Enhancing P2/O3 Biphasic Cathode Performance for Sodium-Ion Batteries: A Metaheuristic Approach to Multi-Element Doping Design.

Sodium-ion batteries (SIBs) have emerged as a compelling alternative to lithium-ion batteries (LIBs), exhibiting comparable electrochemical performance while capitalizing on the abundant availability of sodium resources. In SIBs, P2/O3 biphasic cathodes, despite their high energy, require furthur improvements in stability to meet current energy demands. This study introduces a systematic methodology that leverages the meta-heuristically assisted NSGA-II algorithm to optimize multi-element doping in electrode materials, aiming to transcend conventional trial-and-error methods and enhance cathode capacity by the synergistic integration of P2 and O3 phases. A comprehensive phase analysis of the meta-heuristically designed cathode material Na0.76Ni0.20Mn0.42Fe0.30Mg0.04Ti0.015Zr0.025O2 (D-NFMO) is presented, showcasing its remarkable initial reversible capacity of 175.5 mAh g-1 and exceptional long-term cyclic stability in sodium cells. The investigation of structural composition and the stabilizing mechanisms is performed through the integration of multiple characterization techniques. Remarkably, the irreversible phase transition of P2→OP4 in D-NFMO is observed to be dramatically suppressed, leading to a substantial enhancement in cycling stability. The comparison with the pristine cathode (P-NFMO) offers profound insights into the long-term electrochemical stability of D-NFMO, highlighting its potential as a high-voltage cathode material utilizing abundant earth elements in SIBs. This study opens up new possibilities for future advancements in sodium-ion battery technology.

Silicon nanoparticles encapsulated in Si3N4/carbon sheaths as an anode material for lithium-ion batteries.

Novel composite materials comprising of silicon nanoparticles (SiNPs) encapsulated with thin layers of silicon nitride and reduced graphene oxide shells (Si@Si3N4@rGO) are prepared using a simple and scalable method. The composite exhibits significantly improved cycling stability and rate capability compared to bare SiNPs. The presence of inactiveαandßphases of Si3N4increases the mechanical endurance of SiNPs. Amorphous SiNx, which is possibly present with Si3N4, also contributes to high capacity and Li-ion migration. The rGO sheath enhances the electronic conduction and improves the rate capability. 15-Si@Si3N4@rGO, which is prepared by sintering SiNPs for 15 min at 1300 °C, spontaneous-coating GO on Si@Si3N4, and reducing GO to rGO, delivers the highest specific capacity of 1396 mAh g-1after 100 cycles at a current density of 0.5 A g-1. The improved electrochemical performance of 15-Si@Si3N4@rGO is attributed to the unique combination of positive effects by Si3N4and rGO shells, in which Si3N4mitigates the issue of large volume changes of Si during charge/discharge, and rGO provides efficient electron conduction pathways. Si@Si3N4@rGO composites are likely to have great potential for a high-performance anode in lithium-ion batteries.

Zinc Anodes Modified by One-Molecular-Thick Self-Assembled Monolayers for Simultaneous Suppression of Side-Reactions and Dendrite-Formation in Aqueous Zinc-Ion Batteries.

Repeated charge/discharge in aqueous zinc-ion batteries (ZIBs) commonly results in surface corrosion/passivation and dendrite formation on zinc anodes, which is a major challenge for the commercialization of zinc-based batteries. In this work, metallic Zn modified by self-assembled monolayers is described as a viable anode for ZIBs. ω-mercaptoundecanoic acid that is spontaneously adsorbed on Zn (MUDA/Zn) contributes to the simultaneous suppression of side reactions and dendrite formation in ZIBs. Though one-molecular-thick, densely packed alkyl chains prohibit H2 O and H+ from making direct contact with the underlying Zn, and surface carboxylate moieties (-COO- ) effectively repel anionic species (OH- ) in a solution, which renders a Zn anode inert against zincate formation within a wide range of pH. In contrast, the electrostatic attraction between surface-carboxylates and cations increases the concentration of Zn2+ on the surface of MUDA/Zn to facilitate Zn plating/stripping with less overpotentials. The high concentration of Zn2+ also results in an increased number of nucleation sites, which enhances the lateral growth of Zn with no formation of dendrites. As a result, MUDA/Zn shows excellent stability during prolonged Zn plating/stripping within a wide range of pH. The advantageous properties of MUDA/Zn are also retained in full-cells coupled with δ-MnO2 cathodes.

