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Supporting Information Fe 3 O 4 @Carbon Nanosheets for All-Solid-State Supercapacitor Electrodes Huailin Fan, Ruiting Niu, & Jiaqi Duan, Wei Liu and Wenzhong Shen * State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 31, PR China University of Chinese Academy of Sciences, Beijing, 149, PR China &State Key Laboratory of Separation Membranes and Membrane Processes, Institute of Functional Fiber, School of Materials Science and Engineering, Tianjin Polytechnic University, Tianjin 3387, China. College of Environmental and Chemical Engineering, Shanghai University, Shanghai, 2444, PR China. * E-mail: shenwzh2@yahoo.com S-1

Weight loss 1 8 6 4 a) Intensity b) C-G/AC CO2 Intensity c) NO2 C-G/AC 2 C-AC 1 2 3 4 5 6 7 8 Temperature ( C) 15 3 45 6 75 Temperature ( C) 15 3 45 6 75 Temperature ( C) Figure S1. a) TG-MS curves, b) the exhausted CO 2 of, and C-G/AC in air and c) the exhausted NO 2 of, and C-G/AC in air. Figure S2. SEM images and EDS patterns (a, b) and C-G/AC (c, d). Current density (A/g) -1-5 5 1 15 a) 5mv 1mv 2mv 5mv -1. -.8 -.6 -.4 -.2 Potential (V vs. Hg/HgO) Potential (V vs. Hg/HgO) -.2 -.4 -.6 -.8-1. b).5a/g 1A/g 2A/g 5A/g 1A/g 15A/g 2A/g -1.2 1 2 3 4 5 Time (s) Figure S3. CV of C-G/AC at 5-5mV/s (a) and GCD of C-G/AC at.5-2 A/g (b). S-2

Table S1 Electrochemical capacitance of composites electrode materials in three electrode. Electrode material Electrolyte Specific capacitance (F/g) Current density (A/g) Ref. MnO 2 doped nanoporous carbon 6 M KOH 496 1 1 MnO 2 on porous carbons 3 M KOH 15.5 2 MnO 2 /reduced graphene oxide 1 M Na 2 SO 4 328.5 3 biomass-derived carbon/mno2 1 M Na 2 SO 4 264 1 4 Carbon nanotubes decorated Co 3 O 4 6 M KOH 5 1 5 Co 3 O 4 intercalated reduced GO 1 M KOH 278.2 6 V 2 O 5 /polyindole and carbon cloth 5 M LiNO 3 535 1 7 V 2 O 5 /graphene hybrid aerogel 1 M Na 2 SO 4 486.5 8 MoO 3 /C hybrid 1 M H 2 SO 4 331 1 9 MoO 3 /graphene 1 M H 2 SO 4 36.2 1 Fe 3 O 4 doped porous carbon 2 M KOH 285 1 11 Activated carbon/fe 3 O 4 1 M Na 2 SO 3 168 2 12 Fe 3 O 4 nanoparticles grown on graphene 1 M KOH 22.5 13 Carbon nanosheets embedded Fe 3 O 4 6 M KOH 519 1 This work Carbon nanosheets embedded Fe 3 O 4 6 M KOH 586.5 This work 35 3 Volume (cm 3 /g) 25 2 15 1 5 Pore Volume (cm3/g).15.1.5. 2 4 6 8 1 Pore width (nm)..2.4.6.8 1. Relative Pressure (P/P ) Figure S4. N 2 adsorption isotherms (inset: pore size distributions) of CPY. Figure S5. SEM images of CPY. S-3

