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Carbonaceous materials are promising candidates as anode materials for non-lithium-ion batteries (NLIBs) due to their appealing properties such as good electrical conductivity, low cost, and high safety. However, graphene, a classic two-dimensional (2D) carbon material, is chemically inert to most metal atoms, hindering its application as an electrode material for metal-ion batteries. Inspired by the unique geometry of a four-penta unit, we explore a metallic 2D carbon allotrope C 5-10-16 composed of 5-10-16 carbon rings. The C 5-10-16 monolayer is free from any imaginary frequencies in the whole Brillouin zone. Due to the introduction of a non-sp 2 hybridization state into C 5-10-16 , the extended conjugation of π-electrons is disrupted, leading to the enhanced surface activity toward metal ions. We investigate the performance of C 5-10-16 as the anode for sodium/potassium-ion batteries by using first-principles calculations. The C 5-10-16 sheet has high theoretical specific capacities of Na (850.84 mA h g -1 ) and K (743.87 mA h g -1 ). Besides, C 5-10-16 exhibits a moderate migration barrier of 0.63 (0.32) eV for Na (K), ensuring rapid charging/discharging processes. The average open-circuit voltages of Na and K are 0.33 and 0.62 V, respectively, which are within the voltage acceptance range of anode materials. The fully sodiated (potassiated) C 5-10-16 shows tiny lattice expansions of 1.4% (1.3%), suggesting the good reversibility. Moreover, bilayer C 5-10-16 significantly affects both the adsorption strength and the mobility of Na or K. All these results show that C 5-10-16 could be used as a promising anode material for NLIBs.

High-performance sodium-ion batteries (SIBs) require anode materials with high capacity and fast kinetics. Based on first-principles calculations, we propose BC 3 N 2 and BC 3 N 2 /graphene (B/G) heterostructure as potential SIB anode materials. The BC 3 N 2 monolayer exhibits intrinsic metallic behavior. In addition, BC 3 N 2 possesses a low Na + diffusion barrier (0.15 eV), a high storage capacity (777 mA h g -1 ), a low open-circuit voltage (0.72 V), and a tiny axial expansion (0.36%). Compared with the BC 3 N 2 monolayer, the B/G heterostructure exhibits a lower diffusion barrier of 0.027 eV, suggesting a much faster diffusion. More importantly, although the B/G heterostructure possesses heavier molar weight, its theoretical capacity (689 mA h g -1 ) is comparable to that of the BC 3 N 2 monolayer. Based on the above-mentioned properties, we hope both the BC 3 N 2 monolayer and the B/G heterostructure would be promising anodes for SIBs.

Multivalent-ion batteries have garnered significant attention due to their high energy density, low cost, and superior safety. Calcium-ion batteries (CIBs) are regarded as the next-generation energy storage systems for their abundant natural resources and bivalent characteristics. However, the absence of high-performance anode materials poses a significant obstacle to the progress of battery technology. Two-dimensional (2D) Dirac materials have excellent conductivity and abundant active sites, rendering them promising candidates as anode materials. A novel 2D Dirac material known as "graphene+" has been theoretically reported, exhibiting prominent properties including good stability, exceptional ductility, and remarkable electronic conductivity. By using first-principles calculations, we systematically investigate the performance of graphene+ as an anode material for CIBs. Graphene+ exhibits an ultra-high theoretical capacity (1487.7 mA h g -1 ), a small diffusion barrier (0.21 eV), and a low average open-circuit voltage (0.51 V). Furthermore, we investigate the impact of the electrolyte solvation on the performance of Ca-ion adsorption and migration. Upon contact with electrolyte solvents, graphene+ exhibits strong adsorption strength and rapid migration of Ca-ions on its surface. These results demonstrate the promising potential of graphene+ as a high-performance anode material for CIBs.

Sodium-ion batteries (SIBs) have attracted much attention due to their abundant earth-reserves and low cost. Two-dimensional (2D) Dirac materials show great application prospects as anodes for SIBs because of their excellent electronic conductivity. We explore the performances of AlB 4 (Al 2 B 2 ) monolayers and bilayers as anodes for SIBs by using first-principles calculations. The AlB 4 (Al 2 B 2 ) monolayer exhibits a high theoretical storage capacity of 954.15 (709.17) mA h g -1 and a low diffusion barrier of 0.36 (0.03) eV. The calculated average open-circuit voltage (0.68/0.18 V) falls within the acceptance range of 0.1-1.0 V for anode materials. The fully sodiated AlB 4 (Al 2 B 2 ) monolayer shows a tiny lattice expansion of 0.9% (2.4%), suggesting good reversibility. Furthermore, in comparison with the AlB 4 (Al 2 B 2 ) monolayer, the AlB 4 (Al 2 B 2 ) bilayer can provide stronger binding with Na on the outside surface. These results contribute to a better understanding of the AlB 4 (Al 2 B 2 ) monolayers and bilayers as potential high-performance anode materials for SIBs.

