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Peer-reviewedCC BY-NC-ND 4.0Angewandte Chemie (International Ed. in English)

S‐Scheme Charge Separation Enables Photocarrier‐Regulated Aqueous NH4 + Storage in g‐C3N4@WO3 Heterojunctions

5 affiliations
  1. 1Institute of Clean Energy Chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province College of Chemistry Liaoning University Shenyang China
  2. 2Centre For Atomaterials and Nanomanufacturing (CAN) School of Science RMIT University Melbourne Victoria Australia
  3. 3CNPC Liaohe Petrochemical Company Panjin China
  4. 4Department of Chemistry Tsinghua University Beijing China
  5. 5Institute of Science and Technology for New Energy Xi'an Technological University Xi'an People's Republic of China

Abstract

Aqueous ammonium‐ion (NH4 +) batteries are promising for sustainable energy storage, yet their performance is severely constrained by sluggish reaction kinetics. Photo‐assisted strategies offer a compelling route to overcome these limitations; however, single‐semiconductor electrodes suffer from rapid photogenerated carrier recombination, resulting in poor light‐utilization efficiency. Here, we develop a g‐C3N4@WO3 S‐scheme heterojunction (CNW) that unlocks efficient light‐to‐charge conversion for photocarrier‐regulated reversible NH4 + storage. Characterization and simulation reveal that Fermi level alignment and band bending at the CNW interface establish a built‐in electric field, driving S‐scheme charge separation with selective recombination of low‐energy carriers and retention of high‐energy electrons on g‐C3N4 and holes on WO3. This preserves strong redox capability, thereby enabling efficient utilization of photoexcited carriers in the electrochemical storage process. Together with pronounced interfacial orbital coupling, the resulting photocarrier redistribution accelerates NH4 + adsorption and electron/ion transport. Consequently, the CNW electrode delivers a 187% capacity enhancement under illumination, achieving 452 mAh g−1 at 2 A g−1 with excellent cycling stability, surpassing all currently reported W‐based and C‐based materials for NH4 + storage. Correlative electrochemical, spectroscopic, and theoretical analyses decouple photoelectric and thermal effects, revealing a photoelectric‐dominated, thermally assisted synergistic mechanism that simultaneously enhances NH4 + storage kinetics and capacity.

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BibTeX
@article{zhang2026sscheme,
  title = {{S‐Scheme Charge Separation Enables Photocarrier‐Regulated Aqueous NH4 + Storage in g‐C3N4@WO3 Heterojunctions}},
  author = {Yue Zhang and Yulong Jia and Fanfang Sun and Jichi Liu and Bing Tang and Hui Li and Wubin Du and Hongge Pan and Zi‐Hang Huang and Tianyi Ma},
  journal = {Angewandte Chemie (International Ed. in English)},
  year = {2026},
  month = sep,
  doi = {10.1002/anie.3990578},
  url = {https://doi.org/10.1002/anie.3990578},
  note = {CC BY-NC-ND 4.0},
}
RIS
TY  - JOUR
TI  - S‐Scheme Charge Separation Enables Photocarrier‐Regulated Aqueous NH4 + Storage in g‐C3N4@WO3 Heterojunctions
AU  - Yue Zhang
AU  - Yulong Jia
AU  - Fanfang Sun
AU  - Jichi Liu
AU  - Bing Tang
AU  - Hui Li
AU  - Wubin Du
AU  - Hongge Pan
AU  - Zi‐Hang Huang
AU  - Tianyi Ma
PY  - 2026
DA  - 2026/09/15
JO  - Angewandte Chemie (International Ed. in English)
DO  - 10.1002/anie.3990578
UR  - https://doi.org/10.1002/anie.3990578
AB  - Aqueous ammonium‐ion (NH4 +) batteries are promising for sustainable energy storage, yet their performance is severely constrained by sluggish reaction kinetics. Photo‐assisted strategies offer a compelling route to overcome these limitations; however, single‐semiconductor electrodes suffer from rapid photogenerated carrier recombination, resulting in poor light‐utilization efficiency. Here, we develop a g‐C3N4@WO3 S‐scheme heterojunction (CNW) that unlocks efficient light‐to‐charge conversion for photocarrier‐regulated reversible NH4 + storage. Characterization and simulation reveal that Fermi level alignment and band bending at the CNW interface establish a built‐in electric field, driving S‐scheme charge separation with selective recombination of low‐energy carriers and retention of high‐energy electrons on g‐C3N4 and holes on WO3. This preserves strong redox capability, thereby enabling efficient utilization of photoexcited carriers in the electrochemical storage process. Together with pronounced interfacial orbital coupling, the resulting photocarrier redistribution accelerates NH4 + adsorption and electron/ion transport. Consequently, the CNW electrode delivers a 187% capacity enhancement under illumination, achieving 452 mAh g−1 at 2 A g−1 with excellent cycling stability, surpassing all currently reported W‐based and C‐based materials for NH4 + storage. Correlative electrochemical, spectroscopic, and theoretical analyses decouple photoelectric and thermal effects, revealing a photoelectric‐dominated, thermally assisted synergistic mechanism that simultaneously enhances NH4 + storage kinetics and capacity.
SN  - 1433-7851
SN  - 1521-3773
ER  -