Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte

Ester-based electrolytes, known for their cost-effectiveness and wide voltage windows, face compatibility challenges with lithium metal (Li<sup>0</sup>), leading to irreversible decomposition and dendrite growth, which impede their application in high-energy-density lithium metal batteri...

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Main Author: Baogang Zhao (19139738) (author)
Other Authors: Nuttapon Yodsin (6760856) (author), Haoyu Ma (12190828) (author), Phornphimon Maitarad (1417432) (author), Wanwisa Limphirat (5474471) (author), Zhuobin Han (21463654) (author), Yinghao Zhou (10106450) (author), Mengjia Yu (19139732) (author), Kexin Liu (1547230) (author), Bingqing Yan (8531742) (author), Xiaoyang Zhao (280499) (author), Guorong Chen (1805383) (author), Xin Feng (111466) (author), Rongrong Jia (2220763) (author), Liyi Shi (1366401) (author), Shuai Yuan (305841) (author), Yingying Lv (1645591) (author)
Published: 2025
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_version_ 1852019790558789632
author Baogang Zhao (19139738)
author2 Nuttapon Yodsin (6760856)
Haoyu Ma (12190828)
Phornphimon Maitarad (1417432)
Wanwisa Limphirat (5474471)
Zhuobin Han (21463654)
Yinghao Zhou (10106450)
Mengjia Yu (19139732)
Kexin Liu (1547230)
Bingqing Yan (8531742)
Xiaoyang Zhao (280499)
Guorong Chen (1805383)
Xin Feng (111466)
Rongrong Jia (2220763)
Liyi Shi (1366401)
Shuai Yuan (305841)
Yingying Lv (1645591)
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author_facet Baogang Zhao (19139738)
Nuttapon Yodsin (6760856)
Haoyu Ma (12190828)
Phornphimon Maitarad (1417432)
Wanwisa Limphirat (5474471)
Zhuobin Han (21463654)
Yinghao Zhou (10106450)
Mengjia Yu (19139732)
Kexin Liu (1547230)
Bingqing Yan (8531742)
Xiaoyang Zhao (280499)
Guorong Chen (1805383)
Xin Feng (111466)
Rongrong Jia (2220763)
Liyi Shi (1366401)
Shuai Yuan (305841)
Yingying Lv (1645591)
author_role author
dc.creator.none.fl_str_mv Baogang Zhao (19139738)
Nuttapon Yodsin (6760856)
Haoyu Ma (12190828)
Phornphimon Maitarad (1417432)
Wanwisa Limphirat (5474471)
Zhuobin Han (21463654)
Yinghao Zhou (10106450)
Mengjia Yu (19139732)
Kexin Liu (1547230)
Bingqing Yan (8531742)
Xiaoyang Zhao (280499)
Guorong Chen (1805383)
Xin Feng (111466)
Rongrong Jia (2220763)
Liyi Shi (1366401)
Shuai Yuan (305841)
Yingying Lv (1645591)
dc.date.none.fl_str_mv 2025-06-02T16:09:38Z
dc.identifier.none.fl_str_mv 10.1021/acsnano.5c03410.s002
dc.relation.none.fl_str_mv https://figshare.com/articles/media/Fully_Lithiated_Li_sub_i_x_i_sub_TiO_sub_2_sub_Layer_Coated_Separator_for_Securing_a_Lithium-less_Anode_in_an_Ester-Based_Electrolyte/29213050
dc.rights.none.fl_str_mv CC BY-NC 4.0
info:eu-repo/semantics/openAccess
dc.subject.none.fl_str_mv Biochemistry
Medicine
Developmental Biology
Plant Biology
Chemical Sciences not elsewhere classified
wide voltage windows
solid electrolyte interface
face compatibility challenges
average coulombic efficiency
electrochemical prelithiation strategy
promoting uniform li
fully lithiated li
avg </ sub
layer coated separator
based electrolyte ester
0 </ sup
x </
effective strategy
coated polypropylene
based electrolytes
limited li
li anodes
work provides
work develops
sub ><
side reaction
oxygen vacancies
nmc811 cathodes
maintain 90
lmbs ).
irreversible decomposition
generation lmbs
full cells
free cu
dendrite growth
cycling stability
contact area
capacity retention
areal capacity
></ sub
85 %.
60 cycles
40 μm
100 cycles
dc.title.none.fl_str_mv Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte
dc.type.none.fl_str_mv Dataset
Media
info:eu-repo/semantics/publishedVersion
dataset
description Ester-based electrolytes, known for their cost-effectiveness and wide voltage windows, face compatibility challenges with lithium metal (Li<sup>0</sup>), leading to irreversible decomposition and dendrite growth, which impede their application in high-energy-density lithium metal batteries (LMBs). This work develops an electrochemical prelithiation strategy to obtain a fully lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> coated polypropylene (PP) separator with oxygen vacancies, preventing the depletion of limited Li<sup>0</sup> resources while promoting uniform Li<sup>0</sup> plating. Moreover, the dense closest packing structure of Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> can reduce the contact area and side reaction between Li<sup>0</sup> and ester-based electrolytes, stabilizing the solid electrolyte interface (SEI) on Li<sup>0</sup>. Symmetric Li cells operating under 1.0 mA cm<sup>–2</sup> and 1.0 mA h cm<sup>–2</sup> demonstrate a long cycle life exceeding 5000 h. Full cells with NMC811 cathodes (4.3 mA h cm<sup>–2</sup> areal capacity) and Li anodes (40 μm, N/P ratio ≈ 1.9) maintain 90% capacity retention after 100 cycles with an average Coulombic efficiency (CE<sub>avg</sub>) exceeding 99.85%. The anode-free Cu|NMC811 cells also show a CE<sub>avg</sub> of 98.36% after 60 cycles. This work provides a cost-effective strategy to enhance the safety, cycling stability, and energy density of next-generation LMBs.
