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 acid site regulation for fabricating highly active electrocatalysts for high-performance AEMFCs.

中文翻译：

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通过 Lewis-Acidic Site 调制减弱 O-中间体对 Pd Metallene 的吸附强度以增强氧还原


金属钯的电子性质的合理设计和调制被认为是增强阴离子交换膜燃料电池 （AEMFC） 中氧还原反应 （ORR） 的有前途的途径，但它们仍然是一个艰巨的挑战。在此，使用简单的湿化学方法提出了一种具有大量缺陷的 Zr 掺杂金属钯 （PdZr metallene） 薄片结构，用于高效且高耐久的 ORR 电催化。多项微观结构分析发现，通过 Lewis 酸性 Zr 位点调制对 PdZr 金属烯进行精心编排的电子和亲氧调控可以同时优化 Pd 的电子构型，降低 Pd 的 d 波段中心，从而促进内禀活性。得益于Zr耦合效应促进的独特二维形貌和电子结构优化，所得的PdZr金属烯在碱性溶液中表现出显著增强的ORR电催化性能，具有0.87 V的高半波电位（E_1/2）和值得称道的30 000 s稳定性，超过了文献中报道的Pd金属烯和各种先进的Pd基催化剂。令人鼓舞的是，基于 PdZr 金属烯的 AEMFC 在碱性环境中实现了更高的最大功率密度 （90.4 mW cm^–2） 和令人印象深刻的稳健性超过 12 小时，体现了 PdZr 金属烯在 AEMFC 中的实际应用。本研究展示了 PdZr 金属烯通过 Lewis 酸位点调节制备用于高性能 AEMFC 的高活性电催化剂的适用性。