Density Functional Theory Study of Bilayer Borophene-Based Anode Material for Rechargeable Lithium Ion Batteries

The development of universal anode materials with superlative electrochemical performance poses a great challenge for rechargeable alkali metal (AM) ion battery technologies. In the present work, the viability of the gapless Dirac t-BN (tetragonal boron nitride) monolayer as a lightweight binder-free anode has been systematically evaluated via comprehensive first-principles calculations. Aside from the desirable electronic conductivity, the t-BN monolayer exhibits an excellent ionic conductivity as well due to its moderate affinity for Li, Na, and K atoms with favorable inplane barriers of 0.36, 0.18, and 0.19 eV, respectively. Meanwhile, the presence of B 4 N 4 octagons allows the AM atoms to penetrate through the t-BN monolayer. Excitingly, the host material delivers an ultrahigh specific capacity up to 1080 mA h g −1 for Li, 5400 mA h g −1 for Na, and 2160 mA h g −1 for K in the wake of low mean open-circuit voltages of 0.033, 0.203, and 0.300 V at the half-cell level. According to the standard hydrogen electrode methodology, the energy densities are forecasted to be as large as 3240, 13500, and 5680 mW h g −1 for Li, Na, and K ion batteries, respectively, with robust thermal stability up to at least 400 K. The safety and cycling durability of the t-BN monolayer are jointly corroborated via the moderate mechanical strengths and ab initio molecular dynamics simulations at the maximum intercalated states, as well as via the small lattice changes and its ultrahigh tolerable ultimate tensile strain. These findings unambiguously promise that the t-BN monolayer can serve as an appealing candidate for anode applications in AM ion batteries.

Section: Introductionmentioning

confidence: 99%

Dirac t-Boron Nitride Monolayer as an Appealing Binder-Free Anode for Alkali Metal Ion Batteries

Liu,

Zhang,

Wang

2024

“…The existing lithium-ion batteries have a specific energy limit of approximately 300 Wh kg –1 per cell, , which falls short of meeting the demands for long standby time in electronic devices and long driving range in electric vehicles. , Therefore, there is an urgent need to develop the next-generation high-energy batteries beyond Li-ion technologies. , Against this background, lithium–sulfur batteries have shown a theoretical specific energy of up to 2600 Wh kg –1 and a theoretical specific capacity of 1675 mAh g –1 , indicating great potential for various applications. , However, the practical use of lithium–sulfur batteries faces some key scientific challenges, primarily including the “shuttle effect” of polysulfides at the cathode , and lithium dendrite growth/electrode pulverization at the anode . The essence of the shuttling problem lies in the irreversible reactions occurring between polysulfides shuttling to the lithium metal electrode, , resulting in irreversible losses of sulfur series species and self-discharge.…”

Section: Introductionmentioning

confidence: 99%

High-Energy SiO-Sulfur Battery with Preloaded Li₃N in a Cathode as a Lithiation Reagent

Wang,

Zhang

et al. 2024

The practical use of lithium−sulfur batteries faces the "shuttle effect" and lithium dendrite growth. Employing SiO instead of Li metal can fundamentally solve the above problems. Nevertheless, selecting a convenient prelithiation method is essential for normal operation of the battery system. Hence, this work proposed a novel SiO-sulfur battery with preloaded Li 3 N in a cathode as a prelithiation reagent, which can thoroughly solve the dendrite problem and the side reaction with polysulfides of lithium anode. The S@KB-Li 3 N vs SiO full cell can obtain a high specific capacity of 790 mAh g −1 after the activation process and be maintained at 478 mAh g −1 after 100 cycles. Our design will provide a new prelithiation strategy for a high-specific-energy SiO-sulfur battery system.

“…Borophene, a novel 2D material with rich polymorphism and anisotropic metallic behavior, holds great promise for energy storage of ion batteries, − lithium–sulfur batteries, − and energy conversion of electrochemical catalysis, − and the performance is comparable to other common 2D materials. , The successful synthesis of monolayer borophene and the identification of atomic structures in experiments are inseparable from the above characterization methods. ,, After that, boron sheets beyond monolayer with higher stability and superior antioxidation are predicted in theory, which can be attributed to the formation of pillars and strong coupling strength between interlayers. − In addition, 3D-boron clusters intercalated into layered hydroxides could be utilized in superacid storage and dynamical disordering in MgB 2 materials in hydrogen storage performance . It is worth noting that recent experiments successfully fabricated quasi-freestanding bilayer borophene on Ag(111) and Cu(111) surfaces, and the metallicity is preserved. , In addition, the vibrational modes of bilayer borophene on the Ag(111) substrate found coupling interactions between boron sheets and substrate in visible and IR regions, and the strongest vibration occurred at the interlayer chemical bonds of boron atoms, further proposing the huge potential in optoelectronic devices.…”

Section: Introductionmentioning

confidence: 99%

Structural Characterization of Boron Sheets beyond the Monolayer and Implication for Experimental Synthesis and Identification

Ye,

Xiao,

Fan

et al. 2023

Self Cite

The successful synthesis of quasi-freestanding bilayer borophene has aroused much attention for its superior physical properties and holds great promise for future electronic devices. Herein, we comprehensively explore six boron sheets beyond the monolayer and structurally characterize them via various methods using first-principles calculations for experimental references. On the basis of atomic models of borophenes, simulated scanning tunneling microscope (STM) images show different morphologies at different bias voltages and are explained by the partial densities of states and the height differences in the vertical direction. Simulated transmission electron microscope images further probe the internal atomic arrangement of boron sheets and compensate for the shortcomings of STM images to better distinguish different phases of boron sheets. The interlayer coupling strength is stronger in bilayer borophenes than in the three-layer system via the electron localization function and Mulliken bond population. In addition, simulated X-ray diffraction and infrared spectra show different characteristic peaks and corresponding vibrational modes to further characterize these boron sheets. These theoretical results can decrease the prime cost and provide vital guidance for the experimental synthesis and identification of boron sheets beyond the monolayer.