A Scalable Synthesis of Few-layer MoS2. Incorporated into Hierarchical Porous Carbon. Nanosheets for High-performance Li and Na Ion

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1 Supporting Information A Scalable Synthesis of Few-layer MoS2 Incorporated into Hierarchical Porous Carbon Nanosheets for High-performance Li and Na Ion Battery Anodes Seung-Keun Park, a,b Jeongyeon Lee, a Sungyool Bong, c Byungchul Jang, a Kwang-dong Seong, a Yuanzhe Piao* a,b,d a Program in Nano Science and Technology, Graduate School of Convergence Science and Technology, Seoul National University, 145 Gwanggyo-ro, Yeongtong-gu, Suwon si, Gyeonggi-do, , Republic of Korea. b Advanced Institutes of Convergence Technology, 145 Gwanggyo-ro, Yeongtong-gu, Suwon si, Gyeonggi-do, , Republic of Korea. c Korea Testing and Research Institute, 98, Gyoyukwon-ro, Gwacheon-si, Gyeonggi-do, Republic of Korea d Center for Nanoparticle Research, Institute for Basic Science (IBS), Republic of Korea. *Corresponding author: Yuanzhe Piao: parkat9@snu.ac.kr; S-1

2 Figure S1. SEM and TEM images of MHPC composite before silica etching S-2

3 Figure S2. (a) Low- and (b) high-magnification SEM images of MoS2/C composites synthesized by using oleic acid as the precursors. S-3

4 Figure S3. Large scale synthesis of MHPC composites (using 1 ml of OA and 0.52 g of ATTM) S-4

5 Figure S4. XRD pattern of MHPC-0.05, MHPC-0.2 and MoS2 powder synthesized without OA. S-5

6 Figure S5. TGA curves of MHPC-0.05, MHPC-0.2, and MoS2/C composites S-6

7 Figure S6. SEM images of (a, c) MHPC-0.05 and (b, d) MHPC-0.2 composites. S-7

8 Figure S7. SEM images of MoS2/C composites synthesized without SiO2 template. S-8

9 Figure S8. TEM images of (a, c) MHPC-0.05 and (b, d) MHPC-0.2 composites. S-9

10 Figure S9. (a) The nitrogen sorption isotherm of MHPC-0.05 and 0.2, and (b) their pore size distribution curves. S-10

11 Figure S10. (a) Cyclic voltammograms of bare MoS 2 at a scanning rate of 0.2 mv s -1. (b) Galvanostatic discharge/charge profiles of bare MoS 2 at 0.1 A g -1. S-11

12 Figure S11. Electrochemical performance of MHPC-0.05, 0.1 and 0.2 for LIBs (a) Long-term cycling performance at a current density of 1 A g -1 and (b) rate capability. S-12

13 Figure S12. Electrochemical impedance spectra of MHPC-0.1 and bare MoS2 electrodes in LIBs (a) before cycling and (b) after 50 cycling. S-13

14 Table S1. Atomic and mass concentration of Mo, S and C of MHPC-0.1 from high resolution XPS peak integration. Peak Position BE (ev) FWHM (ev) Atomic Mass Atomic Conc % Mass Conc % S 2p Mo 3d C 1s Table S2. Comparison of the electrochemical performance of some related composite materials for LIBs in the literature Sample Specific discharge capacity Current density Voltage windows Reference MHPC 496 ma h g A g V Our work MoS2/Carbon nanosheets 280 ma h g A g V S1 3D radially oriented MoS2 nanospheres 354 ma h g -1 2 A g V S2 CMK-3/MoS2 composites 380 ma h g -1 1 A g V S3 3D hierarchical MoS2/C 511 ma h g -1 1 A g V S4 MoS2 nanocages 680 ma h g -1 1 A g V S5 Table S3. Comparison of the electrochemical performance of some related composite materials for SIBs in the literature Sample Specific discharge capacity Current density Voltage windows Reference MHPC 293 ma h g -1 1 A g V Our work MoS2/graphene paper 173 ma h g A g V S6 MoS2/graphene synthesized via microwave 214 ma h g -1 1 A g V S7 Liquid exfoliated MoS2 120 ma h g A g V S8 MoS2/CNT 328 ma h g A g V S9 MoS2/graphene 352 ma h g A g V S10 S-14

15 Reference [S1] [S2] [S3] [S4] [S5] [S6] [S7] [S8] [S9] Zhou, J. W.; Qin, J.; Zhang, X.; Shi, C. S.; Liu, E. Z.; Li, J. J.; Zhao, N. Q.; He, C. N., 2D Space-Confined Synthesis of Few-Layer MoS2 Anchored on Carbon Nanosheet for Lithium-Ion Battery Anode. ACS Nano 2015, 9, Zhang, S. P.; Chowdari, B. V. R.; Wen, Z. Y.; Jin, J.; Yang, J. H., Constructing Highly Oriented Configuration by Few-Layer MoS2: Toward High-Performance Lithium-Ion Batteries and Hydrogen Evolution Reactions. ACS Nano 2015, 9, Xu, X.; Fan, Z. Y.; Yu, X. Y.; Ding, S. J.; Yu, D. M.; Lou, X. W., A Nanosheets-on- Channel Architecture Constructed from MoS2 and CMK-3 for High-Capacity and Long-Cycle-Life Lithium Storage. Adv. Energy Mater. 2014, 4, Hu, L. R.; Ren, Y. M.; Yang, H. X.; Xu, Q., Fabrication of 3D Hierarchical MoS2/Polyaniline and MoS2/C Architectures for Lithium-Ion Battery Applications. ACS Appl. Mater. Interfaces 2014, 6, Zuo, X. X.; Chang, K.; Zhao, J.; Xie, Z. Z.; Tang, H. W.; Li, B.; Chang, Z. R., Bubble- Template-Assisted Synthesis of Hollow Fullerene-Like MoS2 Nanocages as a Lithium Ion Battery Anode Material. J. Mater. Chem. A 2016, 4, David, L.; Bhandavat, R.; Singh, G., MoS2/Graphene Composite Paper for Sodium- Ion Battery Electrodes. ACS Nano 2014, 8, Qin, W.; Chen, T. Q.; Pan, L. K.; Niu, L. Y.; Hu, B. W.; Li, D. S.; Li, J. L.; Sun, Z., MoS2-Reduced Graphene Oxide Composites Via Microwave Assisted Synthesis for Sodium Ion Battery Anode with Improved Capacity and Cycling Performance. Electrochim. Acta 2015, 153, Bang, G. S.; Nam, K. W.; Kim, J. Y.; Shin, J.; Choi, J. W.; Choi, S. Y., Effective Liquid-Phase Exfoliation and Sodium Ion Battery Application of MoS2 Nanosheets. ACS Appl. Mater. Interfaces 2014, 6, Zhang, S.; Yu, X. B.; Yu, H. L.; Chen, Y. J.; Gao, P.; Li, C. Y.; Zhu, C. L., Growth of Ultrathin MoS2 Nanosheets with Expanded Spacing of (002) Plane on Carbon Nanotubes for High-Performance Sodium-Ion Battery Anodes. ACS Appl. Mater. Interfaces 2014, 6, [S10] Xie, X. Q.; Ao, Z. M.; Su, D. W.; Zhang, J. Q.; Wang, G. X., MoS2/Graphene Composite Anodes with Enhanced Performance for Sodium-Ion Batteries: The Role of the Two-Dimensional Heterointerface. Adv. Funct. Mater. 2015, 25, S-15

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