Supporting Information for Hydrothermally Activated Graphene Fiber Fabrics for Textile Electrodes of Supercapacitors Zheng Li, Tieqi Huang, Weiwei Gao*, Zhen Xu, Dan Chang, Chunxiao Zhang, and Chao Gao* MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering, Key Laboratory of Adsorption and Separation Materials & Technologies of Zhejiang Province, Zhejiang University, 38 Zheda Road, Hangzhou 3127, China C-OH C=O O1s GOFF HAGFF C-OH C=O 538 536 534 532 53 528 Binding energy (ev) Figure S1. XPS spectra of the deconvoluted O 1s peaks of graphene oxide fiber fabric (GOFF) and hydrothermally activated graphene fiber fabric (HAGFF). S1
Swelling degree (%) Distribution (%) Distribution (%) a 4 GOFF 1.7 1.4 m b 4 HAGFF 11.6 1.4 m 3 3 2 2 1 1 8 9 1 11 12 13 14 15 Diameter ( m) 8 9 1 11 12 13 14 15 Diameter ( m) Figure S2. The variation of fiber diameter in a) GOFF and b) HAGFF. The number at the top-right corner in each panel indicates the average fiber diameter and standard deviation correspondingly. 4 3 2 1 6 C pre-dried GO fiber 1 C pre-dried GO fiber 1 2 3 4 Time (min) Figure S3. The swelling degree of 6 C and 1 C pre-dried GO fibers versus time. S2
a 6HT12 b c d 8HT12 e f 5 μm 1 μm 1 μm 2 μm 5 μm g 8HT15 h i 1 μm 2 μm 5 μm Figure S4. Comparison of the products obtained in different activating conditions. a-c) Photos and SEM images of 6HT12. SEM images of d-f) 8HT12 and g-i) 8HT15. S3
Gravimetric energy density (Wh kg -1 ) Volumetric energy density (mwh cm -3 ) a b c 1 2 3 4 5 2 ( ) C 1s d 12 14 16 18 Wavenumbers (cm -1 ) O 1s C-C C/O=5.8 N 1s O=C-O C-O 8 6 4 2 Binding energy (ev) 292 288 284 28 Binding energy (ev) Figure S5. a) XRD, b) Raman, c) XPS and d) C 1s spectra of N 2 H 4 reduced HAGFF. 6 Gravimetric power density (W kg -1 ) 1 1 1 2 5 4 3 2 1 1 1 1 1 Volumetric power density (mw cm -3 ) Figure S6 Gravimetric and volumetric energy density and power density of the supercapacitor assembled with HAGFF electrodes. S4
Gravimetric capacitance (F g -1 ) -Z" (Ohm) -Z" (Ohm) 5 4 15 GFF HAGFF 3 2 1 1 5 5 1 15 Z' (Ohm) 1 2 3 4 5 Z' (Ohm) Figure S7. Nyquist plots of GFF and HAGFF electrodes. Inset magnifies the high-frequency range. 24 2 16 12 8 HAGFF-15 m HAGFF-13 m HAGFF-2 m 2 4 6 8 1 Current density (A g -1 ) Figure S8. Gravimetric capacitance of HAGFF electrodes with various thicknesses. S5
Areal capacitance (mf cm -2 ) Energy density ( Wh cm -2 ) a 2 b 3 15 2 1 1 5.2.4.6.8 4 6 8 Current density (ma cm -2 ) Power density ( W cm -2 ) Figure S9. a) Areal capacitance and b) Ragone plot of the all-solid-state supercapacitor. S6
