Bimetallic Fenton catalyst has attracted widespread attention in refractory organics removal. Herein, we firstly investigated the influence of ZrO₂ structure features on H₂O₂ activation in Zr-Fe bimetallic catalyst. The results show that the heterojunction structure will be formed after high temperature calcination, which makes the ability of Zr-Fe bimetallic catalyst to activate H₂O₂ for bisphenol A degradation is 3.1 times higher than that of α-Fe₂O₃ without Zr doping. Through characterization and density functional theory, it was identified that compared to (1 1 0) interface, the adsorption energy of H₂O₂ on iron sites at (1 1 0)-(1 0 0) interface reduced by 1.27 kJ mol⁻¹, while the Fe–O bond length in the stable configuration of Fe-OOH increased by 0.16 Å, which was beneficial to the association and dissociation of H₂O₂ on iron sites. Besides, the surface -OH of amorphous ZrO₂ in Zr-Fe bimetallic catalyst synthesized under low temperature conditions could promote HO₂^•/O₂^•- formation through the surface electron transfer, accelerating the Fe(III) reduction. In conclusion, this study reveals the influence of environment-friendly ZrO₂ structure features on H₂O₂ activation, proposes a new insight into strengthening the synergistic effect between bimetals, and provides a reference for the structural optimization of bimetallic catalysts.

双金属芬顿催化剂在难降解有机物去除方面受到广泛关注。在此，我们首先研究了 ZrO ₂结构特征对Zr-Fe 双金属催化剂中H ₂ O ₂活化的影响。结果表明，高温煅烧后会形成异质结结构，这使得Zr-Fe双金属催化剂活化H ₂ O ₂降解双酚A的能力是不含Zr的α-Fe ₂ O _{3 的}3.1倍兴奋剂。通过表征和密度泛函理论，确定与(1 1 0)界面相比，H ₂ O ₂的吸附能(1 1 0)-(1 0 0) 界面铁位点减少 1.27 kJ mol ^-1，而稳定构型 Fe-OOH 中的 Fe-O 键长增加 0.16 Å，有利于缔合和 H ₂ O ₂在铁位点上的解离。此外，低温条件下合成的Zr-Fe双金属催化剂中无定形ZrO ₂的表面-OH可以通过表面电子转移促进HO ₂ ^• /O ₂ ^•-的形成，加速Fe(III)的还原。总之，本研究揭示了环境友好型 ZrO ₂结构特征对 H ₂ O _{2 的影响} 活化，提出了加强双金属间协同效应的新见解，并为双金属催化剂的结构优化提供了参考。