The limitation of areal energy density of rechargeable aqueous hybrid batteries(RAHBs)has been a sig-nificant longstanding problem that impedes the application of RAHBs in miniaturized energy storage.Constructing thick electrodes with optimized geometrical properties is a promising strategy for achieving high areal energy density,but the sluggish ion/electron transfer and poor mechanical stability,as well as the increased electrode thickness,itself present well-known problems.In this work,a 3D printing tech-nique is introduced to construct an ultra-thick lithium iron phosphate(LFP)/carboxylated carbon nan-otube(CNT)/carboxyl terminated cellulose nanofiber(CNF)composite electrode with uncompromised reaction kinetics for high areal energy density Li-Zn RAHBs.The uniformly dispersed CNTs and CNFs form continuous interconnected 3D networks that encapsulate LFP nanoparticles,guaranteeing fast electron transfer and efficient stress relief as the electrode thickness increases.Additionally,multistage ion diffu-sion channels generated from the hierarchical porous structure assure accelerated ion diffusion.As a result,LFP/Zn hybrid pouch cells assembled with 3D printed electrodes deliver a well-retained reversible gravimetric capacity of about 143.5 mAh g-1 at 0.5 C as the electrode thickness increases from 0.52 to 1.56 mm,and establish a record-high areal energy density of 5.25 mWh cm-2 with an impressive utiliza-tion of active material up to 30 mg cm-2 for an ultra-thick(2.08 mm)electrode,which outperforms almost all reported zinc-based hybrid-ion and single-ion batteries.This work opens up exciting prospects for developing high areal energy density energy storage devices using 3D printing.

Hanna He;Dan Luo;Li Zeng;Jun He;Xiaolong Li;Huaibo Yu;Chuhong Zhang

State Key Laboratory of Polymer Materials Engineering,Polymer Research Institute,Sichuan University,Chengdu 610065,China

科学通报（英文版）

[1]Hanna He;Dan Luo;Li Zeng;Jun He;Xiaolong Li;Huaibo Yu;Chuhong Zhang-.3D printing of fast kinetics reconciled ultra-thick cathodes for high areal energy density aqueous Li-Zn hybrid battery)[J].科学通报（英文版）,2022(12):1253-1263

RAHBs,uncompromised

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