Two-Dimensional Biphenylene-Based Carbon Allotrope Family with High Potassium Storage Ability

Abstract

The development of new carbon materials with novel properties and excellent applications is essential and urgent in many fields, such as potassium-ion batteries (PIBs). In this study, a family of 30 two-dimensional biphenylene carbon allotropes (2D-BCAs) have been systematically extended in theory. The energies of these allotropes are slightly higher than that of graphene, which can be well described by a quantitative energy equation. The 2D-BCAs show high synthesizability consistent with the experimental biphenylene network via “HF-zipping” reactions. The 2D-BCAs are metallic or semimetallic. Six representative 2D-BCAs exhibit good lattice dynamical and thermal stability, excellent anisotropic mechanical properties, and ORR catalytic activity. Moreover, the selected 2D-BCAs demonstrate ultrahigh theoretical potassium-storage capacities of 1116–1489 mAh·g–1, low migration barriers of 0.03–0.22 eV, and low open-circuit voltages of 1.10–0.02 V. The remarkable properties render 2D-BCAs as promising anode materials in PIBs, electrocatalysts, and conductors in electronics and iontronics.

Unveiling a New 2D Semiconductor: Biphenylene-Based InN

“…The first one was recently obtained by surface polymer dehydrogenation (HF-zipping), while the second one was produced via polymerization reactions using the 1,3,5-trihydroxybenene precursor . Many reports, mainly based on density functional theory (DFT), have demonstrated that both monolayers are suitable for diverse applications, including catalysis, molecular membranes, water purification, gas sensing, − thermoelectricity, − optoelectronics, energy storage, − electronics, and catalysis. , …”

Biphenylite as Anode Materials for Alkali Metal Ion Batteries with Self-Enhanced Storage Mechanism

“…For the comparison between the BPN monolayer and biphenylite (Figure S9 ), the capacity on the BPN monolayer for storing Li/Na is only 186/83 mAh·g –1 , significantly lower than that in biphenylite (744/372 mAh·g –1 ). In contrast, the monolayer benefits from its bilayer multistorage characteristic, achieving a specific capacity of 1489 mAh·g –1 for K ion storage, several times higher than that of biphenylite (372 mAh·g –1 ). In terms of operating voltage, biphenylite displays a significantly higher and more stable range compared to the BPN monolayer.…”

“…Recently, a new graphene allotrope, biphenylene network (BPN), has been successfully synthesized, which consists of periodically arranged sp 2 hybridized carbon atoms with four-, six-, and eight-membered rings (C 4 , C 6 , and C 8 rings) in its flat and anisotropic structure. It is a metal with good stability and excellent properties, such as anisotropic thermal conductivity, , anisotropic charge transport, slight anisotropic mechanical behavior, etc., for application in topological superconductors; electrocatalytic catalysis for hydrogen evolution and oxygen reduction; anticorrosion coatings; spintronics; Li–sulfur batteries; and Li, − Na, , and K ion storage (via ion adsorption storage on the BPN monolayer surfaces; see part A in the Supporting Information for a more detailed comparison). Furthermore, it has been predicted to prefer applying AA stacking or its slight sliding pattern to form the van der Waals (vdW) layered bulk, , called “biphenylite” here in analogy to graphite.…”