KCrS2 Cathode with Considerable Cyclability and High Rate Performance: The First K+ Stoichiometric Layered Compound for Potassium-Ion Batteries.

KCrS2 is presented as a stable and high-rate layered material that can be used as a cathode in potassium-ion batteries. As far as it is known, KCrS2 is the only layered material with stoichiometric amounts of K+ , which enables coupling with a graphite anode for full-cell construction. Cr(III)/Cr(IV) redox in KCrS2 is also unique, because LiCrS2 and NaCrS2 are known to experience S2- /S2 2- redox. O3-KCrS2 is first charged to P3-K0.39 CrS2 and subsequently discharged to O'3-K0.8 CrS2 , delivering an initial discharge capacity of 71 mAh g-1 . The following charge/discharge (C/D) shows excellent reversibility between O'3-K0.8 CrS2 and P3-K0.39 CrS2 , retaining ≈90% of the initial capacity during 1000 continuous cycles. The rate performance is also noteworthy. A C/D rate increase of 100-fold (0.05 to 5 C) reduces the reversible capacity only by 39% (71 to 43 mAh g-1 ). The excellent cyclic stability and high rate performance are ascribed to the soft sulfide framework, which can effectively buffer the stress caused by K+ deinsertion/insertion. During the transformation between P3-K0.39 CrS2 and O'3-K0.8 CrS2 , the material resides mostly in the P3 phase, which minimizes the abrupt dimension change and allows facile K+ diffusion through spacious prismatic sites. Structural analysis and density functional theory calculations firmly support this reasoning.

Determination of possible configurations for Li0.5CoO2 delithiated Li-ion battery cathodes via DFT calculations coupled with a multi-objective non-dominated sorting genetic algorithm (NSGA-III).

Here, we propose a new and logical approach to systematically treat the configurational diversity in density functional theory (DFT) calculations. To tackle this issue, we select Li0.5CoO2 as a representative example because it is one of the most extensively studied cathodes in Li-ion batteries (LIBs), and it has a huge number of disordered configurations. To delineate the configurations that will match well with the experimentally measured macro-functions of redox potential, band gap energy, and magnetic moment, we adopt a multi-objective, non-dominated sorting, genetic algorithm (NSGA-III) that enables the simultaneous optimization of these three objective functions. The decision variables include configuration of the Li/vacancy, initial input for the magnetic moment distribution reflecting Co3+/Co4+ distribution, and initial input for the lattice parameter and Hubbard U. We use NSGA-III to separate the configurations that exhibit awkward objective function values, which allows us to pinpoint a set of plausible configurations that match the experimentally estimated values of the objective functions. The results reveal a plausible configuration that is a mixture of various ordered/disordered configurations rather than a simple ordered structure.

Density functional theory calculations for the band gap and formation energy of Pr4-xCaxSi12O3+xN18-x; a highly disordered compound with low symmetry and a large cell size.

A novel oxynitride compound, Pr4-xCaxSi12O3+xN18-x, synthesized using a solid-state route has been characterized as a monoclinic structure in the C2 space group using Rietveld refinement on synchrotron powder X-ray diffraction data. The crystal structure of this compound was disordered due to the random distribution of Ca/Pr and N/O ions at various Wyckoff sites. A pragmatic approach for an ab initio calculation based on density function theory (DFT) for this disordered compound has been implemented to calculate an acceptable value of the band gap and formation energy. In general, for the DFT calculation of a disordered compound, a sufficiently large super cell and infinite variety of ensemble configurations is adopted to simulate the random distribution of ions; however, such an approach is time consuming and cost ineffective. Even a single unit cell model gave rise to 43 008 independent configurations as an input model for the DFT calculations. Since it was nearly impossible to calculate the formation energy and the band gap energy for all 43 008 configurations, an elitist non-dominated sorting genetic algorithm (NSGA-II) was employed to find the plausible configurations. In the NSGA-II, all 43 008 configurations were mathematically treated as genomes and the calculated band gap and the formation energy as the objective (fitness) function. Generalized gradient approximation (GGA) was first employed in the preliminary screening using NSGA-II, and thereafter a hybrid functional calculation (HSE06) was executed only for the most plausible GGA-relaxed configurations with lower formation and higher band gap energies. The final band gap energy (3.62 eV) obtained after averaging over the selected configurations, resembles closely the experimental band gap value (4.11 eV).

