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1 Copyright WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, Germany, 213. Supporting Information for Adv. Energy Mater., DOI: 1.12/aenm Reduction of Graphene Oxide by Hydrogen Sulfide: A Promising Strategy for Pollutant Control and as an Electrode for Li-S Batteries Chen Zhang, Wei Lv, Weiguo Zhang, Xiaoyu Zheng, Ming-Bo Wu, Wei Wei, Ying Tao, Zhengjie Li, and Quan-Hong Yang*

2 Copyright WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, Germany, 213. Supporting Information for Adv. Energy Mater., DOI: 1.12/aenm Reduction of Graphene Oxide by Hydrogen Sulfide: A Promising Strategy for Pollutant Control with A Byproduct as Electrode for Li-S Battery Chen Zhang, Wei Lv, Weiguo Zhang, Xiaoyu Zheng, Ming-Bo Wu, Wei Wei, Ying Tao, Zhengjie Li and Quan-Hong Yang* I Experimental Preparation of GO. Graphite oxide was prepared from natural flake graphite (8 mesh) by a modified Hummers method as reported previously. A GO suspension with a concentration of 2 mg ml -1 was obtained by ultrasonication of the graphite oxide in de-ionized water. Synthesis of H 2 S. The H 2 S gas used in this study was generated from the reaction between FeS and diluted H 2 SO 4 (1 wt.%). A certain amount of H 2 SO 4 was added to a flask containing excess FeS and the generated H 2 S gas was bubbled into the GO suspension. Preparation of the hybrid. Typically, was prepared by bubbling H 2 S into the GO suspension while stirring at 7 C. After a 2 h reaction, the obtained suspension was dried at 7 C for 48 h. The as-prepared black powder was denoted and no further heat treatment was made. Preparation of the GN/S hybrid. GN was prepared as reported previously. In brief, the asprepared GO was subjected to a vacuum-promoted low-temperature exfoliation at 2 C. Then, 2 mg GN and 2 mg S (calculated to have the same content of S as ) was ground to form a homogeneous mixture. The obtained mixture was heated at 155 C for 6 h to melt and diffuse S on the graphene layers. The obtained black powder was denoted GN/S. Materials characterization. XRD measurements were conducted at room temperature with a Bruker D-8 diffractometer (Cu Kα radiation, λ= nm). SEM and TEM observations were performed using Hitachi S-48 (Hitachi, Japan) and JEM-21F (JEOL, Japan) 11

3 instruments, respectively. Tecnai F3 (FEI) and Electron Energy Loss Spectrum (EELS, Gatan) was used for the element mapping. EDS was used for elemental analysis. Nitrogen adsorption was measured using a BEL mini-instrument, and the specific surface areas were obtained by Brunauer-Emmett-Teller (BET) analysis of the adsorption isotherms. Thermogravimetric analysis (TG, Rigaku, Japan) was performed in a N 2 atmosphere at a heating rate of 5 C/min to 5 C to calculate the fraction of sulphur in the hybird. Differential Scanning Calorimetry (DSC) was carried out using DSC 827 (Rigaku, Japan) with a heating rate of 5 C/min from RT to 45 o C under N 2 flow. X-ray photoelectron spectroscopy (XPS) analyses were conducted with a Physical Electronics PHI582 instrument using a magnesium anode (monochromatic Kα X-rays at ev) as the source. Raman spectra were recorded using a multi-wavelength micro-raman spectroscope (JY HR8) utilizing nm incident radiation and a 5 aperture. Electrochemical Measurements. The and GN/S cathodes were prepared by mixing 8 wt% or GN/S and 1 wt% super P with 1 wt% PVDF in NMP to form a slurry, which was stirred for 5 h and was then coated on an Al foil and dried under vacuum at 5 C for 24 h. The foil was then cut to a circular pellet with a diameter of 8 mm and used as the cathode. The electrolyte was 1. M LTFSI dissolved in DOL: DME (1:1 volume). A 232 coin cell was used to assemble the test cell in a Ar-filled glovebox (MBraun). CV curves were obtained using an Autolab workstation at a scan rate of.1 mv/s within a potential range of V (vs. Li + /Li). A LAND galvanostatic charge-discharge instrument was used to test the rate performance. The current density set for the cell here is based on the mass of sulfur in. II Results 22

4 Figure S1. Photographs of GO with no heating, GO heated at 7 C and Figure S2. Elemental maps of 33

5 Submitted to Figure S3. HRTEM of showing the fewlayered structure of the reduced graphene oxide, illustrating the graphene oxide is mainly less than 4 layers Va/cm (STP) g P/P 1. Figure S4. N2 isotherm of S DSC/W g Weight/% 8 S Temperature/ C 2 3 Temperature/ C Figure S5. TG and DSC curves of and pure S 4 4 4

6 Specific capacity/mah g GN/S GN/S Cycle number 1 Figure S6. Cycle performance of the and GN/S at a current density of 5 mah g -1. The Coulombic efficiency of is stablized at 94%, which is higher than GN/S (88%) Coulombic efficiency/% 55

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