare WS2 /C composite microspheres. D-WS2 -C with maximized molecular layer contact area between WS2 and carbon and large interlayer spacing greatly enhances the electrical conductivity of WS2 and reduces Li-ion diffusion energy barrier, confirmed by density functional theory calculations. Besides, the unique D-WS2 -C enables the formation of vast superfine W nanoparticles (1-2 nm) during the conversation reaction, resulting in the construction of a space charge zone on W surface. Based on these characteristics of D-WS2 -C, the prepared WS2 /C composite microspheres show superior fast-charging capability with a high capacity of 647.8 mAh g-1 at 20 C in half cells. For full cells, a high-energy density of 100.9 Wh kg-1 is achieved at a charge time of only 8.5 min at 5 C, representing the best fast-charging performances in WS2 -based anode materials to date.

Effect of Distance on Photoluminescence Quenching and Proximity-Induced Spin-Orbit Coupling in Graphene/WSe2 Heterostructures.

Spin-orbit coupling (SOC) in graphene can be greatly enhanced by proximity coupling it to transition metal dichalcogenides (TMDs) such as WSe2. We find that the strength of the acquired SOC in graphene depends on the stacking order of the heterostructures when using hexagonal boron nitride ( h-BN) as the capping layer, i.e., SiO2/graphene/WSe2/ h-BN exhibiting stronger SOC than SiO2/WSe2/graphene/ h-BN. We utilize photoluminescence (PL) as an indicator to characterize the interaction between graphene and monolayer WSe2 grown by chemical vapor deposition. We observe much stronger PL quenching in the SiO2/graphene/WSe2/ h-BN stack than in the SiO2/WSe2/graphene/ h-BN stack and, correspondingly, a much larger weak antilocalization (WAL) effect or stronger induced SOC in the former than in the latter. We attribute these two effects to the interlayer distance between graphene and WSe2, which depends on whether graphene is in immediate contact with h-BN. Our observations and hypothesis are further supported by first-principles calculations, which reveal a clear difference in the interlayer distance between graphene and WSe2 in these two stacks.

Hybrid bilayered vanadium oxide electrodes with large and tunable interlayer distances in lithium-ion batteries.

The interlayer distances in layered electrode materials, influenced by the chemical composition of the confined interlayer regions, have a significant impact on their electrochemical performance. Chemical preintercalation of inorganic metal ions affects the interlayer spacing, yet expansion is limited by the hydrated ion radii. Herein, we demonstrate that using varying concentrations of decyltrimethylammonium (DTA+) and cetyltrimethylammonium (CTA+) cations in chemical preintercalation synthesis followed by hydrothermal treatment, the interlayer distance of hybrid bilayered vanadium oxides (BVOs) can be tuned between 11.1 Å and 35.6 Å. Our analyses reveal that these variations in interlayer spacing are due to different amounts of structural water and alkylammonium cations confined within the interlayer regions. Increased concentrations of alkylammonium cations not only expand the interlayer spacing but also induce local bending and disordering of the V-O bilayers. Electrochemical cycling of hybrid BVO electrodes in non-aqueous lithium-ion cells show that specific capacities decrease as interlayer regions expand, suggesting that the densely packed alkylammonium cations obstruct intercalation sites and hinder Li+ ion transport. Furthermore, we found that greater layer separation facilitates the dissolution of active material into the electrolyte, resulting in rapid capacity decay during extended cycling. This study emphasizes that layered electrode materials require both spacious interlayer regions as well as high structural and chemical stabilities, providing guidelines for structural engineering of organic-inorganic hybrids.

Altering the Alkaline Metal Ions in Lepidocrocite-Type Layered Titanate for Sodium-Ion Batteries.

