Antimony/Graphitic Carbon Composite Anode for High- Performance Sodium-Ion Batteries

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1 Supporting Information Antimony/Graphitic Carbon Composite Anode for High- Performance Sodium-Ion Batteries Xin Zhao, Sean A. Vail, Yuhao Lu *, Jie Song, Wei Pan, David R. Evans, Jong-Jan Lee Sharp Laboratories of America, Camas, WA 9867, USA * S-1

2 Table S1. Cost estimation of Sb/graphite composite powders. Figure S1. SEM images of (a)(b) EG powders and (c)(d) J-SP-α powders. Figure S2. SEM images taken on the surface of Sb/graphite composite anode films: (a) Sb/EG and (b) Sb/J-SP-α composite films. The particle size and agglomerations are highlighted. Figure S3. Galvanostatic charge/discharge profiles of (a) expanded graphite anode and (b) J-SPα graphite anode evaluated at a charge/discharge current density of.1c (25 ma/g). The reversible capacity of EG and J-SP-α was 5.3 and.5 mah/g, respectively. Figure S4. Capacity retention of Sb/EG, Sb/J-SP-α and Sb/carbon black anodes as a function of charge/discharge current density. Figure S5. Electrochemical performance of hard carbon anode in half cells: (a) specific desodiation capacities and coulombic efficiencies evaluated between.5-2. V at charge/discharge current densities of.1c-2c (1C based on a theoretical capacity of 25 mah/g); (b) specific desodiation capacities and coulombic efficiencies evaluated between.5-2. V at constant discharge current densities of.1c/1c and charge current densities of.1c- 2C (charge current densities are labeled). Table S2. Comparison of the electrochemical performance of Sb-based anode reported in this work and the literature. Figure S6. Specific desodiation capacities and coulombic efficiencies of Sb/EG, Sb/J-SP-α and hard carbon anodes on C/Al current collector evaluated between.2-2. V at charge/discharge current densities of.1c-2c. Figure S7. (a) Galvanostatic charge/discharge profiles of Sb/EG anode evaluated at charge/discharge current densities of.1c-2c; (b) galvanostatic charge/discharge profiles of Sb/EG anode evaluated at constant discharge current densities of.1c/1c and various charge current densities of.1c-2c. Figure S8. Specific desodiation capacities and coulombic efficiencies of Sb/J-SP-α anode with two active mass loadings (1.3 and 2.5 mg/cm 2 ) on Cu current collector. Samples were evaluated between.2-2. V at charge/discharge current densities of.1c-2c. Figure S9. Specific desodiation capacities and coulombic efficiencies of Sb/J-SP-α anode with two active mass loadings (1.3 and 2.5 mg/cm 2 ) on C/Al current collector. Samples were evaluated between.2-2. V at charge/discharge current densities of.1c-2c. S-2

3 Figure S1. (a) Galvanostatic charge/discharge profiles of hard carbon anode evaluated at charge/discharge current densities of.1c-2c; (b) galvanostatic charge/discharge profiles of hard carbon anode evaluated at constant discharge current densities of.1c/1c at charge current densities of.1c-2c. Figure S11. Cycle life evaluation of Sb/EG and Sb/J-SP-α anodes at a constant current density of 4C. Figure S12. Digital images of cycled electrodes: comparison of the surface appearances of Sb composite and hard carbon anodes following evaluation in full cells. S-3

4 Table S1. Cost estimation of Sb/graphite composite powders. RAW MATERIALS COST PER KG ~325 mesh Sb powder $12 EG flake $1 J-SP-α flake $5 Ball mill process 1 Electricity $7.2 2 NMP $3 SUM COST Sb/EG $2 per kg SUM COST Sb/J-SP-α $17 per kg 1. Total output of each single batch was 32 g of Sb powders (pre-milling) and 5 g Sb/graphite composite powders. 2. A single ball milling experiment consumed 45 kwh of electricity, at a local electricity unit price of $.8 USD per kwh. S-4

5 Figure S1. SEM images of (a)(b) EG powders and (c)(d) J-SP-α powders. Figure S2. SEM images taken on the surface of Sb/graphite composite anode films: (a) Sb/EG and (b) Sb/J-SP-α composite films. The particle size and agglomerations are highlighted. S-5

6 Figure S3. Galvanostatic charge/discharge profiles of (a) expanded graphite anode and (b) J-SPα graphite anode evaluated at a charge/discharge current density of.1c (25 ma/g). The reversible capacity of EG and J-SP-α was 5.3 and.5 mah/g, respectively. S-6

7 Figure S4. Capacity retention of Sb/EG, Sb/J-SP-α and Sb/carbon black anodes as a function of charge/discharge current density. S-7

