Forced-flow atomic layer deposition nanolamination is employed to fabricate Pt-Ni nanoparticles on XC-72, with the compositions ranging from Pt₉₄Ni₆ to Pt₆₇Ni₃₃. Hydrogen is used as a co-reactant for depositing Pt and Ni. The growth rate of Pt is slower than that using oxygen reactant, and the growth exhibits preferred orientation along the (111) plane. Ni shows much slower growth rate than Pt, and it is only selectively deposited on Pt, not on the substrate. Higher ratios of Ni would hinder subsequent stacking of Pt atoms, resulting in lower overall growth rate and smaller particles (1.3–2.1 nm). Alloying of Pt with Ni causes shifted lattice that leads to larger lattice parameter and d-spacing as Ni fraction increases. From the electronic state analysis, Pt 4f peaks are shifted to lower binding energies with increasing the Ni content, suggesting charge transfer from Ni to Pt. Schematic of the growth behavior is proposed. Most of the alloy nanoparticles exhibit higher electrochemical surface area and oxygen reduction reaction activity than those of commercial Pt. Especially, Pt₈₃Ni₁₇ and Pt₈₇Ni₁₃ show excellent mass activities of 0.76 and 0.59 A mg_Pt⁻¹, respectively, higher than the DOE target of 2025, 0.44 A mg_Pt⁻¹.

中文翻译：

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原子层在氢中沉积纳米层压制备的 Pt-Ni 合金纳米颗粒的形成特性


采用强制流原子层沉积纳米层沉积在 XC-72 上制备 Pt-Ni 纳米颗粒，其成分范围为 Pt₉₄Ni₆ 至 Pt₆₇Ni₃₃。氢用作沉积 Pt 和 Ni 的共反应物。Pt 的生长速率比使用氧反应物的生长速率慢，并且沿 （111） 平面的生长表现出优先方向。Ni 的生长速度比 Pt 慢得多，并且它只是选择性地沉积在 Pt 上，而不是衬底上。较高的 Ni 比率会阻碍 Pt 原子的后续堆叠，从而导致较低的总生长速率和更小的颗粒 （1.3–2.1 nm）。Pt 与 Ni 的合金化会导致晶格偏移，随着 Ni 分数的增加，导致更大的晶格参数和 d 间距。从电子状态分析中，随着 Ni 含量的增加，Pt 4f 峰转移到较低的结合能，表明电荷从 Ni 转移到 Pt。大多数合金纳米颗粒表现出比商业 Pt 更高的电化学表面积和氧还原反应活性。特别是，Pt₈₃Ni₁₇ 和 Pt₈₇Ni₁₃ 分别显示出 0.76 和 0.59 A mg ^Pt-1 的优异质量活性，高于 DOE 目标 2025 年的 0.44 A mg ^Pt-1。