Phase angle(degree) -8-6 -4-2 C-G/AC 2.1 1 1 1 Frenquence/ HZ Figure S6. Phase angle-frequency plot of, and C-G/AC electrode in 6 M KOH electrolyte Potential (V) 1.6 1.4 1.2 1..8.6 -.6V -.8V -1.V -1.2V -1.4V.4.2. 2 4 6 8 1 12 14 16 Time (s) Figure S7. GCDs of all-solid-state asymmetric supercapacitor collected at different voltage windows at 1A/g. Normalized C'' (%) 1 8 6 4 2 6.25s 1.5s.1.1 1 1 1 1 1 Frenquence /HZ Figure S8. Imaginary capacitance-frequency plot of all-solid-state asymmetric supercapacitor from // CPY and //CPY Table S2 Solid state supercapacitor performance Electrode material Electrolyte Energy density Power density Ref. (Wh/kg) (W/kg) Co 3 O 4 nanowires and carbon aerogel PVA/KOH 17.9 75 14 Polyaniline-coated electrospun carbon PVA /H 2 SO 4 4.4 13 15 nanofibers Nitrogen-doped porous carbon PVA/H 2 SO 4 9.2 25 16 nanofibers Heteroatom-doped carbon PVA /Na 2 SO 4 17.2 27 17 composite film S-4

Hierarchical MnO 2 /Carbon Fiber PVA/KCl 19.17 5 18 N-graphene doped polyacrylic PVA /H 2 SO 4 5.8 11 19 acid/polyaniline composites Porous MoO 3 @CuO PVA/LiOH 7.9 8726 2 Carbon nanosheets embedded Fe 3 O 4 PVA/KOH 18.3 351 This work References (1) Zhang, Z. J.; Cheng, L. X.; Chen, X. Y., Nitrogen/Manganese Oxides Co-Doped Nanoporous Carbon Materials: Structure Characterization and Electrochemical Performances for Supercapacitor Applications. Electrochim. Acta, 215, 161, 84-94. (2) Zhang, Y.; Zhang, C.; Huang, G.; Xing, B.; Duan, Y., Synthesis and Capacitive Properties of Manganese Oxide Nanoparticles Dispersed on Hierarchical Porous Carbons. Electrochim. Acta, 215, 166, 17-116. (3) Wang, X.; Fan, X.; Li, G.; Li, M.; Xiao, X.; Yu, A.; Chen, Z., Composites of MnO 2 Nanocrystals and Partially Graphitized Hierarchically Porous Carbon Spheres with Improved Rate Capability for High-Performance Supercapacitors. Carbon, 215, 93, 258-265. (4) Mao, C.; Liu, S.; Pang, L.; Sun, Q.; Liu, Y.; Xu, M.; Lu, Z., Ultrathin MnO 2 Nanosheets Grown on Fungal Conidium-Derived Hollow Carbon Spheres as Supercapacitor Electrodes. RSC Adv., 216, 6, 5184-5191. (5) Ke, Q.; Tang, C.; Yang, Z. C.; Zheng, M.; Mao, L.; Liu, H.; Wang, J., 3D Nanostructure of Carbon Nanotubes Decorated Co 3 O 4 Nanowire Arrays for High Performance Supercapacitor Electrode. Electrochim. Acta, 215, 163, 9-15. (6) Arshad, N.; Duraisamy, N.; Omar, F. S.; MAHIPAL, Y. K.; Kasi, R.; Subramaniam, R. T., Enhanced Electrochemical Performance of Cobalt Oxide Nanocube Intercalated Reduced Graphene Oxide for Supercapacitor Application. RSC Advances, 216, 6, 34894-3492. (7) Zhou, X.; Chen, Q.; Wang, A.; Xu, J.; Wu, S.; Shen, J., Bamboo-Like Composites of V 2 O 5 /Polyindole and Activated Carbon Cloth as Electrodes for All-Solid-State Flexible Asymmetric Supercapacitors. ACS Appl. Mater. Interfaces, 216, 8, 3776-3783. (8) Wu, Y.; Gao, G.; Wu, G., Self-Assembled Three-Dimensional Hierarchical Porous V 2 O 5 /Graphene Hybrid Aerogels for Supercapacitors with High Energy Density and Long Cycle Life. J. Mater. Chem. A, 215, 3, 1828-1832. (9) Ji, H.; Liu, X.; Liu, Z.; Yan, B.; Chen, L.; Xie, Y.; Liu, C.; Hou, W.; Yang, G., In Situ Preparation of Sandwich MoO 3 /C Hybrid Nanostructures for High-Rate and Ultralong-Life Supercapacitors. Adv. Funct. Mater., 215, 25, 1886-1894. (1) Zhou, J.; Song, J.; Li, H.; Feng, X.; Huang, Z.; Chen, S.; Ma, Y.; Wang, L.; Yan, X., The Synthesis of Shape-Controlled [small alpha]-moo 3 /Graphene Nanocomposites for High Performance Supercapacitors. New J. Chem., 215, 39, 878-8786. (11) Wang, L.; Yu, J.; Dong, X.; Li, X.; Xie, Y.; Chen, S.; Li, P.; Hou, H.; Song, Y., Three-Dimensional Macroporous Carbon/Fe 3 O 4 -Doped Porous Carbon Nanorods for High-Performance Supercapacitor. ACS Sustainable Chem. Eng., 216, 4, 1531-1537. (12) Oh, I.; Kim, M.; Kim, J., Controlling Hydrazine Reduction to Deposit Iron Oxides on Oxidized Activated Carbon for Supercapacitor Application. Energy, 215, 86, 292-299. (13) Wang, Q. H.; Jiao, L. F.; Du, H. M.; Wang, Y. J.; Yuan, H. T., Fe 3 O 4 Nanoparticles Grown on S-5