8 Figure S5. Electrochemical performance of hard carbon anode in half cells: (a) specific desodiation capacities and coulombic efficiencies evaluated between.5-2. V at charge/discharge current densities of.1c-2c (1C based on a theoretical capacity of 25 mah/g); (b) specific desodiation capacities and coulombic efficiencies evaluated between.5-2. V at constant discharge current densities of.1c/1c and charge current densities of.1c- 2C (charge current densities are labeled). S-8

9 Table S2. Comparison of the electrochemical performance of Sb-based anode reported in this work and the literature. Data Electrode composition Loading Cycle life source (weight ratio) Rate This work BM 1.5 mg/cm 2 31 mah/g ~1% retention at 16 Sb/graphite/CB/NaA at.1c cycles (.1C) 51/34/5/1 2 mah/g >9% retention at 16 at 2C cycles (1C) Ref. 32 BM Sb 1.4 mg/cm mah/g >9% retention at 14- particle/cb+carbon at.5c 16 cycles (.5C-2C) fiber/cmc 7/15/ mah/g at 2C Ref nm Sb/CB/CMC 64/21/15 1. mg/cm 2 6 mah/g at.5c ~1% retention at 1 cycles (.5C-2C) 5 mah/g at 2C Ref. 35 SnSb/carbon nanofiber/cb/cmc mg 392 mah/g at.1c ~1% retention at 2 cycles (.2C) 48/32/1/1 113 mah/g at 2C Ref nm Sb/CB/CMC 56/34/1 3.3 mg/cm 2 61 mah/g at.22c >9% retention at 1 cycles (.27C) 39 mah/g at 4.3C Ref. 37 Electrospun Sb NP/carbon fiber 3 mg 32 mah/g at.1c >8% retention at 3 cycles (.28C-5.6C) 54/46 1 mah/g at 17C Ref. 47 Sb hollow Not 622 mah/g ~1% retention at 5 S-9

10 nanosphere/cb/cmc provided at.75c cycles (.75C) 7/15/ mah/g at 2.4C Ref. 48 Sb porous hollow mg 617 mah/g ~97% retention at 1 microsphere/cb/cmc at.15c cycles (.15C) 7/15/ mah/g ~87% retention at 1 at 4.8C cycles (1C) Ref. 49 SnSb/CB/CMC Not 52 mah/g ~8% retention at 5 56/34/1 provided at.19c cycles (.19C) 3 mah/g at 1.9C S-1

11 Specific Capacity (mah/g) C.2C.4C 1C 2C 4C Sb/EG Sb/J-SP-a Hard Carbon 1C 2C C Coulombic Efficiency (%) Cycle Number Figure S6. Specific desodiation capacities and coulombic efficiencies of Sb/EG, Sb/J-SP-α and hard carbon anodes on C/Al current collector evaluated between.2-2. V at charge/discharge current densities of.1c-2c. Figure S7. (a) Galvanostatic charge/discharge profiles of Sb/EG anode evaluated at charge/discharge current densities of.1c-2c; (b) galvanostatic charge/discharge profiles of Sb/EG anode evaluated at constant discharge current densities of.1c/1c and various charge current densities of.1c-2c. S-11

12 Specific Capacity (mah/g) C.2C.4C 1C 2C 4C 1C 2C Sb/J-SP-a 1.3 mg/cm 2 Sb/J-SP-a 2.5 mg/cm Coulombic Efficiency (%) Cycle Number Figure S8. Specific desodiation capacities and coulombic efficiencies of Sb/J-SP-α anode with two active mass loadings (1.3 and 2.5 mg/cm 2 ) on Cu current collector. Samples were evaluated between.2-2. V at charge/discharge current densities of.1c-2c. S-12

13 Specific Capacity (mah/g) C.2C.4C 1C 2C Sb/J-SP-a 1.3 mg/cm 2 Sb/J-SP-a 2.5 mg/cm 2 4C 1C 2C Coulombic Efficiency (%) Cycle Number Figure S9. Specific desodiation capacities and coulombic efficiencies of Sb/J-SP-α anode with two active mass loadings (1.3 and 2.5 mg/cm 2 ) on C/Al current collector. Samples were evaluated between.2-2. V at charge/discharge current densities of.1c-2c. S-13

14 Figure S1. (a) Galvanostatic charge/discharge profiles of hard carbon anode evaluated at charge/discharge current densities of.1c-2c; (b) galvanostatic charge/discharge profiles of hard carbon anode evaluated at constant discharge current densities of.1c/1c at charge current densities of.1c-2c. Specific Capacity (mah/g) Sb/EG 4C Sb/J-SP-a 4C Cycle Number Coulombic Efficiency (%) Figure S11. Cycle life evaluation of Sb/EG and Sb/J-SP-α anodes at a constant current density of 4C. S-14

15 Figure S12. Digital images of cycled electrodes: comparison of the surface appearances of Sb composite and hard carbon anodes following evaluation in full cells. S-15

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