Lithium-ion batteries (LIBs) remain irreplaceable for clean energy storage applications. The intrinsic metallic nature of penta-SiCN ensures its promising application in the electrodes of LIBs. Using first-principles calculations, we evaluate the performance of the intrinsic metallic penta-SiCN monolayer as the anode material for LIBs. Penta-SiCN exhibits a low diffusion energy barrier (0.107 eV) for Li atom migration on Si 18 C 18 N 18 , while the diffusion energy barrier for vacancy migration on Li 17 Si 18 C 18 N 18 is only 0.006 eV. Additionally, penta-SiCN possesses a high theoretical capacity of 1485.98 mA h g -1 , average open-circuit voltage of 0.97 V, and small volume expansion of 1%. Remarkably, penta-SiCN exhibits robust wettability towards the electrolytes (solvent molecules and metal salts) widely used in commercial LIBs, indicating the excellent compatibility in electrode applications. These intriguing theoretical findings make penta-SiCN a high performance anode material for LIBs.

Two-dimensional (2D) carbon materials integrated with planar tetracoordinate carbon (ptC) and negative Poisson's ratio (NPR) provide a cornerstone for constructing multifunctional energy-storage devices. As a typical 2D carbon material, the pristine graphene is chemically inert, hindering its application in metal-ion batteries. Introducing the ptC in graphene can break the extended conjugation of π-electrons and lead to an enhanced surface reactivity. Inspired by the unique geometry of [4.6.4.6] fenestrane skeleton with ptC, we theoretically design a ptC-containing 2D carbon allotrope, namely THFS-carbon. It is intrinsically metallic with excellent dynamical, thermal, and mechanical stabilities. The Young's modulus along the x direction (311.37 N m -1 ) is comparable to that of graphene. Intriguingly, THFS-carbon possesses an in-plane half-NPR distinct from most other 2D crystals. As a promising anode for sodium-ion batteries, THFS-carbon delivers an ultra-high theoretical storage capacity (2233 mA h g -1 ), a low diffusion energy barrier (0.03-0.05 eV), a low open-circuit voltage (0.14-0.40 V), and a good reversibility for Na insertion/extraction.

Na-ion batteries (NIBs) have attracted a great deal of attention for large-scale electric energy storage due to their inherent safety, natural abundant resources, and low cost. The exploration of suitable anode materials is the major challenge in advancing NIB technology. On the basis of first-principles calculations, we systematically explore the potential performance of two-dimensional (2D) TiCl 2 as an electrode material for NIBs. Monolayer TiCl 2 can be easily exfoliated from the bulk structure with a small exfoliation energy of 0.64 J m -2 . It shows good stability, as demonstrated by its high cohesive energy, positive phonon modes, and high thermal stability. Monolayer TiCl 2 has high storage capacity (451.3 mA h g -1 ), low diffusion energy barrier (0.02-0.14 eV), moderate average open-circuit voltage (0.81 V), and small lattice change (2.37%). Moreover, bilayer TiCl 2 can significantly enhance the Na adsorption strength but reduce the Na-ion diffusion ability. These results suggest that TiCl 2 is a promising anode candidate for NIBs.

High specific capacity and fast charge/discharge rate are important indicators for the development of next-generation ion batteries. Compared with conventional monovalent ion batteries like lithium-ion batteries and sodium-ion batteries, multivalent ion batteries have attracted extensive attention owing to their high energy densities. Here, we systematically explore the interactions between Mg atoms and α-beryllene monolayers by means of density functional theory calculations. Mg atoms can be adsorbed stably on α-beryllene monolayers with the adsorption energy of -0.24 eV. The low diffusion energy barriers (0.099/0.101 eV) indicate the rapid mobility of Mg during the charge/discharge process. Moreover, the α-beryllene monolayer exhibits an ultra-high theoretical specific capacity of 5956 mA h g -1 for Mg, a low average open-circuit voltage of 0.24 V, and a tiny volume change of -1.08%. Finally, the constructed h-BN/α-beryllene heterostructure shows that h-BN can serve as a protective cover to preserve pristine α-beryllene in respect of metallicity, Mg adsorption capability, and fast ionic mobility. The above mentioned outstanding results make α-beryllene a promising anode material for magnesium-ion batteries.