The relatively large ionic radius of the Na ion is one of the primary reasons for the slow diffusion of Na ions compared to that of Li ions in de/intercalation processes in sodium-ion batteries (SIBs). Interlayer expansion of intercalation hosts is one of the effective techniques for facilitating Na-ion diffusion. For most ionic layered compounds, interlayer expansion relies on intercalation of guest ions. It is important to investigate the role of these ions for material development of SIBs. In this study, alkali-metal ions (Li+, Na+, K+, and Cs+) with different sizes were intercalated into lepidocrocite-type layered titanate by a simple ion-exchange technique to achieve interlayer modulation and those were then evaluated as anode materials for SIBs. By controlling the intercalated alkaline ion species, basal spacings of layered titanates (LTs) in the range of 0.68 to 0.85 nm were obtained. Interestingly, the largest interlayer spacing induced by the large size of Cs did not yield the best performance, while the Na intercalated layered titanate (Na-ILT) demonstrated a superior performance with a specific capacity of 153 mAh g-1 at a current density of 0.1 A g-1. We found that the phenomena can be explained by the high alkaline metal ion concentration and the efficient utilization of the active sites in Na-ILT. The detailed analysis indicates that large intercalating ions like Cs can hamper sodium-ion diffusion although the interlayer spacing is large. Our work suggests that adopting an appropriate interlayer ion species is key to developing highly efficient layered electrode materials for SIBs.

Novel Polymer/Barium Intercalated Vanadium Pentoxide with Expanded Interlayer Spacing as High-Rate and Durable Cathode for Aqueous Zinc-Ion Batteries.

Rechargeable aqueous zinc-ion batteries (AZIBs) exhibit great potential in large-scale energy storage systems. However, limited reaction kinetics and poor long-cycle stability restrict the application of vanadium oxide cathode materials. Herein, we designed and successfully synthesized a novel composite material with polyethylene glycol (PEG) and barium cation (Ba2+) preintercalated between the layers of vanadium pentoxide, denoted as PEG-Ba0.38V2O5·nH2O (PEG-BVO), as a cathode material of AZIBs. The optimized PEG-BVO material shows a uniform nanobelt-like structure with the expanded interlayer spacing of 1.07 nm, significantly promoting the transport kinetics of zinc ions. The theoretical calculation results unravel that an interlayer spacing of 1.07 nm may be at the most stable state for this layered composite structure, ensuring a robust architecture for rapid reversible (de)intercalation of zinc ions. As a result, the PEG-BVO electrode (with a large mass loading of 4 mg cm-2) exhibits an outstanding electrochemical performance including a high specific capacity (345 mAh g-1 at 0.1 A g-1), decent rate capability (up to 175 mAh g-1 at 10 A g-1), and long-term cycling stability (98.8% capacity retention upon 4000 cycles at 6 A g-1). Our discovery provides a new guest preinsertion strategy to construct a robust layered vanadium-based electrode with the expanded interlayer spacing, and the as-prepared PEG-Ba0.38V2O5·nH2O shows great potential as a high-rate positive electrode for AZIBs.

Tunable Graphene Oxide Nanofiltration Membrane for Effective Dye/Salt Separation and Desalination.

Effective dye separation and desalination are critical for the treatment of highly saline textile wastewater with dye mixtures. In this study, a graphene oxide (GO) membrane with a tunable interlayer distance (d) was fabricated to generate clean water via two-stage filtration, namely, the dye/salt separation and desalination stages. In the first stage, under low pressure (e.g., 0.3 MPa), the membrane with a d value of ca. 7.60 Å was suitable for removing the dye from the saline wastewater. The dye and salt (i.e., Na2SO4) rejection rates of >99% and <6.5% were achieved, respectively, indicating the significant potential to recycle the dyes from the highly saline dye wastewater. In the second stage, under a higher pressure (e.g., 0.8 MPa), the d value was reduced to ca. 7.15 Å, bestowing the membrane with a desalination function. The desalination rate of a single filtration process could reach up to 51.8% from 1.0 g/L saline (i.e., Na2SO4) water. The as-prepared membrane also exhibited excellent practical advantages, including ultrahigh permeability, significant antifouling (against dye) performance, and excellent stability. Furthermore, with the stacking of multistage filtration systems, the proposed membrane technology will be capable of regenerating dye and producing clean water.

A Series of Molecule-Intercalated MoS2 as Anode Materials for Sodium Ion Batteries.

