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Fast-Charging High-Energy Battery–Supercapacitor Hybrid: Anodic Reduced Graphene Oxide– Vanadium(IV) Oxide Sheet-on-Sheet Heterostructure Ramkrishna Sahoo, Tae Hoon Lee, Duy Tho Pham, Thi Hoai Thuong Luu, and Young Hee Lee ACS Nano, Just Accepted Manuscript • DOI: 10.1021/acsnano.9b05605 • Publication Date (Web): 21 Aug 2019 Downloaded from pubs.acs.org on August 21, 2019

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ACS Nano

Fast-Charging High-Energy Battery–Supercapacitor Hybrid: Anodic Reduced Graphene Oxide–Vanadium(IV) Oxide Sheet-on-Sheet Heterostructure Ramkrishna Sahoo†,‡, Tae Hoon Lee†, Duy Tho Pham†, Thi Hoai Thuong Luu†,₴, Young Hee Lee†,₴* †

Center for Integrated Nanostructure Physics (CINAP), Institute for Basic Science (IBS), Suwon 16419, Republic of Korea. ‡ Centre for Advanced Studies (CAS), Dr. APJ Abdul Kalam Technical University (AKTU), Lucknow, India. ₴ Department of Energy Science, Sungkyunkwan University (SKKU), Suwon 16419, Republic of Korea. *Corresponding author E-mail address: [email protected] (Y. H. Lee).

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ABSTRACT The battery–supercapacitor hybrid (BSH) device has potential applications in energy storage and can be a remedy for low-power batteries and low-energy supercapacitors. Although several studies have investigated on electrode materials (particularly for a battery-type anode material) and design for BSHs, the energy density and power density are insufficient (far from the levels required for practical applications). Herein, a hierarchical vanadium (IV) oxide on reduced graphene oxide (rGO@VO2) heterostructure as an anode and activated carbon on carbon cloth (AC@CC) as a cathode are proposed for fabricating an advanced BSH. The mixed valency of V ions inside the as-prepared VO2 matrix (V3+ and V4+) facilitates redox reactions at a low potential, giving rise to rGO@VO2 as a typical anode with a working potential of 0.01–3 V (vs Li/Li+). The sheet-on-sheet heterostructured rGO@VO2 yields a high specific capacity of 1214 mAh g−1 at 0.1 A g−1 after 120 cycles, with a high rate capability and stability. The rGO@VO2//AC@CC BSH device exhibits a maximum gravimetric energy density of 126.7 Wh kg−1 and a maximum gravimetric power density of ~10000 W kg−1 within a working voltage range of 1–4 V. Moreover, it exhibits fast charging times of 5 and 834 s with energy densities of 15.6 and 82 Wh kg −1, respectively. KEYWORDS: battery–supercapacitor hybrids, rGO@VO2 sheet-on-sheet heterostructure, working potential, energy density, fast charging, self-discharge.

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ACS Nano

Li-ion batteries (LIBs) dominate the energy-storage market owing to their high energy density (~150 Wh kg−1).1-3 However, intrinsically lethargic solid-state Li-ion diffusion inside the bulk electrode results in a low power density (