Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li
Poly(ethylene oxide) (PEO) was the first lithium‐ion conducting polymer developed 50 years ago and is still the most popular electrolyte matrix for solid‐state lithium metal batteries. While many studies focus on increasing PEO ionic conductivity through doping with Li salts, little work has address...
Ausführliche Beschreibung
Autor*in: |
Pei Liu [verfasserIn] Michael J. Counihan [verfasserIn] Yisi Zhu [verfasserIn] Justin G. Connell [verfasserIn] Daniel Sharon [verfasserIn] Shrayesh N. Patel [verfasserIn] Paul C. Redfern [verfasserIn] Peter Zapol [verfasserIn] Nenad M. Markovic [verfasserIn] Paul F. Nealey [verfasserIn] Larry A. Curtiss [verfasserIn] Sanja Tepavcevic [verfasserIn] |
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E-Artikel |
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Sprache: |
Englisch |
Erschienen: |
2022 |
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Übergeordnetes Werk: |
In: Advanced Energy & Sustainability Research - Wiley-VCH, 2021, 3(2022), 1, Seite n/a-n/a |
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Übergeordnetes Werk: |
volume:3 ; year:2022 ; number:1 ; pages:n/a-n/a |
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DOI / URN: |
10.1002/aesr.202100142 |
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Katalog-ID: |
DOAJ078812356 |
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520 | |a Poly(ethylene oxide) (PEO) was the first lithium‐ion conducting polymer developed 50 years ago and is still the most popular electrolyte matrix for solid‐state lithium metal batteries. While many studies focus on increasing PEO ionic conductivity through doping with Li salts, little work has addressed using PEO and Li directly to generate Li+‐conducting species in situ. Reaction between PEO and Li leads to ionic conductivity largely from Li+, in contrast to the case of added salts where the anion contribution dominates. Herein, electrochemical impedance spectroscopy shows the ionic conductivity of PEO thin films increases up to three orders of magnitude (from 10−7 to 10−4 S cm−1) when contacted with Li at elevated temperature. This is due to the reduction of ether bonds, which produces lithium alkoxides that are responsible for Li+ transport. Density functional theory analysis confirms this mechanism as thermodynamically favorable. X‐ray photoelectron spectroscopy also shows the presence of organolithium species and Li2O, which are responsible for propagating reactions with PEO and forming an electronically insulating layer at the PEO–Li interface that halts further reaction, respectively. The underlying mechanisms of Li–polymer electrolyte reactions is clarified and new pathways for in situ Li+ doping of polymer electrolytes is presented. | ||
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10.1002/aesr.202100142 doi (DE-627)DOAJ078812356 (DE-599)DOAJ0bc9bb7f45504979b864ba026423003f DE-627 ger DE-627 rakwb eng TD1-1066 TJ807-830 Pei Liu verfasserin aut Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Poly(ethylene oxide) (PEO) was the first lithium‐ion conducting polymer developed 50 years ago and is still the most popular electrolyte matrix for solid‐state lithium metal batteries. While many studies focus on increasing PEO ionic conductivity through doping with Li salts, little work has addressed using PEO and Li directly to generate Li+‐conducting species in situ. Reaction between PEO and Li leads to ionic conductivity largely from Li+, in contrast to the case of added salts where the anion contribution dominates. Herein, electrochemical impedance spectroscopy shows the ionic conductivity of PEO thin films increases up to three orders of magnitude (from 10−7 to 10−4 S cm−1) when contacted with Li at elevated temperature. This is due to the reduction of ether bonds, which produces lithium alkoxides that are responsible for Li+ transport. Density functional theory analysis confirms this mechanism as thermodynamically favorable. X‐ray photoelectron spectroscopy also shows the presence of organolithium species and Li2O, which are responsible for propagating reactions with PEO and forming an electronically insulating layer at the PEO–Li interface that halts further reaction, respectively. The underlying mechanisms of Li–polymer electrolyte reactions is clarified and new pathways for in situ Li+ doping of polymer electrolytes is presented. in situ salt formation lithium interfacial reactivities lithium metal batteries poly(ethylene oxide) spectroscopy thin films Environmental technology. Sanitary engineering Renewable energy sources Michael J. Counihan verfasserin aut Yisi Zhu verfasserin aut Justin G. Connell verfasserin aut Daniel Sharon verfasserin aut Shrayesh N. Patel verfasserin aut Paul C. Redfern verfasserin aut Peter Zapol verfasserin aut Nenad M. Markovic verfasserin aut Paul F. Nealey verfasserin aut Larry A. Curtiss verfasserin aut Sanja Tepavcevic verfasserin aut In Advanced Energy & Sustainability Research Wiley-VCH, 2021 3(2022), 1, Seite n/a-n/a (DE-627)1691219312 (DE-600)3010017-3 26999412 nnns volume:3 year:2022 number:1 pages:n/a-n/a https://doi.org/10.1002/aesr.202100142 kostenfrei https://doaj.org/article/0bc9bb7f45504979b864ba026423003f kostenfrei https://doi.org/10.1002/aesr.202100142 kostenfrei https://doaj.org/toc/2699-9412 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_267 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4012 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4367 GBV_ILN_4700 AR 3 2022 1 n/a-n/a |