Molybdenum disulfide (MoS2) with a graphite-like layer structure has attracted substantial interest as an anode material for sodium ion batteries (SIBs), but its inherent poor electrical conductivity and slow sodium ion transportation are the two important factors that limit its use in SIBs. Here, we report a general approach to synthesize a series of molecule-intercalated MoS2 with a precisely controlled interlayer distance of 0.62 to 1.24 nm in which the electrical conductivity could be also widely and finely adjusted from 1.3 × 10-4 to 3.5 × 10-2 S cm-1 via the insertion of different molecules. By adjusting the interlayer space and enhancing the electrical conductivity, the highest initial sodium ion storage capacity of 465 mA h g-1 (vs 195 mA h g-1 for the pure MoS2 anode) and the highest capacity of 420 mA h g-1 (vs 31 mA h g-1 for the pure MoS2 anode) after 600 cycles at a rate of 100 mA g-1 were obtained. The excellent performance is credited to the rapid Na+ and electron transport and higher material utilization derived from the synergistic effect of the expanded interlayer space and the higher electronic conductivity. The results provide some inspiration for the design and construction of superior layered anode materials for sodium-ion batteries.

Tunable Molybdenum Disulfide-Enabled Fiber Mats for High-Efficiency Removal of Mercury from Water.

The application of molybdenum disulfide (MoS2) for water decontamination is expanded toward a novel approach for mercury removal using nanofibrous mats coated with MoS2. A bottom-up synthesis method for growing MoS2 on carbon nanofibers was employed to maximize the nanocomposite decontamination potential while minimizing the release of the nanomaterial to treated water. First, a co-polymer of polyacrylonitrile and polystyrene was electrospun as nanofibrous mats and pretreated to form pristine carbon fibers. Next, three solvothermal methods of controlled in situ MoS2 growth of different morphologies were achieved on the surface of the fibers using three different sets of precursors. Finally, these MoS2-enabled fibers were extensively characterized and evaluated for their mercuric removal efficiency. Two mercury removal mechanisms, including reduction-oxidation reactions and physicochemical adsorption, were elucidated. The two nanocomposites with the fastest (0.436 min-1 mg-1) and highest mercury removal (6258.7 mg g-1) were then further optimized through intercalation with poly(vinylpyrrolidone), which increased the MoS2 interlayer distance from 0.68 nm to more than 0.90 nm. The final, optimal fabrication technique (evaluated according to mercuric capacity, kinetics, and nanocomposite stability) demonstrated five times higher adsorption than the second-best method and obtained 70% of the theoretical mercury adsorption capacity of MoS2. Overall, results from this study indicate an alternative, advanced material to increase the efficiency of aqueous mercury removal while also providing the basis for other novel environmental applications such as selective sensing, disinfection, and photocatalysis.

2D/2D h-BN/N-doped MoS2 Heterostructure Catalyst with Enhanced Peroxidase-like Performance for Visual Colorimetric Determination of H2 O2.

Recently, nanozymes have attracted extensive attention because of their advantages of combining nanomaterials with enzymes. Herein, hexagonal boron nitride (h-BN) and nitride-doped molybdenum disulfide (N-MoS2 ) nano-composites (h-BN/N-MoS2 ) were synthesized by facile and cost-effective liquid exfoliation with a solvothermal method in nontoxic ethanol solution. The results show that h-BN, as a co-catalyst, can not only dope into the lattice of MoS2 but also form a heterogeneous structure with MoS2 NSs. It expanded the layer spacing and specific surface area of MoS2 NSs, which was beneficial to the contact between the catalyst and the substrate, and resulted in a synergistic enhancement of the catalytic activity of hydrogen peroxide (H2 O2 ) with MoS2 . A colorimetric determination platform of h-BN/N-MoS2 -TMB-H2 O2 was constructed. It exhibited a wide linear range of 1-1000 µM with a low limit of detection (LOD) of 0.4 µM under optimal conditions, high sensitivity and stability, as well as good reliability (99.4-110.0%) in practice, making the measurement system more widely applicable.1. Introduction.

