Double-Holey-Heterostructure Frameworks Enable Fast, Stable, and

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Double-Holey-Heterostructure Frameworks Enable Fast, Stable and Simultaneous Ultrahigh Gravimetric, Areal, and Volumetric Lithium Storage Zhonghui Chen, Jiadong Chen, Fanxing Bu, Phillips O. Agboola, Imran Shakir, and Yuxi Xu ACS Nano, Just Accepted Manuscript • DOI: 10.1021/acsnano.8b08071 • Publication Date (Web): 10 Dec 2018 Downloaded from http://pubs.acs.org on December 10, 2018

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Double-Holey-Heterostructure Frameworks Enable Fast, Stable and Simultaneous Ultrahigh Gravimetric, Areal, and Volumetric Lithium Storage Zhonghui Chen†, Jiadong Chen†, Fanxing Bu†, Phillips O. Agboola‡, Imran Shakir*§, Yuxi Xu*† †State

Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular

Science, Fudan University, Shanghai 200433, China ‡Mechanical

Engineering Department, College of Applied Engineering, King Saud University

(Al Muzahimiyah Branch), Riyadh 11421, Saudi Arabia §Sustainable

Energy Technologies Center, College of Engineering, King Saud University,

Riyadh 11421, Kingdom of Saudi Arabia KEYWORDS: double-holey heterostructure, 3D framework, lithium storage, areal and volumetric capacity, electrochemical energy storage

ABSTRACT: Deliberate design of advantageous nanostructures holds great promise for developing high-performance electrode materials for electrochemical energy storage. However, it remains a tremendous challenge to simultaneously gain high gravimetric, areal, and volumetric capacities as well as high rate performance and cyclability to meet practical requirements mainly due to the intractable insufficient ion diffusion and limited active sites for dense electrodes with high areal mass loadings. Herein we report a double-holey-heterostructure framework, in which

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holey Fe2O3 nanosheets (H-Fe2O3) are tightly and conformably grown on the holey reduced graphene oxide (H-RGO). This hierarchical nanostructure allows for rapid ion and electron transport and sufficient utilization of active sites throughout a highly compact and thick electrode. Therefore, the free-standing flexible H-Fe2O3/H-RGO heterostructure anode can simultaneously deliver ultrahigh gravimetric, areal, and volumetric capacities of 1524 mAh g-1, 4.72 mAh cm-2 and 2621 mAh cm-3, respectively, at 0.2 A g-1 after 120 cycles, and extraordinary rate performance with a capacity of 487 mAh g-1 (1.51 mAh cm-2) at a high current density of 30 A g-1 (93 mA cm-2) as well as excellent cycling stability with a capacity retention of 96.3% after 1600 cycles, which has rarely been achieved before.

Electrochemical energy storage devices including batteries and supercapacitors have played vital role in our current society.1-3 The electrode materials are the central components of these devices and largely dictate their ultimate performance. With rapid development of portable electronic products and newly emerging large scale applications such as electric vehicles and electricity grid, the state-of-the-art commercial electrodes cannot meet the increasing requirements for the energy devices such as larger energy density, higher charge-discharge rates, and longer cycling life.4,5 For example, the commercial anodes for lithium-ion batteries (LIBs) are mainly graphite, which severely suffers from low capacity (372 mAh g-1) and poor rate performance.6,7 Therefore, considerable efforts have been devoted to the exploitation of other anode materials with higher theoretical capacity, such as metal/silicon, metal oxides, and organic polymers.8-10 In this regard, deliberate synthesis of advantageous nanostructures has achieved great success in efficiently improving the electrochemical performance of these promising anode materials.11-16 However, most previous studies focus on the enhancement of gravimetric capacity and these excellent results are usually achieved in relatively thin and highly porous electrodes with low areal mass

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