TY - JOUR

T1 - First-principles investigation of Ag-, Co-, Cr-, Cu-, Fe-, Mn-, Ni-, Pd- and Rh-hexaaminobenzene 2D metal-organic frameworks

AU - Mortazavi, Bohayra

AU - Shahrokhi, Masoud

AU - Makaremi, Meysam

AU - Cuniberti, Gianaurelio

AU - Rabczuk, Timon

N1 - Funding information: B. M. and T. R. greatly acknowledge the financial support by European Research Council for COMBAT project (Grant number 615132 ).

PY - 2018/12

Y1 - 2018/12

N2 - Hexaaminobenzene (HAB)-derived two-dimensional metal−organic frameworks (MOFs) (Nature Energy 3(2018), 30–36) have most recently gained remarkable attentions as a novel class of two-dimensional (2D) materials, with outstanding performances for advanced energy storage systems. In the latest experimental advances, Ni-, Co- and Cu-HAB MOFs were synthesized in 2D forms, with high electrical conductivities and capacitances as well. Motivated by these experimental advances, we employed first-principles simulations to explore the mechanical, thermal stability and electronic properties of single-layer Ag-, Co-, Cr-, Cu-, Fe-, Mn-, Ni-, Pd- and Rh-HAB MOFs. Theoretical results reveal that Co-, Cr-, Fe-, Mn-, Ni-, Pd- and Rh-HAB nanosheets exhibit linear elasticity with considerable tensile strengths. Ab-initio molecular dynamics results confirm the high thermal stability of all studied nanomembranes. Co- and Fe-HAB monolayers show metallic behavior with low spin-polarization at the Fermi level. Single-layer Ag-, Cu-, Cr-, and Mn-HAB however yield perfect half-metallic behaviors, thus can be promising candidates for the spintronics. In contrast, Ni-, Pd- and Rh-HAB monolayers exhibit nonmagnetic metallic behavior. The insights provided by this investigation confirm the stability and highlight the outstanding physics of transition metal-HAB nanosheets, which are not only highly attractive for the energy storage systems, but may also serve for other advanced applications, like spintronics.

AB - Hexaaminobenzene (HAB)-derived two-dimensional metal−organic frameworks (MOFs) (Nature Energy 3(2018), 30–36) have most recently gained remarkable attentions as a novel class of two-dimensional (2D) materials, with outstanding performances for advanced energy storage systems. In the latest experimental advances, Ni-, Co- and Cu-HAB MOFs were synthesized in 2D forms, with high electrical conductivities and capacitances as well. Motivated by these experimental advances, we employed first-principles simulations to explore the mechanical, thermal stability and electronic properties of single-layer Ag-, Co-, Cr-, Cu-, Fe-, Mn-, Ni-, Pd- and Rh-HAB MOFs. Theoretical results reveal that Co-, Cr-, Fe-, Mn-, Ni-, Pd- and Rh-HAB nanosheets exhibit linear elasticity with considerable tensile strengths. Ab-initio molecular dynamics results confirm the high thermal stability of all studied nanomembranes. Co- and Fe-HAB monolayers show metallic behavior with low spin-polarization at the Fermi level. Single-layer Ag-, Cu-, Cr-, and Mn-HAB however yield perfect half-metallic behaviors, thus can be promising candidates for the spintronics. In contrast, Ni-, Pd- and Rh-HAB monolayers exhibit nonmagnetic metallic behavior. The insights provided by this investigation confirm the stability and highlight the outstanding physics of transition metal-HAB nanosheets, which are not only highly attractive for the energy storage systems, but may also serve for other advanced applications, like spintronics.

KW - 2D materials

KW - Energy storage

KW - First-principles

KW - MOFs

UR - http://www.scopus.com/inward/record.url?scp=85055903192&partnerID=8YFLogxK

U2 - 10.1016/j.mtener.2018.10.007

DO - 10.1016/j.mtener.2018.10.007

M3 - Article

AN - SCOPUS:85055903192

VL - 10

SP - 336

EP - 342

JO - Materials Today Energy

JF - Materials Today Energy

ER -