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Enhanced photoelectrochemical water splitting resulting from full-dimensional carrier behavior optimization of ZnIn2S4-based dimorphic homojunction

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  • Hao, Zhichao
  • Meng, Xianghui
  • Wang, Ruikai
  • Qu, Lexiao
  • Liu, Xinzheng
  • Sun, Xu
  • Li, Haiyan
  • Xia, Chenghui
  • Dong, Bohua
  • Cao, Lixin

Abstract

Optimizing carrier separation efficiency (8.78 %) and energy barrier of rate-determining step (RDS, 0.96 eV) are critical for advancing solar-driven hydrogen production through ZnIn2S4 photoanodes in carbon-neutral energy cycles. Hexagonal/cubic ZnIn2S4 (hZIS/cZIS) monomorphic homojunctions demonstrate improved photoelectrochemical performance, yet insufficient electronic regulation limits further optimization. This work presents a dual-phase engineering strategy through crystal-phase hybridization and ion doping to construct Zr:hZIS/Ni:cZIS dimorphic homojunctions. Systematic characterization reveals detailed modification mechanisms: (1) Strengthened interfacial electric field with expanded work function difference (0.53 eV vs. 0.29 eV in hZIS/cZIS) of components, elevating carrier separation efficiency to 28.40 %; (2) Surface state reconstruction enables carrier injection efficiency to 43.84 % through accelerated charge transfer; (3) Reduced RDS energy barrier (0.73 eV vs. 0.86 eV in hZIS/cZIS); (4) Broadened light absorption extending to 530 nm. The weakened electron localization across dimensions further enhances charge transfer kinetics. Consequently, photocurrent density of 0.98 mA/cm2 is achieved by Zr:hZIS/Ni:cZIS that is 6.53 and 2.80 times higher than that of hZIS and hZIS/cZIS, respectively. This approach overcomes limitations of fixed band structures and Fermi-level pinning in traditional composite systems, providing new insights into multidimensional material engineering for sustainable energy conversion.

Suggested Citation

  • Hao, Zhichao & Meng, Xianghui & Wang, Ruikai & Qu, Lexiao & Liu, Xinzheng & Sun, Xu & Li, Haiyan & Xia, Chenghui & Dong, Bohua & Cao, Lixin, 2025. "Enhanced photoelectrochemical water splitting resulting from full-dimensional carrier behavior optimization of ZnIn2S4-based dimorphic homojunction," Renewable Energy, Elsevier, vol. 248(C).
    • Handle: RePEc:eee:renene:v:248:y:2025:i:c:s0960148125007657
    DOI: 10.1016/j.renene.2025.123103
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    References listed on IDEAS

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    1. Rui-Ting Gao & Jiangwei Zhang & Tomohiko Nakajima & Jinlu He & Xianhu Liu & Xueyuan Zhang & Lei Wang & Limin Wu, 2023. "Single-atomic-site platinum steers photogenerated charge carrier lifetime of hematite nanoflakes for photoelectrochemical water splitting," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Dong, Zhenbiao & Qin, Dongmei & Ma, Junjie & Li, Zhenyu & Han, Sheng, 2024. "Bulk-phase and surface dual-defective engineering enabled Ti-based nanotubes photoanode for highly efficient photoelectrochemical water splitting," Renewable Energy, Elsevier, vol. 231(C).
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