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10.1002/aesr.202100142 doi (DE-627)DOAJ078812356 (DE-599)DOAJ0bc9bb7f45504979b864ba026423003f DE-627 ger DE-627 rakwb eng TD1-1066 TJ807-830 Pei Liu verfasserin aut Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Poly(ethylene oxide) (PEO) was the first lithium‐ion conducting polymer developed 50 years ago and is still the most popular electrolyte matrix for solid‐state lithium metal batteries. While many studies focus on increasing PEO ionic conductivity through doping with Li salts, little work has addressed using PEO and Li directly to generate Li+‐conducting species in situ. Reaction between PEO and Li leads to ionic conductivity largely from Li+, in contrast to the case of added salts where the anion contribution dominates. Herein, electrochemical impedance spectroscopy shows the ionic conductivity of PEO thin films increases up to three orders of magnitude (from 10−7 to 10−4 S cm−1) when contacted with Li at elevated temperature. This is due to the reduction of ether bonds, which produces lithium alkoxides that are responsible for Li+ transport. Density functional theory analysis confirms this mechanism as thermodynamically favorable. X‐ray photoelectron spectroscopy also shows the presence of organolithium species and Li2O, which are responsible for propagating reactions with PEO and forming an electronically insulating layer at the PEO–Li interface that halts further reaction, respectively. The underlying mechanisms of Li–polymer electrolyte reactions is clarified and new pathways for in situ Li+ doping of polymer electrolytes is presented. in situ salt formation lithium interfacial reactivities lithium metal batteries poly(ethylene oxide) spectroscopy thin films Environmental technology. Sanitary engineering Renewable energy sources Michael J. Counihan verfasserin aut Yisi Zhu verfasserin aut Justin G. Connell verfasserin aut Daniel Sharon verfasserin aut Shrayesh N. Patel verfasserin aut Paul C. Redfern verfasserin aut Peter Zapol verfasserin aut Nenad M. Markovic verfasserin aut Paul F. Nealey verfasserin aut Larry A. Curtiss verfasserin aut Sanja Tepavcevic verfasserin aut In Advanced Energy & Sustainability Research Wiley-VCH, 2021 3(2022), 1, Seite n/a-n/a (DE-627)1691219312 (DE-600)3010017-3 26999412 nnns volume:3 year:2022 number:1 pages:n/a-n/a https://doi.org/10.1002/aesr.202100142 kostenfrei https://doaj.org/article/0bc9bb7f45504979b864ba026423003f kostenfrei https://doi.org/10.1002/aesr.202100142 kostenfrei https://doaj.org/toc/2699-9412 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_267 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4012 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4367 GBV_ILN_4700 AR 3 2022 1 n/a-n/a |
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10.1002/aesr.202100142 doi (DE-627)DOAJ078812356 (DE-599)DOAJ0bc9bb7f45504979b864ba026423003f DE-627 ger DE-627 rakwb eng TD1-1066 TJ807-830 Pei Liu verfasserin aut Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Poly(ethylene oxide) (PEO) was the first lithium‐ion conducting polymer developed 50 years ago and is still the most popular electrolyte matrix for solid‐state lithium metal batteries. While many studies focus on increasing PEO ionic conductivity through doping with Li salts, little work has addressed using PEO and Li directly to generate Li+‐conducting species in situ. Reaction between PEO and Li leads to ionic conductivity largely from Li+, in contrast to the case of added salts where the anion contribution dominates. Herein, electrochemical impedance spectroscopy shows the ionic conductivity of PEO thin films increases up to three orders of magnitude (from 10−7 to 10−4 S cm−1) when contacted with Li at elevated temperature. This is due to the reduction of ether bonds, which produces lithium alkoxides that are responsible for Li+ transport. Density functional theory analysis confirms this mechanism as thermodynamically favorable. X‐ray photoelectron spectroscopy also shows the presence of organolithium species and Li2O, which are responsible for propagating reactions with PEO and forming an electronically insulating layer at the PEO–Li interface that halts further reaction, respectively. The underlying mechanisms of Li–polymer electrolyte reactions is clarified and new pathways for in situ Li+ doping of polymer electrolytes is presented. in situ salt formation lithium interfacial reactivities lithium metal batteries poly(ethylene oxide) spectroscopy thin films Environmental technology. Sanitary engineering Renewable energy sources Michael J. Counihan verfasserin aut Yisi Zhu verfasserin aut Justin G. Connell verfasserin aut Daniel Sharon verfasserin aut Shrayesh N. Patel verfasserin aut Paul C. Redfern verfasserin aut Peter Zapol verfasserin aut Nenad M. Markovic verfasserin aut Paul F. Nealey verfasserin aut Larry A. Curtiss verfasserin aut Sanja Tepavcevic verfasserin aut In Advanced Energy & Sustainability Research Wiley-VCH, 2021 3(2022), 1, Seite n/a-n/a (DE-627)1691219312 (DE-600)3010017-3 26999412 nnns volume:3 year:2022 number:1 pages:n/a-n/a https://doi.org/10.1002/aesr.202100142 kostenfrei https://doaj.org/article/0bc9bb7f45504979b864ba026423003f kostenfrei https://doi.org/10.1002/aesr.202100142 kostenfrei https://doaj.org/toc/2699-9412 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_267 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_4012 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4367 GBV_ILN_4700 AR 3 2022 1 n/a-n/a |
