Lv Xiaojing, Li Mingzhe, Qin Hongye, Jiao Lifang, Lv Yuzhen, Luo Hongyun, Zhou Wei, Guo Lin
Hangzhou International Innovation Institute, Beihang University, Hangzhou, 311115, China.
School of Chemistry, Beihang University, Beijing, 100191, China.
Adv Sci (Weinh). 2025 Sep 8:e12638. doi: 10.1002/advs.202512638.
The difference in hydroxyl adsorption between Ni and Fe sites in NiFeOOH limits the efficient dual-site synergistic mechanism (DSSM) during oxygen evolution reaction (OER). Here, a novel needle-array electrodeposition is reported for the scalable and efficient fabrication of Co and Y co-doped NiFeOOH catalyst. It achieves an ultralow overpotential of 270 mV at 1 A cm with a small Tafel slope of 30.7 mV dec. It maintains stable operation at 1 A cm for 1500 hrs with 98 % initial potential retention. When integrated into a 25 cm anion exchange membrane electrolyzer, the system only needs 2.13 V to achieve 1 A cm. XPS, XAS, and DFT studies reveal that Co and Y dopants increase the Lewis acidity of Ni sites, enhancing OH adsorption. Concurrently, the incorporation of large Y atoms induces lattice distortion and elongates Fe─O─M bonds, weakening OH binding at Fe sites. This dual-site modulation reduces adsorption disparity, activates NiFe dual-active centers, and promotes the DSSM pathway, as confirmed by in situ ATR-SEIRAS. The rate-determining step energy is lowered to 1.71 eV, significantly outperforming the conventional AEM pathway (2.51 eV). This work provides dual-site modulation into engineering high-performance NiFe-based OER catalysts for practical water electrolysis.
NiFeOOH中Ni和Fe位点之间羟基吸附的差异限制了析氧反应（OER）过程中高效的双位点协同机制（DSSM）。在此，报道了一种用于可扩展且高效制备Co和Y共掺杂NiFeOOH催化剂的新型针状阵列电沉积方法。它在1 A cm⁻²时实现了270 mV的超低过电位，塔菲尔斜率仅为30.7 mV dec⁻¹。在1 A cm⁻²下可稳定运行1500小时，初始电位保持率达98%。当集成到25 cm²的阴离子交换膜电解槽中时，该系统仅需2.13 V就能达到1 A cm⁻²。X射线光电子能谱（XPS）、X射线吸收光谱（XAS）和密度泛函理论（DFT）研究表明，Co和Y掺杂剂增加了Ni位点的路易斯酸度，增强了OH吸附。同时，大尺寸Y原子的掺入引起晶格畸变并拉长Fe─O─M键，削弱了Fe位点上的OH结合。这种双位点调制减少了吸附差异，激活了NiFe双活性中心，并促进了DSSM途径，原位衰减全反射表面增强红外吸收光谱（ATR-SEIRAS）证实了这一点。速率决定步骤的能量降低至1.71 eV，显著优于传统的阴离子交换膜（AEM）途径（2.51 eV）。这项工作为工程化高性能NiFe基OER催化剂用于实际水电解提供了双位点调制方法。