Graphene as Advanced Electrode Materials for Supercapacitors. J.Power Sources, 214, 245, 11-16. (14) Liu, W.; Li, X.; Zhu, M.; He, X., High-performance All-solid state Asymmetric Supercapacitor Based on Co 3 O 4 Nanowires and Carbon Aerogel. J.Power Sources, 215, 282, 179-186. (15) Miao, F.; Shao, C.; Li, X.; Lu, N.; Wang, K.; Zhang, X.; Liu, Y., Polyaniline-coated Electrospun Carbon Nanofibers with High Mass Loading and Enhanced Capacitive Performance As Freestanding Electrodes For Flexible Solid-State Supercapacitors. Energy, 216, 95, 233-241. (16) Miao, F.; Shao, C.; Li, X.; Wang, K.; Liu, Y., Flexible Solid-state Supercapacitors Based on Freestanding Nitrogen-Doped Porous Carbon Nanofibers Derived From Electrospun Polyacrylonitrile@Polyaniline Nanofibers. J. Mater. Chem. A, 216, 4, 418-4187. (17) Zou, B. X.; Gao, Y.; Liu, B.; Yu, Y.; Lu, Y., Three Dimensional Heteroatom-doped Carbon Composite Film for Flexible Solid-State Supercapacitors. RSC Adv., 216, 6, 4483-4489. (18) Hu, X.; Xiong, W.; Wang, W.; Qin, S.; Cheng, H.; Zeng, Y.; Wang, B.; Zhu, Z., Hierarchical Manganese Dioxide/Poly(3,4-ethylenedioxythiophene) Core Shell Nanoflakes on Ramie-Derived Carbon Fiber for High-Performance Flexible All-solid-state Supercapacitor. ACS Sustainable Chem. Eng., 216, 4, 121-1211. (19) Wang, Y.; Tang, S.; Vongehr, S.; Syed, J. A.; Wang, X.; Meng, X., High-Performance Flexible solid-state Carbon Cloth Supercapacitors Based On Highly Processible N-graphene Doped Polyacrylic Acid/Polyaniline Composites. Sci. Rep. 216, 6. 12883. (2) Zhang, Y.; Lin, B.; Wang, J.; Han, P.; Xu, T.; Sun, Y.; Zhang, X.; Yang, H., Polyoxometalates@ Metal-Organic Frameworks Derived Porous MoM 3 @CuO as Electrodes for Symmetric All-Solid-State Supercapacitor. Electrochim. Acta, 216, 191, 795-84. S-6