Simultaneously achieving high activity and robust stability is still challenging for direct methanol fuel cells in practical applications. Although noble metal Pt has been applied as an electrocatalyst, it still suffers from low stability and high cost, which significantly limits its wide applications on a large scale. Here, a series of Pt–Ln/C (Ln = La, Ce, Pr, Nd) nanoalloy catalysts were synthesized to improve the electroactivity towards methanol oxidation and suppress the CO poisoning effect of Pt. DFT calculations have unravelled the different electronic structures of different Pt₅Ln samples, in which the optimal d–f coupling in Pt₅Ce leads to significant improvements in both electroactivity and selectivity. Such an electronic structure also effectively suppresses the CO poisoning effect during the MOR. Pt₅Ce/C shows the best performance, with a specific activity of 32.74 mA cm_Pt⁻², which is 11.1 times higher than that of commercial Pt/C (2.94 mA cm_Pt⁻²). This work demonstrates the critical promotion effect of lanthanide elements in the electroactivity of Pt due to the electronic structure perturbation, which provides new ideas for the design of efficient lanthanide alloy catalysts.

中文翻译：

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用于增强甲醇氧化反应活性的 Pt-Ln（La、Ce、Pr ​​和 Nd）合金中的镧系元素电子扰动

同时实现高活性和稳健稳定性对于直接甲醇燃料电池在实际应用中仍然具有挑战性。尽管贵金属Pt已被用作电催化剂，但它仍然存在稳定性低、成本高的问题，这极大地限制了其在大规模上的广泛应用。在这里，合成了一系列 Pt–Ln/C（Ln = La、Ce、Pr、Nd）纳米合金催化剂，以提高对甲醇氧化的电活性并抑制 Pt 的 CO 中毒效应。DFT计算已经解开不同Pt组成的不同的电子结构₅ LN样品，其中，所述最优d-f的在铂联接₅Ce导致电活性和选择性的显着改善。这种电子结构也有效地抑制了 MOR 过程中的 CO 中毒效应。Pt ₅ Ce/C表现出最好的性能，比活度为32.74 mA cm _Pt ^-2，比商业Pt/C（2.94 mA cm _Pt ^-2）高11.1倍。这项工作证明了镧系元素由于电子结构扰动而对 Pt 电活性的关键促进作用，这为设计高效的镧系合金催化剂提供了新思路。