Preparation of Tubular Forest-like and Other Carbon Structures Using Distinct Carbon Sources and Catalyst Concentrations.

BACKGROUND: In this work, various carbon nanotubes (MWCNTs) were synthetized by the spray pyrolysis method. Resulting nanoforest-like and bamboo-like carbon nanotubes, as well as Yjunctions of carbon nanotubes, possess different shapes and morphology, depending on the kind of carbon source used and on the number of iron particles on the furnace tube surface, which derives from various concentrations of ferrocene catalyst. METHODS: We used the spray pyrolysis method, using different carbon sources (n-pentane, n-hexane, nheptane, and acrylonitrile) as precursors and two different concentrations of ferrocene as a catalyst. Reactions of hydrocarbon decomposition were carried out at 800oC. The solution (hydrocarbon and catalyst) was introduced with a syringe, with a flow of 1 mL/min and the synthesis time of 20 min. Argon was used as carrier gas (1000 L/min). Preheater and oven temperatures were selected 180°C and 800°C, respectively, for each carbon source. The solution passed into a quartz tube placed in an oven. RESULTS: According to the studies of carbon nanostructures, obtained from different precursors, it can be proposed that the structures synthesized from n-pentane, n-hexane and n-heptane are formed by the root growth method. The growth mechanism of MWCNTs was studied, confirming that the root growth formation of products takes place, whose parameters also depend on furnace temperature and gas flow rate. Dependence of interlayer distance (0.34-0.50 nm) in the formed MWCNTs on precursors and reaction conditions is also elucidated. The formation of carbon nanotubes does not merely depend on carbon precursors but also has strong correlations with such growth conditions as different catalyst concentrations, furnace temperature and gas flow rate. Such parameters as the amount of catalyst and synthesis time are also needed to be considered, since they are important to find minor values of these parameters in the synthesis of forest-like carbon nanotubes and other structures such as bamboo-like carbon nanotubes and Y-junctions in carbon nanotubes. CONCLUSION: As a result of the evaluation of interlayer distance in CNTs formed from different carbon sources, a standard value of interlayer distance normally for CNTs is 0.34 nm and for pentane A (0.5 wt.%), hexane B (1 wt.%), toluene A (0.5 wt.%) the range is from 0.33 to 0.35 nm. In case of pentane and acrylonitrile, under an increase of the catalyst concentration, an increase of the value of interlayer distance takes place from 0.35 and 0.4 to 0.4 and 0.5 nm, respectively, but for hexane, heptane and cyclohexane, an increase of the catalyst concentration maintains the same interlayer distance. This involves the use of lower quantities of raw materials and, therefore less cost for obtaining these materials.

Holographic reconstruction of the interlayer distance of bilayer two-dimensional crystal samples from their convergent beam electron diffraction patterns.

The convergent beam electron diffraction (CBED) patterns of twisted bilayer samples exhibit interference patterns in their CBED spots. Such interference patterns can be treated as off-axis holograms and the phase of the scattered waves, meaning the interlayer distance can be reconstructed. A detailed protocol of the reconstruction procedure is provided in this study. In addition, we derive an exact formula for reconstructing the interlayer distance from the recovered phase distribution, which takes into account the different chemical compositions of the individual monolayers. It is shown that one interference fringe in a CBED spot is sufficient to reconstruct the distance between the layers, which can be practical for imaging samples with a relatively small twist angle or when probing small sample regions. The quality of the reconstructed interlayer distance is studied as a function of the twist angle. At smaller twist angles, the reconstructed interlayer distance distribution is more precise and artefact free. At larger twist angles, artefacts due to the moiré structure appear in the reconstruction. A method for the reconstruction of the average interlayer distance is presented. As for resolution, the interlayer distance can be reconstructed by the holographic approach at an accuracy of ±0.5 Å, which is a few hundred times better than the intrinsic z-resolution of diffraction limited resolution, as expressed through the spread of the measured k-values. Moreover, we show that holographic CBED imaging can detect variations as small as 0.1 Å in the interlayer distance, though the quantitative reconstruction of such variations suffers from large errors.

