Microstructurally distorted Pt-based nanoalloys with unusual structural defects like Guinier–Preston (GP) zones with in situ coherency strain fields may be suitable for substantially improving their electrocatalytic performance for the oxygen reduction reaction (ORR) in acidic conditions. Herein, GP zones contributing PtCu nanoalloys were first fabricated by additive manufacturing, starting with the formation of metallic Cu clusters as orderly crystal nuclei on ZIF-8-derived carbon, followed by the additive manufacturing of chemically reduced Pt and Cu on the formed clusters in ethylene glycol at 190 °C. The atomic-scale GP zones give rise to high-level coherent strain fields across the nanocrystals, boosting the ORR kinetics. This catalyst exhibits an ultrahigh oxygen reduction half-wave potential of 0.934 V (vs RHE) and a mass activity (MA) of 0.68 A mg_Pt^–1. After the accelerated degradation test of 50,000 cycles, the achieved MA improved instead of decreasing, rising from 0.68 to 0.89 A mg_Pt^–1, surpassing that of commercial Pt/C significantly. The significantly improved activity is attributed to the coherency strain fields reshaping the band structure and reconstructing a favorable charge density for active Pt sites. Importantly, the interface-anchored GP zones, maintaining a completely coherent relationship with the matrix, can effectively impede metal atom migration, segregation, or leaching, thus enhancing long-term stability. Therefore, the novel GP-type alloys may pave another way for designing advanced catalysts in the realm of current energy storage and conversion fields like fuel cells.

中文翻译：

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具有 PtCu 纳米晶体的 Guinier-Preston 区：相干应变场重塑氧还原电催化的能带结构


具有不寻常结构缺陷的微结构变形 Pt 基纳米合金，如具有原位相干应变场的 Guinier-Preston （GP） 区，可能适用于大幅提高其在酸性条件下氧还原反应 （ORR） 的电催化性能。在此，贡献 PtCu 纳米合金的 GP 区首先通过增材制造制造，首先在 ZIF-8 衍生的碳上形成金属铜簇作为有序的晶核，然后在 190 °C 下在乙二醇中形成的团簇上化学还原的 Pt 和 Cu 的增材制造。 原子尺度的 GP 区在纳米晶体上产生高水平的相干应变场，从而增强 ORR 动力学。该催化剂具有 0.934 V （vs RHE） 的超高氧还原半波电位和 0.68 A mg_Pt^–1 的质量活性 （MA）。经过 50,000 次循环的加速降解测试后，实现的 MA 不但没有下降，反而有所提高，从 0.68 A mg ^Pt-1 上升到 0.89 A mg，明显超过了商业 Pt/C。活性的显著改善归因于相干应变场重塑了能带结构并重建了活性 Pt 位点的有利电荷密度。重要的是，界面锚定的 GP 区与基体保持完全连贯的关系，可以有效阻止金属原子迁移、偏析或浸出，从而增强长期稳定性。因此，新型 GP 型合金可能为当前储能和转换领域（如燃料电池）领域的先进催化剂设计铺平了另一条道路。