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Neodymium-doped hollow Ir/IrO2 nanospheres with low geometric iridium density enable excellent acidic water oxidation performance
Xiaoqian Wei, Hanyu Gao, Tiantian Wang, Zijian Li, Yanru Geng, Guiping Zheng, Min Gyu Kim, Haeseong Jang*, Xien Liu*, Qing Qin*
https://doi.org/10.1016/j.cjsc.2025.100600
ABSTRACT
Reducing the Ir loading while preserving catalytic performance and mechanical robustness in anodic catalyst layers remains a critical challenge for the large-scale implementation of proton exchange membrane water electrolysis (PEMWE). Herein, we present a structural engineering strategy involving neodymium-doped Ir/IrO2 (Nd-Ir/IrO2) hollow nanospheres with precisely adjustable shell thickness and cavity dimensions. The optimized catalyst demonstrates excellent oxygen evolution reaction (OER) performance in acidic media, achieving a remarkably low overpotential of 259 mV at a benchmark current density of 10 mA cm-2 while exhibiting substantially enhanced durability compared to commercial IrO2 and Ir/IrO2 counterparts. Notably, the Nd-Ir/IrO2 catalyst delivers a mass activity of 541.6 A gIr-1 at 1.50 V vs RHE, representing a 74.5-fold enhancement over conventional IrO2. Through comprehensive electrochemical analysis and advanced characterization techniques reveal that, the hierarchical hollow architecture simultaneously addresses multiple critical requirements: (i) abundant exposed active sites enabled by an enhanced electrochemical surface area, (ii) optimized mass transport pathways through engineered porosity, and (iii) preserved structural integrity via a continuous conductive framework, collectively enabling significant Ir loading reduction without compromising catalytic layer performance. Fundamental mechanistic investigations further disclose that Nd doping induces critical interfacial Nd-O-Ir configurations that stabilize lattice oxygen, together with intensified electron effect among mixed valent Ir that inhibits the overoxidation of Ir active sites during the OER process, synergistically ensuring enhanced catalytic durability. Our work establishes a dual-modulation paradigm integrating nanoscale architectural engineering with atomic-level heteroatom doping, providing a viable pathway toward high-performance PEMWE systems with drastically reduced noble metal requirements.
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