An Inorganic‐Rich Solid Electrolyte Interphase for Advanced Lithium‐Metal Batteries in Carbonate Electrolytes
In carbonate electrolytes, the organic–inorganic solid electrolyte interphase (SEI) formed on the Li‐metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic‐rich S...
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| Published in | Angewandte Chemie International Edition Vol. 60; no. 7; pp. 3661 - 3671 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Germany
Wiley Subscription Services, Inc
15.02.2021
|
| Edition | International ed. in English |
| Subjects | |
| Online Access | Get full text |
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| Abstract | In carbonate electrolytes, the organic–inorganic solid electrolyte interphase (SEI) formed on the Li‐metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic‐rich SEI is designed on a Li‐metal surface to reduce its bonding energy with Li metal by dissolving 4m concentrated LiNO3 in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene‐carbonate (FEC)‐based electrolyte. Due to the aggregate structure of NO3− ions and their participation in the primary Li+ solvation sheath, abundant Li2O, Li3N, and LiNxOy grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF6− ions. The weak bonding of the SEI (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping Coulombic efficiency of 99.55 % (1 mA cm−2, 1.0 mAh cm−2) and the electrolyte also enables a Li||LiNi0.8Co0.1Mn0.1O2 (NMC811) full cell (2.5 mAh cm−2) to retain 75 % of its initial capacity after 200 cycles with an outstanding CE of 99.83 %.
An inorganic‐rich solid electrolyte interphase (SEI) has been constructed on Li metal to promote dense Li growth with a Coulombic efficiency of 99.55 % in the carbonate electrolyte. It was synthesized on the surface of the Li‐metal anode using concentrated LiNO3 in dimethyl sulfoxide (DMSO) as an additive in the FEC‐based electrolyte, which participates in the primary Li+ solvation shell and promotes the reduction of NO3− ions to form the inorganic‐rich SEI. |
|---|---|
| AbstractList | In carbonate electrolytes, the organic–inorganic solid electrolyte interphase (SEI) formed on the Li‐metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic‐rich SEI is designed on a Li‐metal surface to reduce its bonding energy with Li metal by dissolving 4
m
concentrated LiNO
3
in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene‐carbonate (FEC)‐based electrolyte. Due to the aggregate structure of NO
3
−
ions and their participation in the primary Li
+
solvation sheath, abundant Li
2
O, Li
3
N, and LiN
x
O
y
grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF
6
−
ions. The weak bonding of the SEI (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping Coulombic efficiency of 99.55 % (1 mA cm
−2
, 1.0 mAh cm
−2
) and the electrolyte also enables a Li||LiNi
0.8
Co
0.1
Mn
0.1
O
2
(NMC811) full cell (2.5 mAh cm
−2
) to retain 75 % of its initial capacity after 200 cycles with an outstanding CE of 99.83 %. In carbonate electrolytes, the organic-inorganic solid electrolyte interphase (SEI) formed on the Li-metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic-rich SEI is designed on a Li-metal surface to reduce its bonding energy with Li metal by dissolving 4m concentrated LiNO in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene-carbonate (FEC)-based electrolyte. Due to the aggregate structure of NO ions and their participation in the primary Li solvation sheath, abundant Li O, Li N, and LiN O grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF ions. The weak bonding of the SEI (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping Coulombic efficiency of 99.55 % (1 mA cm , 1.0 mAh cm ) and the electrolyte also enables a Li||LiNi Co Mn O (NMC811) full cell (2.5 mAh cm ) to retain 75 % of its initial capacity after 200 cycles with an outstanding CE of 99.83 %. In carbonate electrolytes, the organic-inorganic solid electrolyte interphase (SEI) formed on the Li-metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic-rich SEI is designed on a Li-metal surface to reduce its bonding energy with Li metal by dissolving 4m concentrated LiNO3 in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene-carbonate (FEC)-based electrolyte. Due to the aggregate structure of NO3 - ions and their participation in the primary Li+ solvation sheath, abundant Li2 O, Li3 N, and LiNx Oy grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF6 - ions. The weak bonding of the SEI (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping Coulombic efficiency of 99.55 % (1 mA cm-2 , 1.0 mAh cm-2 ) and the electrolyte also enables a Li||LiNi0.8 Co0.1 Mn0.1 O2 (NMC811) full cell (2.5 mAh cm-2 ) to retain 75 % of its initial capacity after 200 cycles with an outstanding CE of 99.83 %.In carbonate electrolytes, the organic-inorganic solid electrolyte interphase (SEI) formed on the Li-metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic-rich SEI is designed on a Li-metal surface to reduce its bonding energy with Li metal by dissolving 4m concentrated LiNO3 in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene-carbonate (FEC)-based electrolyte. Due to the aggregate structure of NO3 - ions and their participation in the primary Li+ solvation sheath, abundant Li2 O, Li3 N, and LiNx Oy grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF6 - ions. The weak bonding of the SEI (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping Coulombic