High Salt Removal Capacity of Metal-Organic Gel Derived. Porous Carbon for Capacitive Deionization

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1 Supporting Information High Salt Removal Capacity of Metal-Organic Gel Derived Porous Carbon for Capacitive Deionization Zhuo Wang, Tingting Yan, Guorong Chen, Liyi Shi and Dengsong Zhang* Research Center of Nano Science and Technology, Shanghai University, No. 99 Shangda Road, BaoShan District, Shanghai , P. R. China *: Corresponding authors. Total No. of Pages: 9 (Pages S1-S9). Total No. of Figures: 2 (Figures S1-S2). Total No. of Tables: 2 (Table S1-S2). References: 17 (Ref S1-S6). S-1

2 Experiment section Characterization The surface morphology and structure of the as-synthesized porous carbon were observed by TEM (JEOL, JEM-200CX), SEM (JEOL, JEM-700F), and HRTEM (JEOL, JEM-2010F). XRD patterns were collected by a Rigaku D/MAX-RB with Cu Kα radiation (40 kv, 20 ma). The Raman spectra were recorded on a spectrometer (JY H800UV). Nitrogen sorption isotherms were performed on an ASAP 2020 (Micromeritics) at 77 K. The Brunauer-Emmett-Teller (BET) and nonlocal density functional methods were utilized to calculate the specific surface areas and the pore size distributions. Electrochemical measurements Electrochemical tests were performed in a conventional three-electrode system, in which the as-synthesized PC working electrode, a piece of graphite counter electrode, and a saturated calomel reference electrode were used. The working electrode was prepared by mixing the active material (80%), acetylene black (10%), and polytetrafluoroethylene (10%). The mixture was coated onto the surface of graphite paper, followed by drying in a conventional oven at 110 o C overnight. Cyclic voltammetry (CV) and electrochemical impedance spectroscope (EIS) were carried out using a CHI 660D. Galvanostatic charge-discharge was conducted on an automatic LAND battery test instrument. All measurements were conducted in a 0.5 M aqueous NaCl solution. The specific capacitance (C, in F g -1 ) was calculated based on the formula: C = ( IdV)/ 2 νδvm where I (A) and ν (V s -1 ) are the response current density and scan rate, respectively, dv (V) is the scan potential window, and m (g) is the mass of active electrode material. S-2

3 Figure S1. SEM images of PC600 (a), PC800 (b), and PC1000 (c). S-3

4 Table S1. Comparison of the specific capacitance of carbon materials reported in the literature. Electrode material solution C (F g -1 ) Ref. 3D hierarchically porous graphene 0.5 M NaCl (1 mv s -1 ) S1 Graphene/carbon nanotube composites 0.5 M NaCl 175 (1 mv s -1 ) S2 Graphene 0.5 M NaCl 106 (1 mv s -1 ) S2 sponge-templated graphene 0.5 M NaCl 57 (10 mv s -1 ) S3 3D graphene-based hierarchically porous carbon 1 M NaCl (10 mv s -1 ) S4 carbon nanotube/porous carbon polyhedra hybrid 1 M NaCl (5 mv s -1 ) S5 carbon nanotube 1 M NaCl 37.7 (5 mv s -1 ) S5 PC M NaCl (1 mv s -1 ) This work PC M NaCl 95.3 (5 mv s -1 ) This work PC M NaCl 64.2 (10 mv s -1 ) This work S-4

5 Table S2. Comparison of the salt removal capacity of various carbon materials from the literature. Applied Initial NaCl Salt adsorption Electrode material voltage concentration capacity Ref. (V) (mg/l) (mg/g) Carbon nanotubes S6 Graphene nanosheets S7 Graphene aerogel S8 Nitrogen-doped graphene S9 Mesoporous graphene S10 Purified graphene S11 3D-macroporous graphene architecture 3D-macroporous graphene hierarchically porous carbon S S4 3D-macroporous graphene S1 Carbon spheres S13 Carbon nanorods S14 3D-Graphene Architecture with Nanopores S15 3D graphene S16 Porous Carbon Spheres S17 PC This work PC This work PC This work PC This work S-5

