Molecular‐Electrode Co‐Engineering Enables High‐Capacity, Long‐Cycling Sulfur‐Based p‑Type Organic Cathodes.

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Title: Molecular‐Electrode Co‐Engineering Enables High‐Capacity, Long‐Cycling Sulfur‐Based p‑Type Organic Cathodes.
Authors: Chen, Zixuan1,2 (AUTHOR), Zhang, Haoyu1 (AUTHOR), Yang, Jixing1 (AUTHOR) jackieyang@tju.edu.cn, Li, Yuesheng1 (AUTHOR)
Source: Advanced Energy Materials. 5/20/2026, Vol. 16 Issue 19, p1-12. 12p.
Subject Terms: *Cathodes, *Electropolymerization, *Energy density, *Lithium-ion batteries, *Electrochemical analysis, *Heterocyclic compounds, *Polymer electrodes
Abstract: Sulfur‐centered p‐type organic cathode materials, particularly those based on thianthrene, have attracted significant interest for high‐voltage lithium‐ion batteries due to their intrinsically high redox potentials and versatile molecular designability. Nevertheless, their practical application remains hindered by low reversible capacity and poor cycling durability, mainly arising from severe dissolution in organic electrolytes or unsatisfied polymer electrode architecture. Herein, we shift focus from conventional thianthrene to the high‐capacity benzo[b]thiophene unit and rationally design two non‐fused and rigid monomers, 1,4‐di(benzothiophen‐2‐yl)benzene (DBTB) and 2,5‐di(benzothiophen‐2‐yl)pyrazine (DBTP), that synergistically integrate molecular enlargement, enhanced planarity, and improved van der Waals forces to suppress dissolution. Crucially, subsequent in situ electropolymerization during charging within the assembled cell directly forms morphology‐optimized polymer electrode architecture. This integrated strategy overcomes the fundamental capacity‐stability trade‐off that has plagued sulfur‐based cathodes. As a result, DBTP‐based cathode delivers a high capacity of 155.1 mAh g−1 (99.6% of theoretical capacity) with exceptional cycling stability (82.1% retention after 5000 cycles at 5 C), surpassing all reported thianthrene‐based polymer cathodes (<110 mAh g−1, ≤500 cycles) and small molecule cathodes (<100 mAh g−1, ≤450 cycles). The molecular‐electrode co‐engineering strategy demonstrated here provides a new pathway to high‐capacity, long‐life sulfur‐based p‐type cathodes. [ABSTRACT FROM AUTHOR]
Database: Energy & Power Source
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Header DbId: enr
DbLabel: Energy & Power Source
An: 193923978
AccessLevel: 6
PubType: Academic Journal
PubTypeId: academicJournal
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  Data: Molecular‐Electrode Co‐Engineering Enables High‐Capacity, Long‐Cycling Sulfur‐Based p‑Type Organic Cathodes.
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  Data: &lt;searchLink fieldCode=&quot;JN&quot; term=&quot;%22Advanced+Energy+Materials%22&quot;&gt;Advanced Energy Materials&lt;/searchLink&gt;. 5/20/2026, Vol. 16 Issue 19, p1-12. 12p.
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  Data: *&lt;searchLink fieldCode=&quot;DE&quot; term=&quot;%22Cathodes%22&quot;&gt;Cathodes&lt;/searchLink&gt;&lt;br /&gt;*&lt;searchLink fieldCode=&quot;DE&quot; term=&quot;%22Electropolymerization%22&quot;&gt;Electropolymerization&lt;/searchLink&gt;&lt;br /&gt;*&lt;searchLink fieldCode=&quot;DE&quot; term=&quot;%22Energy+density%22&quot;&gt;Energy density&lt;/searchLink&gt;&lt;br /&gt;*&lt;searchLink fieldCode=&quot;DE&quot; term=&quot;%22Lithium-ion+batteries%22&quot;&gt;Lithium-ion batteries&lt;/searchLink&gt;&lt;br /&gt;*&lt;searchLink fieldCode=&quot;DE&quot; term=&quot;%22Electrochemical+analysis%22&quot;&gt;Electrochemical analysis&lt;/searchLink&gt;&lt;br /&gt;*&lt;searchLink fieldCode=&quot;DE&quot; term=&quot;%22Heterocyclic+compounds%22&quot;&gt;Heterocyclic compounds&lt;/searchLink&gt;&lt;br /&gt;*&lt;searchLink fieldCode=&quot;DE&quot; term=&quot;%22Polymer+electrodes%22&quot;&gt;Polymer electrodes&lt;/searchLink&gt;
– Name: Abstract
  Label: Abstract
  Group: Ab
  Data: Sulfur‐centered p‐type organic cathode materials, particularly those based on thianthrene, have attracted significant interest for high‐voltage lithium‐ion batteries due to their intrinsically high redox potentials and versatile molecular designability. Nevertheless, their practical application remains hindered by low reversible capacity and poor cycling durability, mainly arising from severe dissolution in organic electrolytes or unsatisfied polymer electrode architecture. Herein, we shift focus from conventional thianthrene to the high‐capacity benzo[b]thiophene unit and rationally design two non‐fused and rigid monomers, 1,4‐di(benzothiophen‐2‐yl)benzene (DBTB) and 2,5‐di(benzothiophen‐2‐yl)pyrazine (DBTP), that synergistically integrate molecular enlargement, enhanced planarity, and improved van der Waals forces to suppress dissolution. Crucially, subsequent in situ electropolymerization during charging within the assembled cell directly forms morphology‐optimized polymer electrode architecture. This integrated strategy overcomes the fundamental capacity‐stability trade‐off that has plagued sulfur‐based cathodes. As a result, DBTP‐based cathode delivers a high capacity of 155.1 mAh g−1 (99.6% of theoretical capacity) with exceptional cycling stability (82.1% retention after 5000 cycles at 5 C), surpassing all reported thianthrene‐based polymer cathodes (&lt;110 mAh g−1, ≤500 cycles) and small molecule cathodes (&lt;100 mAh g−1, ≤450 cycles). The molecular‐electrode co‐engineering strategy demonstrated here provides a new pathway to high‐capacity, long‐life sulfur‐based p‐type cathodes. [ABSTRACT FROM AUTHOR]
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RecordInfo BibRecord:
  BibEntity:
    Identifiers:
      – Type: doi
        Value: 10.1002/aenm.70848
    Languages:
      – Code: eng
        Text: English
    PhysicalDescription:
      Pagination:
        PageCount: 12
        StartPage: 1
    Subjects:
      – SubjectFull: Cathodes
        Type: general
      – SubjectFull: Electropolymerization
        Type: general
      – SubjectFull: Energy density
        Type: general
      – SubjectFull: Lithium-ion batteries
        Type: general
      – SubjectFull: Electrochemical analysis
        Type: general
      – SubjectFull: Heterocyclic compounds
        Type: general
      – SubjectFull: Polymer electrodes
        Type: general
    Titles:
      – TitleFull: Molecular‐Electrode Co‐Engineering Enables High‐Capacity, Long‐Cycling Sulfur‐Based p‑Type Organic Cathodes.
        Type: main
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      – PersonEntity:
          Name:
            NameFull: Chen, Zixuan
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            NameFull: Zhang, Haoyu
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            NameFull: Yang, Jixing
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            NameFull: Li, Yuesheng
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          Dates:
            – D: 20
              M: 05
              Text: 5/20/2026
              Type: published
              Y: 2026
          Identifiers:
            – Type: issn-print
              Value: 16146832
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              Value: 16
            – Type: issue
              Value: 19
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            – TitleFull: Advanced Energy Materials
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