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1 Supporting Informtion In-situ grown S nnosheets on fom: An ultrhigh electroctive cthode for roomtemperture N-S tteries Bin-Wei Zhng 1, Yun-Dn Liu 2, Yun-Xio Wng* 1, Lei Zhng 1, Ming-Zhe Chen 1, Wei-Hong Li 1, Shu-Lei Chou 1, Hu-Kun Liu 1 nd Shi-Xue Dou* 1 Mr. B.W. Zhng, Dr. Y.-X. Wng, Mr. L. Zhng, Mr. M. Z. Chen, Mr. W. H. Li, Dr. S.-L. Chou, Prof. H.-K. Liu, Prof. S.-X. Dou 1 Institute for Superconducting nd Electronic Mterils, Austrlin Institute of Innovtive Mterils, University of Wollongong, Innovtion Cmpus, Squires Wy, North Wollongong, New South Wles, Austrli. *E-mil: yunxio@uow.edu.u; shi@uow.edu.u Dr. Y. D. Liu 2 Hunnn Key Lortory of Micro-Nno Energy Mterils nd Devices, Xingtn University, Hunn 41115, PR Chin. S1

2 Experimentl Section Smples preprtion: All the chemicls, including Sulfur powder, NClO4 (98%), propylene cronte (99.7%), ethylene cronte (99%), fluoroethylene cronte (99%), cron lck, doule-wlled cron nnotues (CNTs), croxymethyl cellulose (CMC) (verge Mw ~,), nd poly(crylic cid) (PAA) (verge Mv ~4,), fom, nd glss fire, were purchsed from Sigm-Aldrich. The electrode slurry ws prepred y fully mixing 6wt% S, 1wt% cron lck, 1wt% CNT, 1wt% CMC nd 1wt% PAA in n pproprite mount of wter y plnetry mixer (KK-S). Then, it ws psted on fom, which ws followed y drying t C or C for 2 hours in vcuum oven, nmed s S nnosheets@ fom- (S nnosheets structure) or S prticles@ fom- (S prticles). The electrode slurry psted on foil nd Al foil, which were used doctor lde with thickness of mm, nd then drying t C for 2 hours in vcuum oven (nmed s S/ foil- nd S/Al foil-). Structurl chrcteriztion: The morphologies of the smples were investigted y fieldemission SEM (JEOL JSM-7FA), TEM nd STEM (JEOL ARM-F, ). The XRD ptterns were collected y powder XRD (GBC MMA diffrctometer) with K rdition t scn rte of 2 degree per minute. Electrochemicl mesurements: The electrochemicl tests were conducted y ssemling coin-type hlf-cells in n rgon-filled glove ox. The fom ws cut y 1 cm*1 cm, foil nd Al foil working electrode ws prepred y punching the electrode film into discs.97cm in dimeter. The sodium foil ws cut using surgicl lde from sodium ulk stored in minerl oil, nd it ws employed s oth reference nd counter electrode. The electrodes were seprted y glss fire seprtor. Electrolyte consisting of 1. M NClO4 in propylene cronte/ethylene cronte with volume rtio of 1:1 nd 5wt% fluoroethylene cronte dditive (PC/EC + 5wt% FEC) ws prepred nd used in this work. The electrochemicl S2

3 performnces were tested on LAND Bttery Tester within voltge window of V. All the cpcities of cells hve een normlized sed on the weight of ctive mterils in the form of S. Cyclic voltmmetry ws performed using Biologic VMP-3 electrochemicl worksttion. To evlute the mount of S emedded in the fom, foil nd Al foil fter drying t C, we use weight loss method : four pieces of lnk fom (m1), foil nd Al foil were weight; electrode slurry ws psted on them, dried on room-temperture, nd then t C for 2 hours in vcuum oven. After nturl cooling, their qulities were weight (m2); finlly, dried t C for 2 hours in vcuum oven, nd weight their qulities (m3). The S loding rtio of S ( s) emedded in the fom, foil nd Al foil re: s = (m 2 m 1 ).6 (m 2 m 3 ) m 3 m 1 Tle S1. Weight loss of fom, foil nd Al foil. No. m1/g m2/g m3/g s/% Averge s/% fom foil Al foil S3