Nonradiative energy transfer between two different activator sites in La(4-x)Ca(x)Si12O(3+x)N(18-x):Eu2+.

Energy transfer, which affects the entire performance of luminescent material, has been generally treated as an averaged parameter by assuming the host material to be a homogeneous continuum. However, energy transfer should be investigated in association with the crystallographic local structure around an activator site. To accomplish this, we established an analytical model and derived comprehensive rate equations, elucidating the relationship between the local structure and energy transfer behavior of La(4-x)Ca(x)Si12O(3+x)N(18-x):Eu2+, which is a recently discovered luminescent material for use in light-emitting diodes. Using the rate-equation model with the assistance of particle swarm optimization, the full-scale decay curves of donors and acceptors located at different crystallographic sites was computed.

C-LFP-multi-walled carbon nanotubes composite cathode materials synthesized by solid-state reaction for lithium ion batteries.

Multi-walled carbon nanotubes (MWNT) was utilized as a conductive additive to enhance the capacity and rate capability of carbon coated LiFePO4 (C-LFP). Composites of C-LFP with MWNT (C-LFP-MWNT) were prepared by blending MWNT at different stages of C-LFP synthesis. The pre-blending (PrB) of MWNT (5, 10, 15 wt%) with LFP precursor (PrB-C-LFP-MWNT) before calcination in a reducing environment (5 vol% H2 in N2) at 750 degrees C, produced phase pure crystalline LFP with a reduction in particle size as increase in MWNT content. This was contrasted with post-blending (PoB) of MWNT with as-synthesized C-LFP (PoB-C-LFP-MWNT), which gave inferior electrochemical performances. The PrB-C-LFP-MWNT (10 wt%) composite showed better cycle stability, higher rate capability, and faster Li diffusion characteristics than PoB-C-LFP-MWNT.

Influence of W-doping on electrochemical performance of spinel LiMn2O4.

The structural and electrochemical properties of W-doped LiMn2O4 and LiAl0.025Mn1.975O4 have been investigated to determine the role of W. The cathodic materials were synthesized by sol-gel method, using citric acid as the chelating agent. The results revealed that the substitution of W affects the lattice dimension, the morphology, and the electrochemical performance. Substitution of Al induces an obvious decrease in the electrochemical capacity (but higher capacity retention) and in the case of W the decrease was drastic. As observed from XRD, only a fraction of W is included in the spinel structure. However, for the LiAl0.025W0.025Mn1.95O4, a compromised value is reached between the Al-doped and W-doped LiMn2O4 in terms of capacity and cyclic performance. The pristine spinel LiMn2O4 synthesized by this method shows a relatively superior electrochemical performance at high C-rate with excellent capacity retention.

Unprecedented Cyclability and Moisture Durability of NaCrO2 Sodium-Ion Battery Cathode via Simultaneous Al Doping and Cr2O3 Coating.

Although there are many cathode candidates for sodium-ion batteries (NIBs), NaCrO2 remains one of the most attractive materials due to its reasonable level of capacity, nearly flat reversible voltages, and high thermal stability. However, the cyclic stability of NaCrO2 needs to be further improved in order to compete with other state-of-the-art NIB cathodes. In this study, we show that Cr2O3-coated and Al-doped NaCrO2, which is synthesized through a simple one-pot synthesis, can achieve unprecedented cyclic stability. We confirm the preferential formation of a Cr2O3 shell and a Na(Cr1-2xAl2x)O2 core, rather than xAl2O3/NaCrO2 or Na1/1+2x(Cr1/1+2xAl2x/1+2x)O2, through spectroscopic and microscopic methods. The core/shell compounds exhibit superior electrochemical properties compared to either Cr2O3-coated NaCrO2 without Al dopants or Al-doped NaCrO2 without shells because of their synergistic contributions. As a result, Na(Cr0.98Al0.02)O2 with a thin Cr2O3 layer (5 nm) shows no capacity fading during 1000 charge/discharge cycles while maintaining the rate capability of pristine NaCrO2. In addition, the compound is inert against humid air and water. We also discuss the reasons for the excellent performance of Cr2O3-coated Na(Cr1-2xAl2x)O2.

TiO2-grafted multi-walled carbon nanotubes for dye-sensitized solar cells.