efficiency of 99.55 % (1 mA cm-2 , 1.0 mAh cm-2 ) and the electrolyte also enables a Li||LiNi0.8 Co0.1 Mn0.1 O2 (NMC811) full cell (2.5 mAh cm-2 ) to retain 75 % of its initial capacity after 200 cycles with an outstanding CE of 99.83 %. In carbonate electrolytes, the organic–inorganic solid electrolyte interphase (SEI) formed on the Li‐metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic‐rich SEI is designed on a Li‐metal surface to reduce its bonding energy with Li metal by dissolving 4m concentrated LiNO3 in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene‐carbonate (FEC)‐based electrolyte. Due to the aggregate structure of NO3− ions and their participation in the primary Li+ solvation sheath, abundant Li2O, Li3N, and LiNxOy grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF6− ions. The weak bonding of the SEI (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping Coulombic efficiency of 99.55 % (1 mA cm−2, 1.0 mAh cm−2) and the electrolyte also enables a Li||LiNi0.8Co0.1Mn0.1O2 (NMC811) full cell (2.5 mAh cm−2) to retain 75 % of its initial capacity after 200 cycles with an outstanding CE of 99.83 %. In carbonate electrolytes, the organic–inorganic solid electrolyte interphase (SEI) formed on the Li‐metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic‐rich SEI is designed on a Li‐metal surface to reduce its bonding energy with Li metal by dissolving 4m concentrated LiNO3 in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene‐carbonate (FEC)‐based electrolyte. Due to the aggregate structure of NO3− ions and their participation in the primary Li+ solvation sheath, abundant Li2O, Li3N, and LiNxOy grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF6− ions. The weak bonding of the SEI (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping Coulombic efficiency of 99.55 % (1 mA cm−2, 1.0 mAh cm−2) and the electrolyte also enables a Li||LiNi0.8Co0.1Mn0.1O2 (NMC811) full cell (2.5 mAh cm−2) to retain 75 % of its initial capacity after 200 cycles with an outstanding CE of 99.83 %. An inorganic‐rich solid electrolyte interphase (SEI) has been constructed on Li metal to promote dense Li growth with a Coulombic efficiency of 99.55 % in the carbonate electrolyte. It was synthesized on the surface of the Li‐metal anode using concentrated LiNO3 in dimethyl sulfoxide (DMSO) as an additive in the FEC‐based electrolyte, which participates in the primary Li+ solvation shell and promotes the reduction of NO3− ions to form the inorganic‐rich SEI. |
| Author | Piao, Nan Wang, Chunsheng Jin, Ting Deng, Tao Eidson, Nico Wan, Hongli Li, Jingru Chen, Ji Hou, Singyuk Ji, Xiao Liu, Sufu Chen, Long Tu, Jiangping Xu, Jijian Wang, Pengfei Zhang, Jiaxun |
| Author_xml | – sequence: 1 givenname: Sufu surname: Liu fullname: Liu, Sufu organization: University of Maryland – sequence: 2 givenname: Xiao surname: Ji fullname: Ji, Xiao organization: University of Maryland – sequence: 3 givenname: Nan surname: Piao fullname: Piao, Nan organization: University of Maryland – sequence: 4 givenname: Ji surname: Chen fullname: Chen, Ji organization: University of Maryland – sequence: 5 givenname: Nico surname: Eidson fullname: Eidson, Nico organization: University of Maryland – sequence: 6 givenname: Jijian surname: Xu fullname: Xu, Jijian organization: University of Maryland – sequence: 7 givenname: Pengfei surname: Wang fullname: Wang, Pengfei organization: University of Maryland – sequence: 8 givenname: Long surname: Chen fullname: Chen, Long organization: University of Maryland – sequence: 9 givenname: Jiaxun surname: Zhang fullname: Zhang, Jiaxun organization: University of Maryland – sequence: 10 givenname: Tao surname: Deng fullname: Deng, Tao organization: University of Maryland – sequence: 11 givenname: Singyuk surname: Hou fullname: Hou, Singyuk organization: University of Maryland – sequence: 12 givenname: Ting surname: Jin fullname: Jin, Ting organization: University of Maryland – sequence: 13 givenname: Hongli surname: Wan fullname: Wan, Hongli organization: University of Maryland – sequence: 14 givenname: Jingru surname: Li fullname: Li, Jingru organization: Zhejiang University – sequence: 15 givenname: Jiangping surname: Tu fullname: Tu, Jiangping organization: Zhejiang University – sequence: 16 givenname: Chunsheng orcidid: 0000-0002-8626-6381 surname: Wang fullname: Wang, Chunsheng email: cswang@umd.edu organization: University of Maryland |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/33166432$$D View this record in MEDLINE/PubMed |
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| Snippet | In carbonate electrolytes, the organic–inorganic solid electrolyte interphase (SEI) formed on the Li‐metal anode surface is strongly bonded to Li and... In carbonate electrolytes, the organic-inorganic solid electrolyte interphase (SEI) formed on the Li-metal anode surface is strongly bonded to Li and... |
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| SubjectTerms | Anodes Batteries Bonding strength carbonate electrolytes dendrite-free structures Dendritic structure Dimethyl sulfoxide electrode interphases Electrolytes Interphase Ions Lithium Lithium fluoride lithium nitrate Lithium oxides lithium-metal batteries Metal surfaces Metals Molten salt electrolytes Plating Sheaths Solid electrolytes Solvation Stripping |
| Title | An Inorganic‐Rich Solid Electrolyte Interphase for Advanced Lithium‐Metal Batteries in Carbonate Electrolytes |
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