Graphitic Carbon Nitride (g-C3 N4 )-Derived N-Rich Graphene with Tuneable Interlayer Distance as a High-Rate Anode for Sodium-Ion Batteries.

Heteroatom-doped carbon materials with expanded interlayer distance have been widely studied as anodes for sodium-ion batteries (SIBs). However, it remains unexplored to further enlarge the interlayer spacing and reveal the influence of heteroatom doping on carbon nanostructures for developing more efficient SIB anode materials. Here, a series of N-rich few-layer graphene (N-FLG) with tuneable interlayer distance ranging from 0.45 to 0.51 nm is successfully synthesized by annealing graphitic carbon nitride (g-C3 N4 ) under zinc catalysis and selected temperature (T = 700, 800, and 900 °C). More significantly, the correlation between N dopants and interlayer distance of resultant N-FLG-T highlights the effect of pyrrolic N on the enlargement of graphene interlayer spacing, due to its stronger electrostatic repulsion. As a consequence, N-FLG-800 achieves the optimal properties in terms of interlayer spacing, nitrogen configuration and electronic conductivity. When used as an anode for SIBs, N-FLG-800 shows remarkable Na+ storage performance with ultrahigh rate capability (56.6 mAh g-1 at 40 A g-1 ) and excellent long-term stability (211.3 mAh g-1 at 0.5 A g-1 after 2000 cycles), demonstrating the effectiveness of material design.

Engineering a High-Energy-Density and Long Lifespan Aqueous Zinc Battery via Ammonium Vanadium Bronze.

Aqueous rechargeable zinc batteries (ARZBs) are desirable for energy storage devices owing to their low cost and abundance of the Zn anode, but their further development is limited by a dearth of ideal cathode materials that can simultaneously possess high capacity and stability. Herein, we employ a layered structure of ammonium vanadium bronze (NH4)0.5V2O5 as the cathode material for ARZBs. The large interlayer distance supported by the NH4+ insertion not only facilitates the Zn2+-ion intercalation/deintercalation but also improves the electrochemical stability in ARZBs. As a result, the layered structural (NH4)0.5V2O5 cathode delivers a high capacity up to 418.4 mA h g-1 at a current density of 0.1 A g-1. A reversible capacity of 248.8 mA h g-1 is still retained after 2000 cycles and a capacity retention of 91.4% was maintained at 5 A g-1. Furthermore, in comparison with previously reported Zn-ion batteries, the Zn/(NH4)0.5V2O5 battery achieves a prominent high energy density of 418.4 W h kg-1 while delivering a high power density of 100 W kg-1. The results would enlighten and push the ammonium vanadium compounds to a brand new stage for the application of aqueous batteries.

Deciphering the Rules for Amino Acid Co-Assembly Based on Interlayer Distances.

Metabolite materials are extremely useful to obtain functional bioinspired assemblies with unique physical properties for various applications in the fields of material science, engineering, and medicine by self-assembly of the simplest biological building blocks. Supramolecular co-assembly has recently emerged as a promising extended approach to further expand the conformational space of metabolite assemblies in terms of structural and functional complexity. Yet, the design of synergistically co-assembled amino acids to produce tailor-made functional architectures is still challenging. Herein, we propose a design rule to predict the supramolecular co-assembly of naturally occurring amino acids based on their interlayer separation distances observed in single crystals. Using diverse experimental techniques, we demonstrate that amino acids with comparable interlayer separation strongly interact and co-assemble to produce structural composites distinctly different from their individual properties. However, such an interaction is hampered in a mixture of differentially layer-separated amino acids, which self-sort to generate individual characteristic structures. This study provides a different paradigm for the modular design of supramolecular assemblies based on amino acids with predictable properties.

Sandwich-like SnS2/Graphene/SnS2 with Expanded Interlayer Distance as High-Rate Lithium/Sodium-Ion Battery Anode Materials.

