Investigation of the Na Intercalation Mechanism into Nanosized V 2 O 5 /C Composite Cathode Material for Na-Ion Batteries Ghulam Ali, , Ji-Hoon Lee, Si Hyoung Oh, , Byung Won Cho, Kyung-Wan Nam, § and Kyung Yoon Chung* ,, Center for Energy Convergence Research, Korea Institute of Science and Technology, Hwarang-ro 14-gil 5, Seongbuk-gu, Seoul 136-791, Republic of Korea Korea University of Science and Technology, 217 Gajeong-ro Yuseong-gu, Daejeon 305-333, Republic of Korea § Department of Energy and Materials Engineering, Dongguk University-Seoul, Seoul 100-715, Republic of Korea ABSTRACT: There is a signicant interest to develop high- performance and cost-eective electrode materials for next- generation sodium ion batteries. Herein, we report a facile synthesis method for nanosized V 2 O 5 /C composite cathodes and their electrochemical performance as well as energy storage mechanism. The composite exhibits a discharge capacity of 255 mAh g -1 at a current density of 0.05 C, which surpasses that of previously reported layered oxide materials. Furthermore, the electrode shows good rate capability; discharge capacity of 160 mAh g -1 at a current density of 1 C. The reaction mechanism of V 2 O 5 upon sodium insertion/extraction is investigated using ex situ X-ray diraction (XRD) and synchrotron based near edge X-ray absorption ne structure (NEXAFS) spectroscopy. Ex situ XRD result of the fully discharged state reveals the appearance of NaV 2 O 5 as a major phase with minor Na 2 V 2 O 5 phase. Upon insertion of sodium into the array of parallel ladders of V 2 O 5 , it was conrmed that lattice parameter of c is increased by 9.09%, corresponding to the increase in the unit-cell volume of 9.2%. NEXAFS results suggest that the charge compensation during de/ sodiation process accompanied by the reversible changes in the oxidation state of vanadium (V 4+ V 5+ ). KEYWORDS: Na-ion batteries, nanosized V 2 O 5 , NaV 2 O 5 , X-ray diraction, near-edge X-ray absorption ne structure INTRODUCTION Electricity produced by dierent intermittent renewable power sources such as wind and solar energies often relies on stationary energy storage systems (ESS). Achieving the high eciency and superior safety is essential for large-scale rechargeable batteries. 1,2 Lithium-ion batteries (LIBs) are facing the issues of high production cost, limited resources, and serious safety concerns thus not suitable for the use of ESS. In recent years, researchers have been investigating sodium-ion batteries (NIBs) as a potential alternative to the LIBs for the use of large-scale ESS. 3-5 World-wide abundant resources of sodium make NIBs a potentially low cost technology. 5-7 Although, sodium is the next smallest and lightest alkali-metal after lithium in periodic table, 8 NIBs are still inferior to LIBs in terms of energy and power densities because of the larger size and lower negative reduction potential of sodium as compared to its counterpart. 9 To solve these issues, electrode material should be designed with a large concentration of interstitial site, where the sodium could be reversibly occupied, as well as large open tunnels. 10 As one of the strategies, a number of layered cathode materials (Na x MO 2 ; x = 0.44-1, M = 3d transition metals) have been investigated for the reversible sodium intercalation. Unfortunately, they delivered limited reversible capacity of 160 mAh g -1 and suered with poor cycle and rate performance because of structural instability. 8 Vanadium pentoxide (V 2 O 5 ) is considered as promising active material because of its unique crystal structure with large interlayer spacing of 4.4 Å. 11,12 To date, layered V 2 O 5 has been intensively investigated in LIBs and supercapacitors. 13,14 The lithium insertion mechanism of V 2 O 5 is well understood. 15 Two lithium ions can be reversibly inserted/extracted from the layered V 2 O 5 (with a composition of Li 2 V 2 O 5 ), resulting in a high capacity of 294 mAh g -1 . 11,12 It is also known that layered V 2 O 5 is electrochemically active when the electrode was applied in NIBs but exhibiting less noticeable performances. 16 Layered vanadium oxide xerogel delivers high capacity in NIBs but it shows fast capacity fade because of large lattice breathing upon de/sodiation. 17 Despite having a high theoretical capacity, V 2 O 5 is also facing barriers of poor electrical conductivity and low working potential compared to other cathodes in NIBs. 15 Furthermore, sodium insertion mechanism in layered V 2 O 5 is Received: December 8, 2015 Accepted: February 18, 2016 Published: February 18, 2016 Research Article www.acsami.org © 2016 American Chemical Society 6032 DOI: 10.1021/acsami.5b11954 ACS Appl. Mater. Interfaces 2016, 8, 6032-6039