4 nm nm c Figure S1. () nd () SEM imges of S nnosheets@ fom-. (c). Picture of S nnosheets@ fom-. S4

5 Figure S2. () HADDF-STEM imge of S prticles; () mpping of S element. nm nm Figure S3. SEM imge of () S/ foil- nd () S/Al foil-. S5

6 nm nm Figure S4. SEM imge of () fom CMC- nd () fom PAA-. S nnosheets@ nno-sheet@ fom- S 2 S Intense /.u. S prticle@ fom- (111) () S power / degree Figure S5. XRD of S nnosheets@ fom- (red line), S prticles@ fom- (lue line) nd S power. S6

7 d C S e C S c f C S Figure S6. SEM imges of S nnosheets@ fom- with different res ()-(c); (d)-(f), the corresponding EDX nlysis with ()-(c). Tle S2. EDX nlysis for S nnosheets@ fom- from SEM in figure S6. Position C (wt.%) C (t.%) (wt.%) (t.%) S (wt.%) S (t.%) S (wt.%) c verge Active mterils S7

8 d C S e C S c f C S Figure S7. SEM imges of S prticle@ fom- with different res ()-(c); (d)-(f), the corresponding EDX nlysis with ()-(c). Tle S3. EDX nlysis for S prticle@ fom- from SEM in figure S7. Position C (wt.%) C (t.%) (wt.%) (t.%) S (wt.%) S (t.%) 2S (wt.%) c verge Active mterils S8

9 Tle S4. Comprison of our est-performing mterils with previously pulished N/S tteries, in terms of initil cpcity. 1 st cycling dischrge cpcity (mah g -1 ) Electrode (current density) S nno-sheet 3189 (this work) ( ma g -1 ) microporous cron sulfur composite 1614 cthode 1 (.1 C) Inter-connected mesoporous cron 1215 mah g -1 hollow nnospheres S composite 2 ( ma g -1 ) nno-copper-ssisted immoi- mah g -1 lizing S 3 (.3 C) cron nnotue inside nd sulfurcontining microporous cron sheth 161 mah g -1 (.1 C) outside 4 One-dimensionl cron-sulfur composite 1158 mah g -1 fiers 5 (.1 C) S9

10 .1 S prticles@ fom-. S/ foil- i / ma. -.1 i / ma -.1 the first cycle the first cycle E / V E / V c. S/Al foil- i / ma -.5 the first cycle E / V Figure S8. Cyclic voltmmogrms of () S prticles@ fom-, () S/ foil-, nd (c) S/Al foil- in RT N-S cell in the 9 cycles within the voltge window of V t scn rte of.1 mv s -1. References (1) Wei, S.; Xu, S.; Agrwrl, A.; Choudhury, S.; Lu, Y.; Tu, Z.; M, L.; Archer, L. A. A Stle Room-Temperture Sodium-Sulfur Bttery. Nt. commun. 216, 7, (2) Wng, Y. X.; Yng, J.; Li, W.; Chou, S. L.; Gu, Q. F.; Liu, H. K.; Zho, D.; Dou, S. X. Achieving High-Performnce Room-Temperture Sodium-Sulfur Btteries With S@Interconnected Mesoporous Cron Hollow Nnospheres. J. Am. Chem. Soc. 216, 138, (3) Zheng, S.; Hn, P.; Hn, Z.; Li, P.; Zhng, H.; Yng, J. Nno-Copper-Assisted Immoiliztion of Sulfur in High-Surfce-Are Mesoporous Cron Cthodes for Room Temperture N-S Btteries. Adv. Energy Mter. 214, 4, (4) Xin, S.; Yin, Y. X.; Guo, Y. G.; Wn, L. J. A High-Energy Room-Temperture Sodium-Sulfur Bttery. Adv. Mter. 214, 26, S1

11 (5) Hwng, T. H.; Jung, D. S.; Kim, J. S.; Kim, B. G.; Choi. J. W. One-Dimensionl Cron-Sulfur Composite Fiers for N-S Rechrgele Btteries Operting t Room Temperture. Nno Lett. 213, 13, S11