Achieving Fast and Durable Lithium Storage through Amorphous FeP Nanoparticles Encapsulated in Ultrathin 3D P-Doped Porous Carbon Nanosheets

Abstract

Conversion-type transition-metal phosphide anode materials with high theoretical capacity usually suffer from low-rate capability and severe capacity decay, which are mainly caused by their inferior electronic conductivities and large volumetric variations together with the poor reversibility of discharge product (Li 3 P), impeding their practical applications. Herein, guided by density functional theory calculations, these obstacles are simultaneously mitigated by confining amorphous FeP nanoparticles into ultrathin 3D interconnected P-doped porous carbon nanosheets (denoted as FeP@CNs) via a facile approach, forming an intriguing 3D flake-CNs-like configuration. As an anode for lithium-ion batteries (LIBs), the resulting FeP@CNs electrode not only reaches a high reversible capacity (837 mA h g −1 after 300 cycles at 0.2 A g −1 ) and an exceptional rate capability (403 mA h g −1 at 16 A g −1 ) but also exhibits extraordinary durability (2500 cycles, 563 mA h g −1 at 4 A g −1 , 98% capacity retention). By combining DFT calculations, in situ transmission electron microscopy, and a suite of ex situ microscopic and spectroscopic techniques, we show that the superior performances of FeP@CNs anode originate from its prominent structural and compositional merits, which render fast electron/ion-transport kinetics and abundant active sites (amorphous FeP nanoparticles and structural defects in P-doped CNs) for charge storage, promote the reversibility of conversion reactions, and buffer the volume variations while preventing pulverization/aggregation of FeP during cycling, thus enabling a high rate and highly durable lithium storage. Furthermore, a full cell composed of the prelithiated FeP@CNs anode and commercial LiFePO 4 cathode exhibits impressive rate performance while maintaining superior cycling stability. This work fundamentally and experimentally presents a facile and effective structural engineering strategy for markedly improving the performance of conversion-type anodes for advanced LIBs.

In Situ Atomic‐Scale Observation of Reversible Potassium Storage in Sb2S3@Carbon Nanowire Anodes

“…The rapidly growing markets of renewable energy grid storage and electric vehicles have created a strong demand for high‐energy/power‐density rechargeable batteries, such as lithium‐ion batteries (LIBs). [ 1–9 ] Considering the increasing cost of lithium and the geographically uneven distribution of lithium resources, rechargeable batteries with cheap and abundant elements (e.g., sodium, potassium, magnesium, etc.) have attracted notable attention from the electrochemical energy storage field.…”

Ultra-small Fe3O4 nanodots encapsulated in layered carbon nanosheets with fast kinetics for lithium/potassium-ion battery anodes

“…Layered carbon sheets are functioned as an elastic buffer with pre-reserved spaces to prevent pulverization or aggregation of encapsulated ultra-small Fe 3 O 4 nanodots during cycles, maintaining stable and unobstructed channels for the fast electronic and ionic conductivity. [54][55][56] The thin and layered carbon nanosheets not only enable full utilization of active ultra-small Fe 3 O 4 nanodots and abundant accessibility of electrolyte, but also accommodate the mechanical stress from the volume variations, as shown in Fig. S11a-i † in both LIBs and KIBs.…”

Revealing the working mechanism of a multi-functional block copolymer binder for lithium-sulfur batteries

“…Electrochemical energy storage systems with high energy density, low cost, and long cycle life have been sought for numerous applications, including modern mobile electronic devices, electric vehicles, and the sustainable energy industry [1][2][3][4]. Among the various energy storage candidates, lithiumsulfur (Li-S) batteries stand out because the abundance of sulfur, and it has low cost, high theoretical capacity (1675 mAh g -1 ), and high theoretical energy density (2567 Wh kg -1 ) [5][6][7].…”