Although great successes have been accomplished on the controlled synthesis of 2D and 3D Pd-containing nanomaterials, tapping into the novel Pd-containing electrocatalysts that combined the advantages of both 2D and 3D structures remains a significant challenge. Here, an approach to systematically produce porous Fe-doped Pd nanosheet assemblies (NSAs) with a geometry tuning from PdFe hollow nanospheres (HNSs), PdFe nanocages (NCs), to PdFe nanoplates (NPs) is reported. The inherent ultrathin and porous features endow these PdFe catalysts with excellent electrocatalytic performance. As a result, the optimized 3D PdFe NCs show a much-improved methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR) activities in comparison with PdFe HNSs, Pd NPs, and commercial Pd/C catalysts. Moreover, these PdFe nanocatalysts also display greatly enhanced electrocatalytic stability, which can endure 500 cycles with negligible activity loss and structural changes. The mechanism investigations reveal that the introduced Fe atom efficiently modulates the electronic structure of Pd, leading to the downshift of the d-band center of Pd, which is beneficial for the adsorption of reactants. Moreover, the porous nanosheet assembly structure can provide rich mass and electron transfer channels, further boosting the improvement of electrocatalytic performance.

中文翻译：

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纳米结构的多孔铁掺杂Pd纳米片组件，用于有效的甲醇和乙醇电催化。

尽管在2D和3D含Pd纳米材料的控制合成方面已经取得了巨大的成功，但要开发出结合了2D和3D结构优点的新型含Pd电催化剂，仍然是一个巨大的挑战。在这里，报告了一种系统地生产多孔Fe掺杂的Pd纳米片组件（NSA）的方法，其几何形状从PdFe空心纳米球（HNSs），PdFe纳米笼（NCs）到PdFe纳米板（NPs）进行了调整。固有的超薄和多孔特性使这些PdFe催化剂具有出色的电催化性能。结果，与PdFe HNS，Pd NP和商用Pd / C催化剂相比，优化的3D PdFe NCs显示出大大改善的甲醇氧化反应（MOR）和乙醇氧化反应（EOR）活性。而且，这些PdFe纳米催化剂还显示出大大增强的电催化稳定性，可以忍受500次循环，而活性损失和结构变化可忽略不计。机理研究表明，引入的Fe原子有效地调节了Pd的电子结构，导致Pd d谱带中心的下移，这有利于反应物的吸附。而且，多孔纳米片组装结构可以提供丰富的质量和电子转移通道，进一步促进了电催化性能的提高。这有利于反应物的吸附。而且，多孔纳米片组装结构可以提供丰富的质量和电子转移通道，进一步促进了电催化性能的提高。这有利于反应物的吸附。而且，多孔纳米片组装结构可以提供丰富的质量和电子转移通道，进一步促进了电催化性能的提高。