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1 Electronic Supplementry Informtion Assemling cron-coted hollow α-fe 2 nnohorns on the CNT ckone for superior lithium storge cpility Corresponding uthor: Xiong Wen (Dvid) Lou* School of Chemicl nd Biomedicl Engineering, Nnyng Technologicl University, 70 Nnyng Drive, Singpore, Emil: xwlou@ntu.edu.sg; Tel: Experimentl Detils Pre-tretment of cron nnotues Cron nnotues (CNTs) used in this work re provided y X2 Lwres Pte. Ltd., of which the dimeter is in rnge of nm nd the length is round severl micrometers. 3 g of the CNTs is refluxed in 90 ml of HN (65 wt.%) t 120 o C for 6 h. After tht, the cid treted CNTs re rinsed with DI wter until neutrl ph vlue is reched. Then they re collected y filtrtion nd dried t 60 o C for further use. Synthesis of the CNT@FeOOH hierrchicl structure For the growth of β-feooh nnospindles on CNT ckones, 5 mg of the CNTs is dispersed in 10 ml of queous solution of FeCl 3 (0.12 M) y ultr-soniction for min in cpped ottle. After thorough mixing, the suspension is kept in n oil th under stirring t 75 o C for 5 h. The finl products re collected y severl rinse-centrifugtion (2000 rpm) cycles efore drying t 60 o C. Synthesis of the CNT@Fe 2 hierrchicl structure For the formtion of hollow α-fe 2 nnohorns on CNT ckones, certin mount of CNT@FeOOH hierrchicl structures is nneled in ir t 400 o C for 4 h with slow rmp rte of 0.5 o C min -1. Cron coting of CNT@Fe 2 hierrchicl structures For the cron coting of CNT@Fe 2 hierrchicl structures, 20 mg of the CNT@Fe 2 smples is dispersed in 40 ml of queous solution of glucose (0.06 M). After thorough mixing, the suspension is trnsferred into 50 ml Teflon-lined stinless steel utoclve nd kept in n oven t 180 o C for 6 h. The otined products re collected y severl rinse-centrifugtion (2000 rpm) cycles efore drying t 60 o C. Mterils chrcteriztion All smples were chrcterized y field-emission scnning electron microscope (FESEM, JEOL, JSM-7600F), trnsmission electron microscope (TEM, JEOL, JEM-2010 nd JEM-2100F), powder X-ry diffrction (XRD, Bruker, D8-Advnce X-ry Diffrctometer, Cu Kα, λ = Å), nitrogen dsorption/desorption (Quntchrome Instruments, Autosor AS-6B) nd thermogrvimetric nlysis (TGA, Shimdzu, DRG-60). The electrochemicl mesurements were conducted using two-electrode Swgelok cells with pure lithium foil s the counter nd reference electrode t room temperture. The S1

2 working electrode consists of test mteril (e.g., 2 with or without cron coting), cron lck (Super-P-Li) nd polyvinylidene difluoride (PVDF) in weight rtio of 7:2:1. The electrolyte used is 1.0 M LiPF 6 in 50:50 (w/w) mixture of ethylene cronte nd diethyl cronte. Cell ssemly is crried out in n Ar-filled gloveox with concentrtions of moisture nd oxygen elow 1.0 ppm. The glvnosttic chrge/dischrge tests were performed using Newre ttery tester t different current densities with cut-off voltge window of V. The clcultion of the specific cpcity is sed on the overll mss of the composite mteril synthesized, for exmple, cron coted CNT@Fe 2 structures. Electrochemicl impednce spectroscopy (EIS) ws performed using n CHI660C electrochemistry worksttion y pplying n c mplitude of 5 mv over the frequency rnge from 0.1 to 10 5 Hz. CNT@FeOOH nnostructures CNT@Fe 2 nnostructures Intensity (.u.) (002) CNT (130) (012) (002) CNT (400) (211) (301) (104) (110) (113) (202) (411) (024) (600) (251) Thet (degree) Figure S1 XRD profiles of CNT@FeOOH nd CNT@Fe 2 hierrchicl structures. CNT FeOOH CNT Fe 2 Figure S2 HRTEM imges of CNT@FeOOH nd CNT@Fe 2 hierrchicl structures. S2

3 c d Figure S3 TEM imges of the smples otined y the hydrolysis of FeCl 3 with vrious initil concentrtion: (, ) 0.03 M, (c) 0.06 M, (d) 0.36 M. Figure S4 TEM imges of CNT@Fe 2 structures otined y nneling t different temperture: () 250 o C, () 300 o C. Figure S5 N 2 dsorption/desorption isotherms of () CNT@FeOOH, () CNT@Fe 2 nd (c) cron coted CNT@Fe 2 hierrchicl structures. S3

4 Weight (wt. %) Temperture o C 30 wt. % Figure S6 Thermogrvimetric nlysis of cron coted CNT@Fe 2 structures. The test ws conducted in ir with rmpe rte of 10 o C min -1. Cron Figure S7 TEM imge showing the presence of uniform cron nnocoting round the scffold of CNT@Fe 2 hierrchicl structures. 100 Coulomic Efficiency (%) Cycle Numer Figure S8 Coulomic efficiency of cron coted CNT@Fe 2 structures cycled etween V t current density of 500 ma g -1. S4

5 1400 Cron coted 2 -Fe 2 nnoprticles Z im /ohm Z re /ohm Figure S9 Nyquist plots of the electrodes composed of the hierrchicl structures of cron coted CNT@Fe 2 or α-fe 2 nnoprticles. S5

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