Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries
Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO 2 (-ACl)-A 2 ZrCl 6 (A = Li or Na) that demonstrate improved i...
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Published in | Nature communications Vol. 14; no. 1; p. 2459 |
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Main Authors | , , , , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
London
Nature Publishing Group UK
28.04.2023
Nature Publishing Group Nature Portfolio |
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Abstract | Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO
2
(-ACl)-A
2
ZrCl
6
(A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm
−1
and from 0.011 to 0.11 mS cm
−1
for Li
+
and Na
+
, respectively, compared to A
2
ZrCl
6
, and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li
2
O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and
6
Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li
2
ZrCl
6
, the fluorinated ZrO
2
−2Li
2
ZrCl
5
F HNSE shows improved high-voltage stability and interfacial compatibility with Li
6
PS
5
Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li
+
conductivity. We also report the assembly and testing of a Li-In||LiNi
0.88
Co
0.11
Mn
0.01
O
2
all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g
−1
after almost 2000 cycles at 400 mA g
−1
.
Compositional tuning is a standard procedure to improve the ionic conductivity of inorganic superionic conductors. Here, the authors report (electro)chemical stable composite halide solid electrolytes applying a nanostructure approach that promotes interfacial superionic conductivity. |
---|---|
AbstractList | Abstract
Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO
2
(-ACl)-A
2
ZrCl
6
(A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm
−1
and from 0.011 to 0.11 mS cm
−1
for Li
+
and Na
+
, respectively, compared to A
2
ZrCl
6
, and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li
2
O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and
6
Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li
2
ZrCl
6
, the fluorinated ZrO
2
−2Li
2
ZrCl
5
F HNSE shows improved high-voltage stability and interfacial compatibility with Li
6
PS
5
Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li
+
conductivity. We also report the assembly and testing of a Li-In||LiNi
0.88
Co
0.11
Mn
0.01
O
2
all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g
−1
after almost 2000 cycles at 400 mA g
−1
. Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO 2 (-ACl)-A 2 ZrCl 6 (A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm −1 and from 0.011 to 0.11 mS cm −1 for Li + and Na + , respectively, compared to A 2 ZrCl 6 , and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li 2 O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and 6 Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li 2 ZrCl 6 , the fluorinated ZrO 2 −2Li 2 ZrCl 5 F HNSE shows improved high-voltage stability and interfacial compatibility with Li 6 PS 5 Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li + conductivity. We also report the assembly and testing of a Li-In||LiNi 0.88 Co 0.11 Mn 0.01 O 2 all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g −1 after almost 2000 cycles at 400 mA g −1 . Compositional tuning is a standard procedure to improve the ionic conductivity of inorganic superionic conductors. Here, the authors report (electro)chemical stable composite halide solid electrolytes applying a nanostructure approach that promotes interfacial superionic conductivity. Abstract Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO2(-ACl)-A2ZrCl6 (A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm−1 and from 0.011 to 0.11 mS cm−1 for Li+ and Na+, respectively, compared to A2ZrCl6, and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li2O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and 6Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li2ZrCl6, the fluorinated ZrO2−2Li2ZrCl5F HNSE shows improved high-voltage stability and interfacial compatibility with Li6PS5Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li+ conductivity. We also report the assembly and testing of a Li-In||LiNi0.88Co0.11Mn0.01O2 all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g−1 after almost 2000 cycles at 400 mA g−1. Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO2(-ACl)-A2ZrCl6 (A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm-1 and from 0.011 to 0.11 mS cm-1 for Li+ and Na+, respectively, compared to A2ZrCl6, and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li2O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and 6Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li2ZrCl6, the fluorinated ZrO2-2Li2ZrCl5F HNSE shows improved high-voltage stability and interfacial compatibility with Li6PS5Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li+ conductivity. We also report the assembly and testing of a Li-In||LiNi0.88Co0.11Mn0.01O2 all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g-1 after almost 2000 cycles at 400 mA g-1. Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO (-ACl)-A ZrCl (A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm and from 0.011 to 0.11 mS cm for Li and Na , respectively, compared to A ZrCl , and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li ZrCl , the fluorinated ZrO -2Li ZrCl F HNSE shows improved high-voltage stability and interfacial compatibility with Li PS Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li conductivity. We also report the assembly and testing of a Li-In||LiNi Co Mn O all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g after almost 2000 cycles at 400 mA g . Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO2(-ACl)-A2ZrCl6 (A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm−1 and from 0.011 to 0.11 mS cm−1 for Li+ and Na+, respectively, compared to A2ZrCl6, and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li2O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and 6Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li2ZrCl6, the fluorinated ZrO2−2Li2ZrCl5F HNSE shows improved high-voltage stability and interfacial compatibility with Li6PS5Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li+ conductivity. We also report the assembly and testing of a Li-In||LiNi0.88Co0.11Mn0.01O2 all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g−1 after almost 2000 cycles at 400 mA g−1.Compositional tuning is a standard procedure to improve the ionic conductivity of inorganic superionic conductors. Here, the authors report (electro)chemical stable composite halide solid electrolytes applying a nanostructure approach that promotes interfacial superionic conductivity. |
ArticleNumber | 2459 |
Author | Park, Changhyun Kim, Jae-Seung Nam, Kyung-Wan Kwon, Gihan Lee, Hyun-Wook Jung, Yoon Seok Han, Daseul Kim, Jong Seok Heo, Unseon Park, Juhyoun Kwak, Hiram Bak, Seong-Min Seo, Dong-Hwa |
Author_xml | – sequence: 1 givenname: Hiram surname: Kwak fullname: Kwak, Hiram organization: Department of Chemical and Biomolecular Engineering, Yonsei University – sequence: 2 givenname: Jae-Seung surname: Kim fullname: Kim, Jae-Seung organization: School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST) – sequence: 3 givenname: Daseul surname: Han fullname: Han, Daseul organization: Department of Energy and Materials Engineering, Dongguk University – sequence: 4 givenname: Jong Seok surname: Kim fullname: Kim, Jong Seok organization: Department of Chemical and Biomolecular Engineering, Yonsei University – sequence: 5 givenname: Juhyoun surname: Park fullname: Park, Juhyoun organization: Department of Chemical and Biomolecular Engineering, Yonsei University – sequence: 6 givenname: Gihan orcidid: 0000-0002-7963-2136 surname: Kwon fullname: Kwon, Gihan organization: National Synchrotron Light Source II, Brookhaven National Laboratory – sequence: 7 givenname: Seong-Min orcidid: 0000-0002-1626-5949 surname: Bak fullname: Bak, Seong-Min organization: National Synchrotron Light Source II, Brookhaven National Laboratory, Department of Materials Science and Engineering, Yonsei University – sequence: 8 givenname: Unseon surname: Heo fullname: Heo, Unseon organization: Department of Energy and Materials Engineering, Dongguk University – sequence: 9 givenname: Changhyun orcidid: 0000-0003-1269-7581 surname: Park fullname: Park, Changhyun organization: School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST) – sequence: 10 givenname: Hyun-Wook orcidid: 0000-0001-9074-1619 surname: Lee fullname: Lee, Hyun-Wook organization: School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST) – sequence: 11 givenname: Kyung-Wan orcidid: 0000-0001-6278-6369 surname: Nam fullname: Nam, Kyung-Wan email: knam@dongguk.edu organization: Department of Energy and Materials Engineering, Dongguk University – sequence: 12 givenname: Dong-Hwa orcidid: 0000-0002-7200-7186 surname: Seo fullname: Seo, Dong-Hwa email: dseo@unist.ac.kr organization: School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST) – sequence: 13 givenname: Yoon Seok orcidid: 0000-0003-0357-9508 surname: Jung fullname: Jung, Yoon Seok email: yoonsjung@yonsei.ac.kr organization: Department of Chemical and Biomolecular Engineering, Yonsei University |
BackLink | https://www.ncbi.nlm.nih.gov/pubmed/37117172$$D View this record in MEDLINE/PubMed https://www.osti.gov/servlets/purl/1988606$$D View this record in Osti.gov |
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Snippet | Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state... Abstract Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing... Abstract Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing... |
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Title | Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries |
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