Dye-Sensitized Solar Cells (DSSCs) comprised of TiO2 porous films with multi-walled carbon nanotubes (MWNT) were prepared at low temperature (150 degrees C). MWNT were incorporated to facilitate the fast electron transport resulting from metallic properties of carbon nanotubes. In order to enhance the effect of MWNT incorporation, TiO2-grafted MWNT (TiO2-MWNT) was synthesized which can increase the electron transport rate further due to proximity of TiO2 to MWNT The presence of TiO2 nanoparticles on the surface of MWNT was confirmed by electron microscopy and energy dispersive X-ray spectroscopy. As in the DSSCs prepared through high temperature sintering of photoanodes, the maximum content of MWNT incorporated into TiO2 was limited to 0.01 wt% relative to TiO2. TiO2 photoanodes including TiO2-grafted MWNT (TiO2-MWNT/P25) enhanced the cell efficiencies by ca. 28% and 14%, relative to TiO2 photoanodes without and with MWNT respectively, reaching the efficiency of 5.0%. Electrochemical impedance spectroscopy (EIS) was utilized to examine the effect of incorporation of TiO2 nanoparticles grafted to MWNT on the cell performance.

Unravelling the Nature of the Intrinsic Complex Structure of Binary-Phase Na-Layered Oxides.

The layered sodium transition metal oxide, NaTMO2 (TM = transition metal), with a binary or ternary phases has displayed outstanding electrochemical performance as a new class of strategy cathode materials for sodium-ion batteries (SIBs). Herein, an in-depth phase analysis of developed Na1-x TMO2 cathode materials, Na0.76 Ni0.20 Fe0.40 Mn0.40 O2 with P2- and O3-type phases (NFMO-P2/O3) is offered. Structural visualization on an atomic scale is also provided and the following findings are unveiled: i) the existence of a mixed-phase intergrowth layer distribution and unequal distribution of P2 and O3 phases along two different crystal plane indices and ii) a complete reversible charge/discharge process for the initial two cycles that displays a simple phase transformation, which is unprecedented. Moreover, first-principles calculations support the evidence of the formation of a binary NFMO-P2/O3 compound, over the proposed hypothetical monophasic structures (O3, P3, O'3, and P2 phases). As a result, the synergetic effect of the simultaneous existence of P- and O-type phases with their unique structures allows an extraordinary level of capacity retention in a wide range of voltage (1.5-4.5 V). It is believed that the insightful understanding of the proposed materials can introduce new perspectives for the development of high-voltage cathode materials for SIBs.

Optimal Composition of Li Argyrodite with Harmonious Conductivity and Chemical/Electrochemical Stability: Fine-Tuned Via Tandem Particle Swarm Optimization.

A tandem (two-step) particle swarm optimization (PSO) algorithm is implemented in the argyrodite-based multidimensional composition space for the discovery of an optimal argyrodite composition, i.e., with the highest ionic conductivity (7.78 mS cm-1 ). To enhance the industrial adaptability, an elaborate pellet preparation procedure is not used. The optimal composition (Li5.5 PS4.5 Cl0.89 Br0.61 ) is fine-tuned to enhance its practical viability by incorporating oxygen in a stepwise manner. The final composition (Li5.5 PS4.23 O0.27 Cl0.89 Br0.61 ), which exhibits an ionic conductivity (σion ) of 6.70 mS cm-1 and an activation barrier of 0.27 eV, is further characterized by analyzing both its moisture and electrochemical stability. Relative to the other compositions, the exposure of Li5.5 PS4.23 O0.27 Cl0.89 Br0.61 to a humid atmosphere results in the least amount of H2 S released and a negligible change in structure. The improvement in the interfacial stability between the Li(Ni0.9 Co0.05 Mn0.05 )O2 cathode and Li5.5 PS4.23 O0.27 Cl0.89 Br0.61 also results in greater specific capacity during fast charge/discharge. The structural and chemical features of Li5.5 PS4.5 Cl0.89 Br0.61 and Li5.5 PS4.23 O0.27 Cl0.89 Br0.61 argyrodites are characterized using synchrotron X-ray diffraction, Raman spectroscopy, and X-ray photoelectron spectroscopy. This work presents a novel argyrodite composition with favorably balanced properties while providing broad insights into material discovery methodologies with applications for battery development.

Ca2+-Based Dual-Carbon Batteries in Ternary Ionic Liquid Electrolytes.

