Weakening O-Intermediates Adsorption Strength Over the Pd Metallene via Lewis-Acidic Site Modulation for Enhanced Oxygen Reduction

作者：Tongfei Li, Tianheng Du, Shuya Xu, Luping Zhang, Yukun Peng, Xianzhe Zhao, Xi Zhou, Chenglin Yan, Tao Qian · 发表于：Inorganic Chemistry · 年份：2024 · DOI：10.1021/acs.inorgchem.4c03455 · 被引用次数：13 · 研究领域：Electrocatalysts for Energy Conversion、Catalytic Processes in Materials Science、Fuel Cells and Related Materials

The reasonable design and modulation of the electronic properties of Pd metallene are acknowledged as a promising avenue for enhancing the oxygen reduction reaction (ORR) in anion exchange membrane fuel cells (AEMFCs), yet they remain a formidable challenge. Herein, a thin-sheet structure of Zr-doped Pd metallene (PdZr metallene) with abundant defects is proposed using a facile wet-chemical approach for efficient and highly durable ORR electrocatalysis. Multiple microstructural analyses uncover that orchestrated electronic and oxophilic regulation of PdZr metallene via Lewis-acidic Zr site modulation could concurrently optimize the electronic configuration of Pd, downshift the d-band center of Pd, and, thus, promote the intrinsic activity. Benefiting from the unique two-dimensional morphology and electronic structure optimization facilitated by the Zr coupling effect, the resultant PdZr metallene demonstrates significantly enhanced ORR electrocatalytic performance in basic solutions, with a high half-wave potential ( E 1/2 ) of 0.87 V and commendable stability for 30 000 s, surpassing those of Pd metallene and various advanced Pd-based catalysts reported in the literature. Encouragingly, the PdZr metallene-based AEMFC achieves an increased maximum power density (90.4 mW cm –2 ) and impressive robustness over 12 h in an alkaline environment, manifesting the practical application of PdZr metallene in AEMFCs. This study showcases the applicability of PdZr metallene via Lewis aci...