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Pei Liu misc TD1-1066 misc TJ807-830 misc in situ salt formation misc lithium interfacial reactivities misc lithium metal batteries misc poly(ethylene oxide) misc spectroscopy misc thin films misc Environmental technology. Sanitary engineering misc Renewable energy sources Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li |
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TD1-1066 TJ807-830 Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li in situ salt formation lithium interfacial reactivities lithium metal batteries poly(ethylene oxide) spectroscopy thin films |
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Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li |
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Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li |
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Poly(ethylene oxide) (PEO) was the first lithium‐ion conducting polymer developed 50 years ago and is still the most popular electrolyte matrix for solid‐state lithium metal batteries. While many studies focus on increasing PEO ionic conductivity through doping with Li salts, little work has addressed using PEO and Li directly to generate Li+‐conducting species in situ. Reaction between PEO and Li leads to ionic conductivity largely from Li+, in contrast to the case of added salts where the anion contribution dominates. Herein, electrochemical impedance spectroscopy shows the ionic conductivity of PEO thin films increases up to three orders of magnitude (from 10−7 to 10−4 S cm−1) when contacted with Li at elevated temperature. This is due to the reduction of ether bonds, which produces lithium alkoxides that are responsible for Li+ transport. Density functional theory analysis confirms this mechanism as thermodynamically favorable. X‐ray photoelectron spectroscopy also shows the presence of organolithium species and Li2O, which are responsible for propagating reactions with PEO and forming an electronically insulating layer at the PEO–Li interface that halts further reaction, respectively. The underlying mechanisms of Li–polymer electrolyte reactions is clarified and new pathways for in situ Li+ doping of polymer electrolytes is presented. |
abstractGer |
Poly(ethylene oxide) (PEO) was the first lithium‐ion conducting polymer developed 50 years ago and is still the most popular electrolyte matrix for solid‐state lithium metal batteries. While many studies focus on increasing PEO ionic conductivity through doping with Li salts, little work has addressed using PEO and Li directly to generate Li+‐conducting species in situ. Reaction between PEO and Li leads to ionic conductivity largely from Li+, in contrast to the case of added salts where the anion contribution dominates. Herein, electrochemical impedance spectroscopy shows the ionic conductivity of PEO thin films increases up to three orders of magnitude (from 10−7 to 10−4 S cm−1) when contacted with Li at elevated temperature. This is due to the reduction of ether bonds, which produces lithium alkoxides that are responsible for Li+ transport. Density functional theory analysis confirms this mechanism as thermodynamically favorable. X‐ray photoelectron spectroscopy also shows the presence of organolithium species and Li2O, which are responsible for propagating reactions with PEO and forming an electronically insulating layer at the PEO–Li interface that halts further reaction, respectively. The underlying mechanisms of Li–polymer electrolyte reactions is clarified and new pathways for in situ Li+ doping of polymer electrolytes is presented. |
abstract_unstemmed |
Poly(ethylene oxide) (PEO) was the first lithium‐ion conducting polymer developed 50 years ago and is still the most popular electrolyte matrix for solid‐state lithium metal batteries. While many studies focus on increasing PEO ionic conductivity through doping with Li salts, little work has addressed using PEO and Li directly to generate Li+‐conducting species in situ. Reaction between PEO and Li leads to ionic conductivity largely from Li+, in contrast to the case of added salts where the anion contribution dominates. Herein, electrochemical impedance spectroscopy shows the ionic conductivity of PEO thin films increases up to three orders of magnitude (from 10−7 to 10−4 S cm−1) when contacted with Li at elevated temperature. This is due to the reduction of ether bonds, which produces lithium alkoxides that are responsible for Li+ transport. Density functional theory analysis confirms this mechanism as thermodynamically favorable. X‐ray photoelectron spectroscopy also shows the presence of organolithium species and Li2O, which are responsible for propagating reactions with PEO and forming an electronically insulating layer at the PEO–Li interface that halts further reaction, respectively. The underlying mechanisms of Li–polymer electrolyte reactions is clarified and new pathways for in situ Li+ doping of polymer electrolytes is presented. |
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Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li |
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Michael J. Counihan Yisi Zhu Justin G. Connell Daniel Sharon Shrayesh N. Patel Paul C. Redfern Peter Zapol Nenad M. Markovic Paul F. Nealey Larry A. Curtiss Sanja Tepavcevic |
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