Supporting Information Controlled Pre-lithiation of Silicon Monoxide ...
Supporting Information
Controlled Pre-lithiation of Silicon Monoxide for High Performance Lithium-ion Rechargeable Full Cells HyeJin Kim,† Sunghun Choi,† Seung Jong Lee,† Myung Won Seo,‡ Jae Goo Lee,‡ Erhan Deniz,*,§ YongJu Lee,∥Eun Kyung Kim,∥ and Jang Wook Choi*,† †
Graduate School of Energy, Environment Water, and Sustainability (EEWS) and Center for
Nature-inspired Technology (CNiT) in KAIST Institute NanoCentury, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea ‡
Climate Change Research Division, Korea Institute of Energy Research (KIER), 152 Gajeong-
ro, Yuseong-gu, Daejeon 34129, Republic of Korea §
Department of Chemistry and Earth Sciences, College of Arts and Sciences, Qatar University,
P.O. Box 2713, Doha, Qatar ∥
Battery Research and Development, LG Chem, LTd., Research Park 104-1, Moonji-dong,
Yuseong-gu, Daejeon 305-380, Republic of Korea *Corresponding author e-mail: [email protected], [email protected]
S1
Calculation of the Gravimetric Energy Density of Different Types of Li-ion Battery Systems. The specific energy density (ED) of afull cell is calculated using ED =
𝐶%&'()*+ ×𝐶&.)*+ 𝑉 𝐶%&'()*+ + 𝐶&.)*+ .)12.&3
, where C indicates the capacity of cathode oranode, and V indicates the nominal voltagebetween both electrodes. Table S1 shows the theoretical values used for the calculations in Fig. 5c.
Table S1. Specific capacities and energy densitiesof various anode and cathode pairs Ccathode
Canode
Vnominal
Energy Density
[mAh g-1]
[mAh g-1]
[V]
[Wh kg-1]
LiMn2O4 / graphite
100
370
3.7
291
LiCoO2 / graphite
120
370
3.7
335
LiFePO4 / graphite
160
370
3.3
367
Li(Co1/3Ni1/3Mn1/3)O2 / graphite
160
370
3.7
413
Li(Ni0.8Co0.15Al0.05)O2 / graphite
180
370
3.7
448
Cathode / Anode Material
In the main text, energy density comparison was also providedusing experimental values of the specific capacity of c-SiOx / NCA full cell in the first discharge. The pristine c-SiOx / NCA system exhibited Ccathode = 106.33 mAh g-1, Canode = 636.69 mAh g-1, and Vnominal = 3.6 V. The pre-lithiated c-SiOx / NCA full cell showed Ccathode = 165.09 mAh g-1, Canode = 977.94 mAh g-1, and Vnominal = 3.6 V. These values yield the experimental gravimetric energy densities of 328 Wh kg-1 and 508 Wh kg-1, respectively.The experimental volumetric energy density was also calculated based on the same procedure. The densities of NCA and c-SiOx are 2.8 g cm-3 and 0.88 g cm-3, respectively. Based on these densities, the specific capacities and energy density of the pristine c-SiOx / NCA system are converted to Ccathode = 297.72 mAh cm-3, Canode = 560.29 mAh cm-3, and ED = 700 Wh L-1, respectively. By the same metric, the values of the prelithiated c-SiOx / NCA system are converted to Ccathode = 462.25 mAh cm-3, Canode = 860.89 mAh cm-3, and ED = 1083 Wh L-1, respectively.
S2
Figure S1. The process and kit for pre-lithiation. (a) The pre-lithiation kit and setting. The prelithiation kit includes a variable resistor, a switch and, a coin socket. (b) The assembly procedure of a coin cell for pre-lithiation. (c) Insertion of the assembled c-SiOx coin cell into a coin socket, followed by connection to the pre-lithiation kit and a multi-meter for voltage monitoring. (d) The dis-assembled units after pre-lithiation. The red box indicates the Li metal used for pre-lithiation, and the white dotted circle corresponds to the area that was in contact with the facing c-SiOx electrode. The Li metal and coin cell assembly are reusable.
S3
Figure S2. Comparison of cycling performance of the pristine c-SiOx half cell with (a) 10min, (b) 20min, (c) 30min, (d) 40min pre-lithiated c-SiOx half cells. 5 precyclesat 0.07C and remaining cycles at 1C.
S4
Figure S3. TOF-SIMS depth profiles of (a) normal electrochemically lithiated c-SiOx and (b) 30min pre-lithiated c-SiOx.
Figure S4. Voltage profiles of the Li[Ni0.8Co0.15Al0.05]O2 half Cell.