Herein, we propose Ca2+-based dual-carbon batteries (DCBs) that undergo a simultaneous occurrence of reversible accommodations of Ca2+ in a graphite anode (mesocarbon microbeads) and of bis(trifluoromethanesulfonyl)imide (TFSI-) in a graphite cathode (KS6L). For this purpose, we precisely tune electrolytes composed of Ca2+ complexed with a single tetraglyme molecule ([Ca:G4]) in N-butyl-N-methylpyrrolidinium TFSI (Pyr14TFSI) ionic liquid (IL). This ternary electrolyte is required for the enhancement of anodic stability that is needed to accomplish maximal TFSI- intercalation into KS6L at a high potential. A solution of 0.5 M [Ca:G4] in IL ([Ca:G4]/IL) is found to be optimal for DCBs. First, the electrochemical properties and the structural evolution of each graphite in a half-cell configuration are described to demonstrate excellent electrochemical performance. Second, the negligible intercalation of Pyr14+ into an MCMB anode is ascertained in 0.5 M [Ca:G4]/IL. Finally, DCBs are constructed by coupling two electrodes to show high capacity (54.0 mA h g-1 at 200 mA g-1) and reasonable cyclability (capacity fading of 0.022 mA h g-1 cycle-1 at 200 mA g-1 during 300 charge/discharge cycles). This work is the first to examine DCBs based on Ca2+ intercalation and helps pave the way for the development of a new type of next-generation batteries.

Aliovalent-doped sodium chromium oxide (Na0.9Cr0.9Sn0.1O2 and Na0.8Cr0.9Sb0.1O2) for sodium-ion battery cathodes with high-voltage characteristics.

NaCrO2 with high rate-capability is an attractive cathode material for sodium-ion batteries (NIBs). However, the amount of reversibly extractable Na+ ions is restricted by half, which results in relatively low energy density for practical NIB cathodes. Herein, we describe aliovalent-doped O3-Na0.9[Cr0.9Sn0.1]O2 (NCSnO) and O3-Na0.8[Cr0.9Sb0.1]O2 (NCSbO), both of which show high-voltage characteristics that translate to an increase in energy density. In contrast to NaCrO2, NCSnO and NCSbO can be reversibly charged to 3.80 and 3.95 V, respectively, delivering 0.5 Na+ along with Cr3+/4+ redox alone. The reversible chargeability to Na0.4[Cr0.9Sn0.1]O2 and Na0.3[Cr0.9Sb0.1]O2 is not associated with the suppression of Cr6+ formation. Both compounds show concentrations of Cr6+ that are higher than that of Na0.3CrO2, with an absence of O3' phases. This implies that aliovalent-doping contributes to a suppression of the Cr6+ migration into tetrahedral sites in the interslab space, which reduces the possibility of irreversible comproportionation. NCSnO and NCSbO deliver capacities comparable to that of NaCrO2, but show a higher average discharge voltage (2.94 V for NaCrO2; 3.14 V for NCSnO; 3.21 V for NCSbO), which leads to a noticeable increase in energy densities. The high-voltage characteristics of NCSnO and NCSbO are also validated via density-functional-theory calculations.

Graphite as a Long-Life Ca2+-Intercalation Anode and its Implementation for Rocking-Chair Type Calcium-Ion Batteries.

Herein, graphite is proposed as a reliable Ca2+-intercalation anode in tetraglyme (G4). When charged (reduced), graphite accommodates solvated Ca2+-ions (Ca-G4) and delivers a reversible capacity of 62 mAh g-1 that signifies the formation of a ternary intercalation compound, Ca-G4·C72. Mass/volume changes during Ca-G4 intercalation and the evolution of in operando X-ray diffraction studies both suggest that Ca-G4 intercalation results in the formation of an intermediate phase between stage-III and stage-II with a gallery height of 11.41 Å. Density functional theory calculations also reveal that the most stable conformation of Ca-G4 has a planar structure with Ca2+ surrounded by G4, which eventually forms a double stack that aligns with graphene layers after intercalation. Despite large dimensional changes during charge/discharge (C/D), both rate performance and cyclic stability are excellent. Graphite retains a substantial capacity at high C/D rates (e.g., 47 mAh g-1 at 1.0 A g-1 s vs 62 mAh g-1 at 0.05 A g-1) and shows no capacity decay during as many as 2000 C/D cycles. As the first Ca2+-shuttling calcium-ion batteries with a graphite anode, a full-cell is constructed by coupling with an organic cathode and its electrochemical performance is presented.