Sodium-ion batteries (SIBs) have been attracting great attention as the most promising alternative to lithium-ion batteries (LIBs) for large-scale energy storage. However, the absence of suitable anode materials is the main bottleneck for the commercial application of SIBs. Herein, the adsorption and diffusion behaviors of Na on graphether are predicted by first-principles density functional calculations. Our results show that Na atoms can be adsorbed on graphether forming a uniform and stable coverage on both sides. Even at low intercalated Na concentrations, the semiconducting graphether can be changed to a metallic state, ensuring good electrical conductivity. Due to the structural anisotropy of graphether, the Na+ ions show a remarkable one-dimensional diffusion with an ultralow energy barrier of 0.04 eV, suggesting ultrafast charge/discharge characteristics. The graphether monolayer has a high theoretical specific capacity of 670 mA h g-1, which is much higher than commercial graphite anode materials. Furthermore, the average voltage is 1.58 V, comparable with that of commercial TiO2 anode materials for LIBs (1.5 V). During the charge/discharge process, graphether could mostly preserve the structural integrity upon the adsorption of Na even at the maximum concentration, suggesting its good reversibility. All these results show that graphether is a promising anode material for high-performance SIBs.

Searching for high-performance electrode materials is an important topic in rechargeable batteries. Using first-principles calculations, we systematically explore the potential application of a two-dimensional BP2 monolayer as a cathode material for Li-ion and Na-ion batteries. The pristine BP2 monolayer exhibits metallic characteristics, which facilitate the transportation of electrons. The Li and Na atoms bind strongly to the BP2 monolayer, indicating a good structural stability. Furthermore, the geometrical structure of BP2 is well maintained during the adsorption process. The Li and Na ions prefer to move along the zigzag direction with relatively low energy barriers. Especially, the ultralow Na diffusion barrier (0.03 eV) implies that monolayer BP2 has an excellent charge/discharge capability. The specific capacity and average electrode potential of Li (Na) are 619.45 (279.93) mA h g-1 and 2.89 (2.49) V, respectively. These results reveal that the BP2 monolayer is an appealing cathode material for alkali-metal batteries.

Two-dimensional (2D) ultra-wide bandgap (UWBG) semiconductors have attracted tremendous attention because of their unique electronic properties and promising applications. Using first-principles calculations, monolayer (bilayer) CaFCl has a cleavage energy of 0.93 J m-2 (0.72 J m-2), suggesting that the exfoliation of monolayer and few-layer materials from the bulk phase could be feasible. The CaFCl monolayer is an UWBG semiconductor with a direct bandgap of 6.62 eV. In addition to the dynamic and thermodynamic stability, it can remain thermally stable at 2200 K, suitable for operation in high-temperature environments. The bandgap of monolayer CaFCl can be tuned by external strain and layer thickness. The decrease of the layer thickness leads to not only a bandgap increase but also an indirect-to-direct bandgap transition, suggesting a strong interlayer quantum confinement effect. Under biaxial strain, the direct bandgap can also be turned into an indirect one. The adsorption of a tetrathiafulvalene (TTF) molecule introduces deep donor states in the gap of CaFCl. Under an external electric field with direction from CaFCl to TTF, the TTF-derived donor states move closer to the conduction band edge of CaFCl and then the adsorption complex becomes effectively n-doped. Furthermore, monolayer CaFCl exhibits pronounced optical absorption in the ultraviolet range of the solar spectrum. These results render CaFCl an attractive 2D material for applications in flexible nanoelectronic and optoelectronic devices.

A balance between the hydrogen capacity and reversibility is a big challenge in the search for hydrogen storage materials. Using van der Waals-corrected density functional theory, we perform a detailed study of the hydrogen molecules adsorption on lithium (Li) decorated zero- and two-dimensional boron-carbon (B-C) compounds. It is found that not only the Li bond strength but also the number of adsorbed hydrogen molecules depends on the B concentration. First, the binding of Li on the B-C compounds strengthens with the increase of the B concentration due to the stronger hybridization between the lowest unoccupied molecular orbitals of the B-C compounds and Li 2p orbitals. Thus, Li atoms are not likely to form clusters, indicating a good reversible hydrogen storage. Second, higher B concentration results in weaker electric field produced by the charge transfer from Li to the B-C compounds. Therefore, one Li atom can adsorb up to 5H(2) molecules with the B concentration less than 50%. In contrast, the adsorption number of H(2) molecules is reduced to 4 when the B concentration is greater than or equal to 50%. Third, using a statistical model parametrized by the results of ab initio calculations, the adsorption and desorption of molecular hydrogens are calculated at ambient temperature and pressure. We find that the usable number of adsorbed H(2) per Li under ambient conditions decreases with the increase of B concentration. These results can serve as a guide in the design of new hydrogen storage materials based on B-C compounds.