eu_rights_str_mv openAccess
id Manara_56d3d00c8e34f7d76ffbe1cd8ec8fcf8
identifier_str_mv 10.1021/acsnano.5c03410.s002
network_acronym_str Manara
network_name_str ManaraRepo
oai_identifier_str oai:figshare.com:article/29213050
publishDate 2025
repository.mail.fl_str_mv
repository.name.fl_str_mv
repository_id_str
rights_invalid_str_mv CC BY-NC 4.0
spelling Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based ElectrolyteBaogang Zhao (19139738)Nuttapon Yodsin (6760856)Haoyu Ma (12190828)Phornphimon Maitarad (1417432)Wanwisa Limphirat (5474471)Zhuobin Han (21463654)Yinghao Zhou (10106450)Mengjia Yu (19139732)Kexin Liu (1547230)Bingqing Yan (8531742)Xiaoyang Zhao (280499)Guorong Chen (1805383)Xin Feng (111466)Rongrong Jia (2220763)Liyi Shi (1366401)Shuai Yuan (305841)Yingying Lv (1645591)BiochemistryMedicineDevelopmental BiologyPlant BiologyChemical Sciences not elsewhere classifiedwide voltage windowssolid electrolyte interfaceface compatibility challengesaverage coulombic efficiencyelectrochemical prelithiation strategypromoting uniform lifully lithiated liavg </ sublayer coated separatorbased electrolyte ester0 </ supx </effective strategycoated polypropylenebased electrolyteslimited lili anodeswork provideswork developssub ><side reactionoxygen vacanciesnmc811 cathodesmaintain 90lmbs ).irreversible decompositiongeneration lmbsfull cellsfree cudendrite growthcycling stabilitycontact areacapacity retentionareal capacity></ sub85 %.60 cycles40 μm100 cyclesEster-based electrolytes, known for their cost-effectiveness and wide voltage windows, face compatibility challenges with lithium metal (Li<sup>0</sup>), leading to irreversible decomposition and dendrite growth, which impede their application in high-energy-density lithium metal batteries (LMBs). This work develops an electrochemical prelithiation strategy to obtain a fully lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> coated polypropylene (PP) separator with oxygen vacancies, preventing the depletion of limited Li<sup>0</sup> resources while promoting uniform Li<sup>0</sup> plating. Moreover, the dense closest packing structure of Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> can reduce the contact area and side reaction between Li<sup>0</sup> and ester-based electrolytes, stabilizing the solid electrolyte interface (SEI) on Li<sup>0</sup>. Symmetric Li cells operating under 1.0 mA cm<sup>–2</sup> and 1.0 mA h cm<sup>–2</sup> demonstrate a long cycle life exceeding 5000 h. Full cells with NMC811 cathodes (4.3 mA h cm<sup>–2</sup> areal capacity) and Li anodes (40 μm, N/P ratio ≈ 1.9) maintain 90% capacity retention after 100 cycles with an average Coulombic efficiency (CE<sub>avg</sub>) exceeding 99.85%. The anode-free Cu|NMC811 cells also show a CE<sub>avg</sub> of 98.36% after 60 cycles. This work provides a cost-effective strategy to enhance the safety, cycling stability, and energy density of next-generation LMBs.2025-06-02T16:09:38ZDatasetMediainfo:eu-repo/semantics/publishedVersiondataset10.1021/acsnano.5c03410.s002https://figshare.com/articles/media/Fully_Lithiated_Li_sub_i_x_i_sub_TiO_sub_2_sub_Layer_Coated_Separator_for_Securing_a_Lithium-less_Anode_in_an_Ester-Based_Electrolyte/29213050CC BY-NC 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/292130502025-06-02T16:09:38Z
spellingShingle Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte
Baogang Zhao (19139738)
Biochemistry
Medicine
Developmental Biology
Plant Biology
Chemical Sciences not elsewhere classified
wide voltage windows
solid electrolyte interface
face compatibility challenges
average coulombic efficiency
electrochemical prelithiation strategy
promoting uniform li
fully lithiated li
avg </ sub
layer coated separator
based electrolyte ester
0 </ sup
x </
effective strategy
coated polypropylene
based electrolytes
limited li
li anodes
work provides
work develops
sub ><
side reaction
oxygen vacancies
nmc811 cathodes
maintain 90
lmbs ).
irreversible decomposition
generation lmbs
full cells
free cu
dendrite growth
cycling stability
contact area
capacity retention
areal capacity
></ sub
85 %.
60 cycles
40 μm
100 cycles
status_str publishedVersion
title Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte
title_full Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte
title_fullStr Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte
title_full_unstemmed Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte
title_short Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte
title_sort Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2−δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte
topic Biochemistry
Medicine
Developmental Biology
Plant Biology
Chemical Sciences not elsewhere classified
wide voltage windows
solid electrolyte interface
face compatibility challenges
average coulombic efficiency
electrochemical prelithiation strategy
promoting uniform li
fully lithiated li
avg </ sub
layer coated separator
based electrolyte ester
0 </ sup
x </
effective strategy
coated polypropylene
based electrolytes
limited li
li anodes
work provides
work develops
sub ><
side reaction
oxygen vacancies
nmc811 cathodes
maintain 90
lmbs ).
irreversible decomposition
generation lmbs
full cells
free cu
dendrite growth
cycling stability
contact area
capacity retention
areal capacity
></ sub
85 %.
60 cycles
40 μm
100 cycles