SnS2 materials have attracted broad attention in the field of electrochemical energy storage due to their layered structure with high specific capacity. However, the easy restacking property during charge/discharge cycling leads to electrode structure instability and a severe capacity decrease. In this paper, we report a simple one-step hydrothermal synthesis of SnS2/graphene/SnS2 (SnS2/rGO/SnS2) composite with ultrathin SnS2 nanosheets covalently decorated on both sides of reduced graphene oxide sheets via C-S bonds. Owing to the graphene sandwiched between two SnS2 sheets, the composite presents an enlarged interlayer spacing of ∼8.03 Šfor SnS2, which could facilitate the insertion/extraction of Li+/Na+ ions with rapid transport kinetics as well as inhibit the restacking of SnS2 nanosheets during the charge/discharge cycling. The density functional theory calculation reveals the most stable state of the moderate interlayer spacing for the sandwich-like composite. The diffusion coefficients of Li/Na ions from both molecular simulation and experimental observation also demonstrate that this state is the most suitable for fast ion transport. In addition, numerous ultratiny SnS2 nanoparticles anchored on the graphene sheets can generate dominant pseudocapacitive contribution to the composite especially at large current density, guaranteeing its excellent high-rate performance with 844 and 765 mAh g-1 for Li/Na-ion batteries even at 10 A g-1. No distinct morphology changes occur after 200 cycles, and the SnS2 nanoparticles still recover to a pristine phase without distinct agglomeration, demonstrating that this composite with high-rate capabilities and excellent cycle stability are promising candidates for lithium/sodium storage.

In Silico Design and Characterization of Graphene Oxide Membranes with Variable Water Content and Flake Oxygen Content.

Graphene oxide (GO) membranes offer exceptional promise for certain aqueous separation challenges, such as desalination. Central to unlocking this promise and optimizing performance for a given separation is the establishment of a detailed molecular-level understanding of how the membrane's composition affects its structural and transport properties. This understanding is currently lacking, in part due to the fact that, until recently, molecular models with a realistic distribution of oxygen functionalities and interlayer flake structure were unavailable. To understand the effect of composition on the properties of GO membranes, models with water contents and oxygen contents, varying between 0% and 40% by weight, were prepared in this work using classical molecular dynamics simulations. The change in membrane interlayer distance distribution, water connectivity, and water diffusivity with water and oxygen content was quantified. Interlayer distance distribution analysis showed that the swelling of GO membranes could be controlled by separately tuning both the flake oxygen content and the membrane water content. Water-molecule cluster analysis showed that a continuous and fully connected network of water nanopores is not formed until the water content reaches ∼20%. The diffusivity of water in the membrane was also found to strongly depend on both the water and the oxygen content. These insights help understand the structure and transport properties of GO membranes with sub-nanometer interlayer distances and could be exploited to enhance the performance of GO membranes for aqueous separation applications. More broadly, the high-throughput in silico approach adopted could be applied to other nanomaterials with intrinsic non-stoichiometry and structural heterogeneity.

2D Perovskites with Short Interlayer Distance for High-Performance Solar Cell Application.

2D perovskites have emerged as one of the most promising photovoltaic materials owing to their excellent stability compared with their 3D counterparts. However, in typical 2D perovskites, the highly conductive inorganic layers are isolated by large organic cations leading to quantum confinement and thus inferior electrical conductivity across layers. To address this issue, the large organic cations are replaced with small propane-1,3-diammonium (PDA) cations to reduce distance between the inorganic perovskite layers. As shown by optical characterizations, quantum confinement is no longer dominating in the PDA-based 2D perovskites. This leads to considerable enhancement of charge transport as confirmed with electrochemical impedance spectroscopy, time-resolved photoluminescence, and mobility measurements. The improved electric properties of the interlayer-engineered 2D perovskites yield a power conversion efficiency of 13.0%. Furthermore, environmental stabilities of the PDA-based 2D perovskites are improved. PDA-based 2D perovskite solar cells (PSCs) with encapsulation can retain over 90% of their efficiency upon storage for over 1000 h, and PSCs without encapsulation can maintain their initial efficiency at 70 °C for over 100 h, which exhibit promising stabilities. These results reveal excellent optoelectronic properties and intrinsic stabilities of the layered perovskites with reduced interlayer distance.