Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices

The interest in aqueous energy storage devices is surging due to their exceptional safety profile. However, in aqueous energy storage systems, interfacial side reactions, predominantly attributed to the oxygen evolution reaction (OER), result in significant self-discharge, which is concomitant with...

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Main Author: Jin Li (119007) (author)
Other Authors: Shuo Sun (626584) (author), Hao Huang (111923) (author), Teng Zhai (1459396) (author), Yanchen Liu (3691888) (author), Minghui Gu (803521) (author), Hongye Yang (11624399) (author), Mingqing Sun (18843015) (author), Tianyi Kou (1530160) (author), Shuang Li (146392) (author), Hui Xia (133168) (author)
Published: 2025
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_version_ 1852022753291403264
author Jin Li (119007)
author2 Shuo Sun (626584)
Hao Huang (111923)
Teng Zhai (1459396)
Yanchen Liu (3691888)
Minghui Gu (803521)
Hongye Yang (11624399)
Mingqing Sun (18843015)
Tianyi Kou (1530160)
Shuang Li (146392)
Hui Xia (133168)
author2_role author
author
author
author
author
author
author
author
author
author
author_facet Jin Li (119007)
Shuo Sun (626584)
Hao Huang (111923)
Teng Zhai (1459396)
Yanchen Liu (3691888)
Minghui Gu (803521)
Hongye Yang (11624399)
Mingqing Sun (18843015)
Tianyi Kou (1530160)
Shuang Li (146392)
Hui Xia (133168)
author_role author
dc.creator.none.fl_str_mv Jin Li (119007)
Shuo Sun (626584)
Hao Huang (111923)
Teng Zhai (1459396)
Yanchen Liu (3691888)
Minghui Gu (803521)
Hongye Yang (11624399)
Mingqing Sun (18843015)
Tianyi Kou (1530160)
Shuang Li (146392)
Hui Xia (133168)
dc.date.none.fl_str_mv 2025-02-13T06:04:55Z
dc.identifier.none.fl_str_mv 10.1021/jacs.4c16996.s002
dc.relation.none.fl_str_mv https://figshare.com/articles/media/Ferrocyanide_Skin_-Mediated_Anticatalysis_Mitigating_Self-Discharge_in_Aqueous_Electrochemical_Devices/28406744
dc.rights.none.fl_str_mv CC BY-NC 4.0
info:eu-repo/semantics/openAccess
dc.subject.none.fl_str_mv Medicine
Immunology
Infectious Diseases
Space Science
Biological Sciences not elsewhere classified
Chemical Sciences not elsewhere classified
undesired phase transition
transition metal compounds
reaction pathway presents
oxygen evolution reaction
interfacial side reactions
exceptional safety profile
broadly applicable paradigm
aqueous electrochemical devices
significant energy barrier
fully charged electrode
oh )< sub
nickel cobalt oxide
2 </ sub
remarkable voltage retention
oer ), result
significant self
modified electrode
vanadium oxide
manganese oxide
tmc materials
taking nio
surging due
predominantly attributed
n –
mitigating self
idling within
idling process
hydroxyl ions
findings highlight
effectively shielding
bonding process
active sites
1 week
dc.title.none.fl_str_mv Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices
dc.type.none.fl_str_mv Dataset
Media
info:eu-repo/semantics/publishedVersion
dataset
description The interest in aqueous energy storage devices is surging due to their exceptional safety profile. However, in aqueous energy storage systems, interfacial side reactions, predominantly attributed to the oxygen evolution reaction (OER), result in significant self-discharge, which is concomitant with the deterioration of both voltage and capacity. Herein, we propose the construction of a ferrocyanide “skin” on transition metal compounds (TMCs) to mitigate this issue. This engineered “skin” creates Fe–CN terminations, initiating a new reaction pathway featured by the bonding process of N–O and N–H bonds. This reaction pathway presents a significant energy barrier, effectively shielding the active sites for the OER from H<sub>2</sub>O molecules and hydroxyl ions. Taking NiO as an example, the ferrocyanide “skin” effectively suppresses the undesired phase transition from NiOOH to Ni(OH)<sub>2</sub> during the idling process of a fully charged electrode, enabling the as-modified electrode to achieve a remarkable voltage retention of 80.0% after 1 week of idling within a device. Furthermore, this concept demonstrates extensive applicability, extending to a range of TMC materials, including but not limited to manganese oxide, vanadium oxide, and nickel cobalt oxide. These findings highlight the efficacy of the ferrocyanide “skin” design strategy as a broadly applicable paradigm for suppressing H<sub>2</sub>O-induced undesirable phase transitions in aqueous energy storage devices.