S5
Controlled Pre-lithiation of Silicon Monoxide for High Performance Lithium-ion Rechargeable Full Cells HyeJin Kim,† Sunghun Choi,† Seung Jong Lee,† Myung Won Seo,‡ Jae Goo Lee,‡ Erhan Deniz,*,§ YongJu Lee,∥Eun Kyung Kim,∥ and Jang Wook Choi*,† †
Graduate School of Energy, Environment Water, and Sustainability (EEWS) and Center for
Nature-inspired Technology (CNiT) in KAIST Institute NanoCentury, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea ‡
Climate Change Research Division, Korea Institute of Energy Research (KIER), 152 Gajeong-
ro, Yuseong-gu, Daejeon 34129, Republic of Korea §
Department of Chemistry and Earth Sciences, College of Arts and Sciences, Qatar University,
P.O. Box 2713, Doha, Qatar ∥
Battery Research and Development, LG Chem, LTd., Research Park 104-1, Moonji-dong,
Yuseong-gu, Daejeon 305-380, Republic of Korea *Corresponding author e-mail: [email protected], [email protected]
S1
Calculation of the Gravimetric Energy Density of Different Types of Li-ion Battery Systems. The specific energy density (ED) of afull cell is calculated using ED =
𝐶%&'()*+ ×𝐶&.)*+ 𝑉 𝐶%&'()*+ + 𝐶&.)*+ .)12.&3
, where C indicates the capacity of cathode oranode, and V indicates the nominal voltagebetween both electrodes. Table S1 shows the theoretical values used for the calculations in Fig. 5c.
Table S1. Specific capacities and energy densitiesof various anode and cathode pairs Ccathode
Canode
Vnominal
Energy Density
[mAh g-1]
[mAh g-1]
[V]
[Wh kg-1]
LiMn2O4 / graphite
100
370
3.7
291
LiCoO2 / graphite
120
370
3.7
335
LiFePO4 / graphite
160
370
3.3
367
Li(Co1/3Ni1/3Mn1/3)O2 / graphite
160
370
3.7
413
Li(Ni0.8Co0.15Al0.05)O2 / graphite
180
370
3.7
448
Cathode / Anode Material
In the main text, energy density comparison was also providedusing experimental values of the specific capacity of c-SiOx / NCA full cell in the first discharge. The pristine c-SiOx / NCA system exhibited Ccathode = 106.33 mAh g-1, Canode = 636.69 mAh g-1, and Vnominal = 3.6 V. The pre-lithiated c-SiOx / NCA full cell showed Ccathode = 165.09 mAh g-1, Canode = 977.94 mAh g-1, and Vnominal = 3.6 V. These values yield the experimental gravimetric energy densities of 328 Wh kg-1 and 508 Wh kg-1, respectively.The experimental volumetric energy density was also calculated based on the same procedure. The densities of NCA and c-SiOx are 2.8 g cm-3 and 0.88 g cm-3, respectively. Based on these densities, the specific capacities and energy density of the pristine c-SiOx / NCA system are converted to Ccathode = 297.72 mAh cm-3, Canode = 560.29 mAh cm-3, and ED = 700 Wh L-1, respectively. By the same metric, the values of the prelithiated c-SiOx / NCA system are converted to Ccathode = 462.25 mAh cm-3, Canode = 860.89 mAh cm-3, and ED = 1083 Wh L-1, respectively.
S2
Figure S1. The process and kit for pre-lithiation. (a) The pre-lithiation kit and setting. The prelithiation kit includes a variable resistor, a switch and, a coin socket. (b) The assembly procedure of a coin cell for pre-lithiation. (c) Insertion of the assembled c-SiOx coin cell into a coin socket, followed by connection to the pre-lithiation kit and a multi-meter for voltage monitoring. (d) The dis-assembled units after pre-lithiation. The red box indicates the Li metal used for pre-lithiation, and the white dotted circle corresponds to the area that was in contact with the facing c-SiOx electrode. The Li metal and coin cell assembly are reusable.
S3
Figure S2. Comparison of cycling performance of the pristine c-SiOx half cell with (a) 10min, (b) 20min, (c) 30min, (d) 40min pre-lithiated c-SiOx half cells. 5 precyclesat 0.07C and remaining cycles at 1C.
S4
Figure S3. TOF-SIMS depth profiles of (a) normal electrochemically lithiated c-SiOx and (b) 30min pre-lithiated c-SiOx.
Figure S4. Voltage profiles of the Li[Ni0.8Co0.15Al0.05]O2 half Cell.
S5