Simultaneous Suppression of Metal Corrosion and Electrolyte Decomposition by Graphene Oxide Protective Coating in Magnesium-Ion Batteries: Toward a 4-V-Wide Potential Window.

Despite remarkable developments in electrolyte systems over the past 2 decades, magnesium-ion batteries still suffer from corrosion susceptibility and low anodic limits. Herein we describe how graphene oxide (GO), coated onto non-noble metals (Al, Cu, and stainless steel) via electrophoretic deposition, can solve this problem. In all phenyl complex electrolytes, GO coating results in a significant suppression of corrosion and extends the anodic limits (up to 4.0 V vs Mg/Mg2+) with no impact on reversible Mg plating/stripping reactions. The same effect of GO coating is also established in magnesium aluminum chloride complex electrolytes. This remarkable improvement is associated with the electrostatic interaction between the ionic charges of electrolytes and the surface-functional groups of GO. In addition, GO coating does not aggravate the cathode performance of Mo6S8, which allows the use of non-noble metals as current collectors. We also discuss the role of GO in increasing anodic limits when it is hybridized with α-MnO2.

Classification of crystal structure using a convolutional neural network.

A deep machine-learning technique based on a convolutional neural network (CNN) is introduced. It has been used for the classification of powder X-ray diffraction (XRD) patterns in terms of crystal system, extinction group and space group. About 150 000 powder XRD patterns were collected and used as input for the CNN with no handcrafted engineering involved, and thereby an appropriate CNN architecture was obtained that allowed determination of the crystal system, extinction group and space group. In sharp contrast with the traditional use of powder XRD pattern analysis, the CNN never treats powder XRD patterns as a deconvoluted and discrete peak position or as intensity data, but instead the XRD patterns are regarded as nothing but a pattern similar to a picture. The CNN interprets features that humans cannot recognize in a powder XRD pattern. As a result, accuracy levels of 81.14, 83.83 and 94.99% were achieved for the space-group, extinction-group and crystal-system classifications, respectively. The well trained CNN was then used for symmetry identification of unknown novel inorganic compounds.

Systematic Approach To Calculate the Band Gap Energy of a Disordered Compound with a Low Symmetry and Large Cell Size via Density Functional Theory.

An ab initio calculation based on density functional theory (DFT) was used to verify the disordered structure of a novel oxynitride phosphor host, La4-x Ca x Si12O3+x N18-x , with a large unit cell (74 atoms), low level of symmetry (C2), and large band gap (4.45 eV). Several Wyckoff sites in the La4-x Ca x Si12O3+x N18-x structure were randomly shared by La/Ca and O/N ions. This type of structure is referred to as either partially occupied or disordered. The adoption of a supercell that is sufficiently large along with an infinite variety of ensemble configurations to simulate such a random distribution in a partially occupied structure would be an option that could achieve a reliable DFT calculation, but this would increase the calculation expenses significantly. We chose 5184 independent unit cell configurations to be used as input model structures for DFT calculations, which is a reduction from a possible total of 20 736 unit cell configurations for C2 symmetry. Instead of calculating the total energy as well as the band gap energy for all 5184 configurations, we pinpointed configurations that would exhibit a band gap that approximated the actual value by employing an elitist nondominated sorting genetic algorithm (NSGA-II) wherein the 5184 configurations were represented mathematically as genomes and the calculated total and band gap energies were represented as objective (fitness) functions. This preliminary screening based on NSGA-II was completed using a generalized gradient approximation (GGA), and thereafter, we executed a hybrid functional calculation (HSE06) for only the most plausible GGA-relaxed configurations with higher band gap energies and lower total energies. Finally, we averaged the HSE06 band gap energy over these selected configurations using the Boltzmann energy distribution and achieved a realistic band gap energy that more closely approximated the experimental measurement.

SnO2/graphene composites with self-assembled alternating oxide and amine layers for high Li-storage and excellent stability.

An alternating stack (SG/GN) consisting of SnO2-functionalized graphene oxide (SG) and amine-functionalized GO (GN) is prepared in solution. The thermally reduced SG/GN (r(SG/GN)) with decreased micro-mesopores and completely eliminated macropores, results in a high reversible capacity and excellent capacity retention (872 mA h g⁻¹ after 200 cycles at 100 mA g⁻¹) when compared to a composite without GN.