eu_rights_str_mv openAccess
id Manara_2783efed83c19e2e5bdf6d50aa6c1027
identifier_str_mv 10.1021/jacs.4c16996.s002
network_acronym_str Manara
network_name_str ManaraRepo
oai_identifier_str oai:figshare.com:article/28406744
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 Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical DevicesJin Li (119007)Shuo Sun (626584)Hao Huang (111923)Teng Zhai (1459396)Yanchen Liu (3691888)Minghui Gu (803521)Hongye Yang (11624399)Mingqing Sun (18843015)Tianyi Kou (1530160)Shuang Li (146392)Hui Xia (133168)MedicineImmunologyInfectious DiseasesSpace ScienceBiological Sciences not elsewhere classifiedChemical Sciences not elsewhere classifiedundesired phase transitiontransition metal compoundsreaction pathway presentsoxygen evolution reactioninterfacial side reactionsexceptional safety profilebroadly applicable paradigmaqueous electrochemical devicessignificant energy barrierfully charged electrodeoh )< subnickel cobalt oxide2 </ subremarkable voltage retentionoer ), resultsignificant selfmodified electrodevanadium oxidemanganese oxidetmc materialstaking niosurging duepredominantly attributedn –mitigating selfidling withinidling processhydroxyl ionsfindings highlighteffectively shieldingbonding processactive sites1 weekThe interest in aqueous energy storage devices is surging due to their exceptional safety profile. However, in aqueous energy storage systems, interfacial side reactions, predominantly attributed to the oxygen evolution reaction (OER), result in significant self-discharge, which is concomitant with the deterioration of both voltage and capacity. Herein, we propose the construction of a ferrocyanide “skin” on transition metal compounds (TMCs) to mitigate this issue. This engineered “skin” creates Fe–CN terminations, initiating a new reaction pathway featured by the bonding process of N–O and N–H bonds. This reaction pathway presents a significant energy barrier, effectively shielding the active sites for the OER from H<sub>2</sub>O molecules and hydroxyl ions. Taking NiO as an example, the ferrocyanide “skin” effectively suppresses the undesired phase transition from NiOOH to Ni(OH)<sub>2</sub> during the idling process of a fully charged electrode, enabling the as-modified electrode to achieve a remarkable voltage retention of 80.0% after 1 week of idling within a device. Furthermore, this concept demonstrates extensive applicability, extending to a range of TMC materials, including but not limited to manganese oxide, vanadium oxide, and nickel cobalt oxide. These findings highlight the efficacy of the ferrocyanide “skin” design strategy as a broadly applicable paradigm for suppressing H<sub>2</sub>O-induced undesirable phase transitions in aqueous energy storage devices.2025-02-13T06:04:55ZDatasetMediainfo:eu-repo/semantics/publishedVersiondataset10.1021/jacs.4c16996.s002https://figshare.com/articles/media/Ferrocyanide_Skin_-Mediated_Anticatalysis_Mitigating_Self-Discharge_in_Aqueous_Electrochemical_Devices/28406744CC BY-NC 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/284067442025-02-13T06:04:55Z
spellingShingle Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices
Jin Li (119007)
Medicine
Immunology
Infectious Diseases
Space Science
Biological Sciences not elsewhere classified
Chemical Sciences not elsewhere classified
undesired phase transition
transition metal compounds
reaction pathway presents
oxygen evolution reaction
interfacial side reactions
exceptional safety profile
broadly applicable paradigm
aqueous electrochemical devices
significant energy barrier
fully charged electrode
oh )< sub
nickel cobalt oxide
2 </ sub
remarkable voltage retention
oer ), result
significant self
modified electrode
vanadium oxide
manganese oxide
tmc materials
taking nio
surging due
predominantly attributed
n –
mitigating self
idling within
idling process
hydroxyl ions
findings highlight
effectively shielding
bonding process
active sites
1 week
status_str publishedVersion
title Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices
title_full Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices
title_fullStr Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices
title_full_unstemmed Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices
title_short Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices
title_sort Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices
topic Medicine
Immunology
Infectious Diseases
Space Science
Biological Sciences not elsewhere classified
Chemical Sciences not elsewhere classified
undesired phase transition
transition metal compounds
reaction pathway presents
oxygen evolution reaction
interfacial side reactions
exceptional safety profile
broadly applicable paradigm
aqueous electrochemical devices
significant energy barrier
fully charged electrode
oh )< sub
nickel cobalt oxide
2 </ sub
remarkable voltage retention
oer ), result
significant self
modified electrode
vanadium oxide
manganese oxide
tmc materials
taking nio
surging due
predominantly attributed
n –
mitigating self
idling within
idling process
hydroxyl ions
findings highlight
effectively shielding
bonding process
active sites
1 week