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Hui Wan, Yu-Ting Yu, Ming-Hua Xian, Yang Liu, Yan Luo, Jia-Rong Huang, Zi-Xuan Yang, Lan Long, Chao Wang, Guang-Dong Liu, Jian-Hang Nie, Gui-Fang Huang, Wei-Qing Huang. Sacrificial Cr-Triggered Cascade Reconstruction of NiFe LDH: Balancing Active Site Density and Intrinsic Activity for Water Oxidation. Green Energy&Environment. doi: 10.1016/j.gee.2026.06.019
Citation: Hui Wan, Yu-Ting Yu, Ming-Hua Xian, Yang Liu, Yan Luo, Jia-Rong Huang, Zi-Xuan Yang, Lan Long, Chao Wang, Guang-Dong Liu, Jian-Hang Nie, Gui-Fang Huang, Wei-Qing Huang. Sacrificial Cr-Triggered Cascade Reconstruction of NiFe LDH: Balancing Active Site Density and Intrinsic Activity for Water Oxidation. Green Energy&Environment. doi: 10.1016/j.gee.2026.06.019
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Sacrificial Cr-Triggered Cascade Reconstruction of NiFe LDH: Balancing Active Site Density and Intrinsic Activity for Water Oxidation

doi: 10.1016/j.gee.2026.06.019

  • a. School of Materials and Environmental Engineering, Changsha University, Changsha, 410082, China;

  • b. Department of Applied Physics, School of Physics and Electronics, Hunan University, Changsha 410082, China;

  • c. Shandong Xiehe University, Jinan 250107, China

Funds:

This work is supported by the Natural Science Foundation of Shandong Province (ZR2024QB185), Natural Science Foundation of Hunan Province (2026JJ60482, 2024JJ7616), Scientific Research Fund of Hunan Provincial Education Department (25B0816), Changsha Natural Science Foundation (kq2502099).

  • Received date 25 February 2026, Accepted date 17 June 2026, RevRecd date 27 May 2026, Available online 22 June 2026
    Abstract
  • NiFe-based layered double hydroxides (LDHs) are among the most effective oxygen evolution reaction (OER) catalysts, yet their performance is fundamentally constrained by the quantity-quality paradox: the trade-off between active site density and intrinsic activity. Herein, we leverage a sacrificial Cr3+-triggered cascade reconstruction to modulate the surface Fe/Ni stoichiometry and unveil a high density of Ni active centers. Driven by its local environment, the preferential dissolution of Cr3+ during electrochemical activation yields a transient CrO42--enriched interfacial layer, thereby inducing selective Fe leaching and regulating the local bonding environment to promote Ni oxidation. This cascade evolution effectively modulates the surface Fe/Ni stoichiometry, thereby expanding the population of Ni centers and stabilizing high-valent Ni3+ species with enhanced intrinsic kinetics. As a result, a cation-vacancy-rich NiFeOOH@NiFe LDH heterointerface is spontaneously constructed with optimized electronic structure and favorable reaction energetics. Compared to the undoped sample, the Cr-modified catalyst exhibits significantly enhanced OER kinetics and robust electrochemical durability. Density functional theory calculations further elucidate the origins of the enhanced activity, confirming that the reconstructed heterointerface significantly mitigates the kinetic barriers for the rate-determining steps. This study elucidates a sacrificial-ion-mediated reconstruction pathway, offering a general strategy for designing high-performance OER.

     

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