TY - JOUR
T1 - In-Situ Laser Synthesis of Molecularly Dispersed and Covalently Bound Phosphorus-Graphene Adducts as Self-Standing 3D Anodes for High-Performance Fast-Charging Lithium-Ion Batteries
AU - Daffan, Gil
AU - Kothuru, Avinash
AU - Eran, Assaf
AU - Patolsky, Fernando
N1 - Publisher Copyright:
© 2024 The Author(s). Advanced Energy Materials published by Wiley-VCH GmbH.
PY - 2024/9/26
Y1 - 2024/9/26
N2 - Phosphorus shows promise as a next-generation anode material due to its high theoretical capacity of 2596 mAh g−1. However, challenges such as low conductivity, severe volume expansion, and the dissolution and migration of electrolyte-soluble lithium polyphosphides hamper high-performance capabilities. While carbon composites are widely researched as a solution through the physical encapsulation of micro-nano-phosphorus domains, anodes still exhibit low cycling stability and rate performance. In response, this work proposes a new approach, focusing on chemical anchoring and molecular dispersion of phosphorus within the carbon host. Through laser irradiation of a red phosphorus/phenolic resin blend, in-situ covalent binding of molecular phosphorus adducts to the as-forming laser-induced graphene is observed; directly synthesizing an additive-free, flexible and 3-dimensional mesoporous composite anode with high phosphorus content (33 wt.%), specific surface area (163.4 m2 g−1) and intrinsic conductivity (12 S cm−1). These anodes demonstrate remarkable cycling stability, with capacity retention of 98% after 3000 cycles at a high current density of 2 A g−1 and capacity of 673 mAh g−1. The high cycling stability is further confirmed through the complete inhibition of lithium polyphosphide “shuttle effect” by chemical anchoring of the molecularly dispersed active material. Furthermore, scale-up prospects utilizing laser-assisted additive manufacturing are investigated.
AB - Phosphorus shows promise as a next-generation anode material due to its high theoretical capacity of 2596 mAh g−1. However, challenges such as low conductivity, severe volume expansion, and the dissolution and migration of electrolyte-soluble lithium polyphosphides hamper high-performance capabilities. While carbon composites are widely researched as a solution through the physical encapsulation of micro-nano-phosphorus domains, anodes still exhibit low cycling stability and rate performance. In response, this work proposes a new approach, focusing on chemical anchoring and molecular dispersion of phosphorus within the carbon host. Through laser irradiation of a red phosphorus/phenolic resin blend, in-situ covalent binding of molecular phosphorus adducts to the as-forming laser-induced graphene is observed; directly synthesizing an additive-free, flexible and 3-dimensional mesoporous composite anode with high phosphorus content (33 wt.%), specific surface area (163.4 m2 g−1) and intrinsic conductivity (12 S cm−1). These anodes demonstrate remarkable cycling stability, with capacity retention of 98% after 3000 cycles at a high current density of 2 A g−1 and capacity of 673 mAh g−1. The high cycling stability is further confirmed through the complete inhibition of lithium polyphosphide “shuttle effect” by chemical anchoring of the molecularly dispersed active material. Furthermore, scale-up prospects utilizing laser-assisted additive manufacturing are investigated.
KW - anode
KW - covalent
KW - graphene
KW - laser
KW - lithium-ion
KW - molecular dispersion
KW - phosphorus
UR - http://www.scopus.com/inward/record.url?scp=85196728272&partnerID=8YFLogxK
U2 - 10.1002/aenm.202401832
DO - 10.1002/aenm.202401832
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AN - SCOPUS:85196728272
SN - 1614-6832
VL - 14
JO - Advanced Energy Materials
JF - Advanced Energy Materials
IS - 36
M1 - 2401832
ER -