6 Figure S2. Current transient of PC800 in different concentrations of NaCl solution at 1.4 V. S-6

7 References (S1) Wang, H.; Yan, T.; Liu, P.; Chen, G.; Shi, L.; Zhang, J.; Zhong Q.; Zhang, D. In Situ Creating Interconnected Pores across 3D Graphene Architectures and Their Application as High Performance Electrodes for Flow-Through Deionization Capacitors. J. Mater. Chem. A 2016, 4, (S2) Zhang, D. S.; Yan, T. T.; Shi, L. Y.; Peng, Z.; Wen X. R.; Zhang, J. P. Enhanced Capacitive Deionization Performance of Graphene/Carbon Nanotube Composites. J. Mater. Chem. 2012, 22, (S3) Yang, Z. Y.; Jin, L. J.; Lu, G. Q.; Xiao, Q. Q.; Zhang, Y. X.; Jing, L.; Zhang, X. X.; Yan, Y. M.; Sun, K. N. Sponge-Templated Preparation of High Surface Area Graphene with Ultrahigh Capacitive Deionization Performance. Adv. Funct. Mater. 2014, 24, (S4) Wen, X.; Zhang, D.; Yan, T.; Zhang, J.; Shi, L. Three-Dimensional Graphene-Based Hierarchically Porous Carbon Composites Prepared by a Dual-Template Strategy for Capacitive Deionization. J. Mater. Chem. A 2013, 1, (S5) Xu, X.; Li, J.; Wang, M.; Liu, Y.; Lu, T.; Pan, L. Metal-Organic Framework-Engaged Formation of a Hierarchical Hybrid with Carbon Nanotube Inserted Porous Carbon Polyhedra for Highly Efficient Capacitive Deionization. J. Mater. Chem. A 2016, 4, (S6) Li, H. B.; Lu, T.; Pan, L. K.; Zhang, Y. P.; Sun, Z. Electrosorption Behavior of Graphene in NaCl Solutions. J. Mater. Chem. 2009, 19, (S7) Jia, B. P.; Zou, L. D. Graphene Nanosheets Reduced by a Multi-Step Process as High-Performance Electrode Material for Capacitive Deionisation. Carbon 2012, 50, S-7

8 (S8) Yin, H.; Zhao, S.; Wan, J.; Tang, H.; Chang, L.; He, L.; Zhao, H.; Gao, Y.; Tang, Z. Three-Dimensional Graphene/Metal Oxide Nnanoparticle Hybrids for High-Performance Capacitive Deionization of Saline Water. Adv. Mater. 2013, 25, (S9) Xu, X.; Pan, L.; Liu, Y.; Lu, T.; Sun, Z. Enhanced Capacitive Deionization Performance of Graphene by Nitrogen Doping. J.Colloid Interf. Sci. 2015, 445, (S10) Gu, X.; Hu, M.; Du, Z.; Huang, J.; Wang, C. Fabrication of Mesoporous Graphene Electrodes with Enhanced Capacitive Deionization. Electrochim. Acta. 2015, 182, (S11) Tuan, T. N.; Chung, S.; Lee, J. K.; Lee, J. Improvement of Water Softening Efficiency in Capacitive Deionization by Ultra Purification Process of Reduced Graphene Oxide. Current Appl. Phys. 2015, 15, (S12) Wang, H.; Zhang, D.; Yan, T.; Wen, X.; Zhang, J.; Shi, L.; Zhong, Q. Three-Dimensional Macroporous Graphene Architectures as High Performance Electrodes for Capacitive Deionization. J. Mater. Chem. A 2013, 1, (S13) Liu, Y.; Pan, L. K.; Chen, T. Q.; Xu, X. T.; Lu, T.; Sun, Z.; Chua, D. H. C. Porous Carbon Spheres via Microwave-Assisted Synthesis for Capacitive Deionization. Electrochim. Acta, 2015, 151, (S14) Liu, Y.; Pan, L. K.; Xu, X. T.; Lu, T.; Sun, Z.; Chua, D. H. C. Carbon Nanorods Derived From Natural Based Nanocrystalline Cellulose for Highly Efficient Capacitive Deionization. J. Mater. Chem. A 2014, 2, (S15) Shi, W.; Li, H.; Cao, X.; Leong, Z. Y.; Zhang, J.; Chen, T.; Zhang, H.; Yang, H. Y. Ultrahigh Performance of Novel Capacitive Deionization Electrodes Based on a Three-Dimensional Graphene Architecture with Nanopores. Sci. Rep. 2016, 6, S-8

9 (S16) Liu, P.; Wang, H.; Yan, T.; Zhang, J.; Shi, L.; Zhang, D., Grafting sulfonic and amine functional groups on 3D graphene for improved capacitive deionization. J. Mater. Chem. A 2016, 4, (S17) Liu, Y.; Xu, X.; Wang, M.; Lu, T.; Sun, Z.; Pan, L., Nitrogen-doped carbon nanorods with excellent capacitive deionization ability. J. Mater. Chem. A 2015, 3, S-9

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