Table S1. Elemental analysis of C and O in GOFF, HAGFF and N 2 H 4 reduced HAGFF. GOFF HAGFF N 2 H 4 reduced HAGFF C 64.1% 79.5% 82.2% O 32.1% 18.7% 14.2% Table S2. Comparison of the capacitance of HAGFF electrodes with previously reported carbon textile electrodes. Material Electrolyte C G [F g -1 ] C A [mf cm -2 ] Ref HAGFF 1 M H 2 SO 4 244 (.1 A g -1 ) 16 (1 ma cm -2 ) This work 231 (1 A g -1 ) 984 (1 ma cm -2 ) GFF 1 M H 2 SO 4 151 (.1 A g -1 ) 334 (1 ma cm -2 ) This work 139 (1 A g -1 ) 37 (1 ma cm -2 ) Paper+CNT+MnO 2 6 M KOH - 123 (1 ma cm -2 ) Ref 1 Graphene-cellulose paper 1 M H 2 SO 4 12 (1 mv s -1 ) 81 (1 mv s -1 ) Ref 2 Carbonized cotton mat 1 M Na 2 SO 4 -.7 (.112 ma cm -2 ) Ref 3 -.64 (.112 ma cm -2 ) N-doped carbonized cotton 1 M H 2 SO 4 27 (1 A g -1 ) - Ref 4 177 (14 A g -1 ) - Activated carbon cloth 1 M H 2 SO 4.76 (1 mv s -1 ) 76 (1 mv s -1 ) Ref 5 Electrochemically activated carbon cloth 5 M LiCl - 756 (6 ma cm -2 ) Ref 6 Carbon cloth grown with CNT.5 M Na 2 SO 4 21 (1 A g -1 ) - Ref 7 N-doped carbon nanofiber mat 2 M Li 2 SO 4 22 (.2 A g -1 ) - Ref 8 Double-capillary carbon nanofiber mat 6 M KOH 23 (1 A g -1 ) - Ref 9 - No data available in the references. S7
References (1) Dong, L.; Xu, C.; Li, Y.; Pan, Z.; Liang, G.; Zhou, E.; Kang, F.; Yang, Q.-H. Breathable and Wearable Energy Storage Based on Highly Flexible Paper Electrodes. Adv. Mater. 216, 28, 9313-9319. (2) Weng, Z.; Su, Y.; Wang, D.-W.; Li, F.; Du, J.; Cheng, H.-M. Graphene-Cellulose Paper Flexible Supercapacitors. Adv. Energy Mater. 211, 1, 917-922. (3) Xue, J.; Zhao, Y.; Cheng, H.; Hu, C.; Hu, Y.; Meng, Y.; Shao, H.; Zhang, Z.; Qu, L. An All-Cotton-Derived, Arbitrarily Foldable, High-Rate, Electrochemical Supercapacitor. Phys. Chem. Chem. Phys. 213, 15, 842-845. (4) Li, L.; Zhong, Q.; Kim, N. D.; Ruan, G.; Yang, Y.; Gao, C.; Fei, H.; Li, Y.; Ji, Y.; Tour, J. M. Nitrogen-Doped Carbonized Cotton for Highly Flexible Supercapacitors. Carbon 216, 15, 26-267. (5) Wang, G.; Wang, H.; Lu, X.; Ling, Y.; Yu, M.; Zhai, T.; Tong, Y.; Li, Y. Solid-State Supercapacitor Based on Activated Carbon Cloths Exhibits Excellent Rate Capability. Adv. Mater. 214, 26, 2676-2682. (6) Wang, W.; Liu, W.; Zeng, Y.; Han, Y.; Yu, M.; Lu, X.; Tong, Y. A Novel Exfoliation Strategy to Significantly Boost the Energy Storage Capability of Commercial Carbon Cloth. Adv. Mater. 215, 27, 3572-3578. (7) Hsu, Y.-K.; Chen, Y.-C.; Lin, Y.-G.; Chen, L.-C.; Chen, K.-H. High-Cell-Voltage Supercapacitor of Carbon Nanotube/Carbon Cloth Operating in Neutral Aqueous Solution. J. Mater. Chem. 212, 22, 3383-3387. (8) Liang, Q.; Ye, L.; Xu, Q.; Huang, Z.-H.; Kang, F.; Yang, Q.-H. Graphitic Carbon Nitride Nanosheet-Assisted Preparation of N-Enriched Mesoporous Carbon Nanofibers S8
with Improved Capacitive Performance. Carbon 215, 94, 342-348. (9) Wang, J.; Tang, J.; Xu, Y.; Ding, B.; Chang, Z.; Wang, Y.; Hao, X.; Dou, H.; Kim, J. H.; Zhang, X.; Yamauchi, Y. Interface Miscibility Induced Double-Capillary Carbon Nanofibers for Flexible Electric Double Layer Capacitors. Nano Energy 216, 28, 232-24. S9