Hierarchical 3D Porous Hydrogen-Substituted Graphdiyne for High-Performance Electrochemical Lithium-Ion Storage

Abstract

Graphdiyne (GDY) has realized significant achievements in lithium-ion batteries (LIBs) because of its unique π-conjugated skeleton with sp- and sp2-hybridized carbon atoms. Enriching the accessible surface areas and diffusion pathways of Li ions can realize more storage sites and rapid transport dynamics. Herein, three-dimensional porous hydrogen-substituted GDY (HsGDY) is developed for high-performance Li-ion storage. HsGDY, fabricated via a versatile interface-assisted synthesis strategy, exhibits a large specific surface area (667.9 m2 g–1), a hierarchical porous structure, and an expanded interlayer space, which accelerate Li-ion accessibility and lithiation/delithiation. Owing to this high π-conjugated, conductive, and porous framework, HsGDY exhibits a large reversible capacity (930 mA h g–1 after 100 cycles at 1 A g–1), superior cycle (720 mA h g–1 after 300 cycles at 1 A g–1), and rate (490 mA h g−1 at 5 A g–1) performances. Density functional theory calculations of the low diffusion barrier in the lamination and vertical directions further reveal the fast Li-ion transport kinetics of HsGDY. Additionally, a LiCoO2–HsGDY full cell is constructed, which exhibits a good practical charge/discharge capacity of 128 mA h g–1 and stable cycling behavior. This study highlights the advanced design of next-generation LIBs to sustainably develop the new energy industry.

Promoting CO2 electroreduction to CO by a graphdiyne-stabilized Au nanoparticle catalyst

“…10 Each acetylene unit in GDY is connected to the benzene ring, forming a planar porous structure that facilitates electrolyte diffusion, mass transfer and gas release. 11–13 In addition, due to its highly π-conjugated structure, large surface area, evenly distributed pores, good chemical stability, and excellent electron conductivity, GDY has shown great prospects in the fields of batteries, 14–18 optoelectronic devices 19–23 and electrocatalysis. 24–31 More importantly, due to its unique physical and chemical properties, there is a strong d–π electron interaction between the GDY substrate and metal catalysts.…”

Intercalating Elemental Se8 Rings and Cs+ Ions by Layered Selenidostannate: A Semiconductive Material for High-Energy Li-Ion Battery Anodes

“…Among them, rechargeable lithium-ion batteries (LIBs), hybrid electric vehicles, and smart grids, etc. are widely used. − …”

In Situ Fabrication of Graphdiyne Nanoisland Anchored Ti3C2Tx Film to Accelerate Intercalation Pseudocapacitance Kinetics

“…[ 22 ] As a novel all‐carbon framework, hydrogen‐rich graphdiyne (GDY) has a unique π‐conjugated sp 2 and sp‐hybridized skeleton, as well as a macroporous structure. [ 23,24 ] Therefore, if the realization of in situ growth of GDY within MXene generates a precisely controllable component, tunable enlarged interlayer spacing, great accessible active surface, and strong interfacial adhesion, in principle, the accelerated ion migration kinetics/storage and interfacial electron conduction will significantly enhance the intercalated capacitive behaviors and E vol .…”