Li Tongfei, Du Tianheng, Xu Shuya, Zhang Luping, Peng Yukun, Zhao Xianzhe, Zhou Xi, Yan Chenglin, Qian Tao
School of Chemistry and Chemical Engineering, Nantong University, Nantong 226019, China.
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, China.
Inorg Chem. 2024 Oct 14;63(41):19450-19457. doi: 10.1021/acs.inorgchem.4c03455. Epub 2024 Sep 27.
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 () 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) 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.
钯金属烯电子性质的合理设计与调控被认为是增强阴离子交换膜燃料电池（AEMFC）中氧还原反应（ORR）的一条有前景的途径，但仍面临巨大挑战。在此，我们采用简便的湿化学方法提出了一种具有大量缺陷的Zr掺杂钯金属烯（PdZr金属烯）薄片结构，用于高效且高度耐用的ORR电催化。多种微观结构分析表明，通过路易斯酸性Zr位点调控对PdZr金属烯进行精心的电子和氧ophilic调节，可以同时优化Pd的电子构型，降低Pd的d带中心，从而提高本征活性。得益于Zr耦合效应促进的独特二维形态和电子结构优化，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，半波电位（）高达0.87 V，在30000 s内具有良好的稳定性，超过了文献报道的钯金属烯和各种先进的钯基催化剂。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），并在12小时内表现出令人印象深刻的稳健性，这表明PdZr金属烯在AEMFC中的实际应用。这项研究展示了通过路易斯酸位点调控的PdZr金属烯在制造用于高性能AEMFC的高活性电催化剂方面的适用性。
