Parnigotto Mattia, Dal Sasso Gregorio, Berretti Enrico, Mazzucato Marco, Bertolotti Federica, Lavacchi Alessandro, Dalconi Maria Chiara, Gavioli Luca, Durante Christian
Department of Chemical Sciences, University of Padova, Via Marzolo 1, Padova, 35131, Italy.
Italian National Research Council, Institute of Geosciences and Earth Resources, Corso Stati Uniti 4, Padova, 35121, Italy.
Small. 2025 Jun;21(25):e2403127. doi: 10.1002/smll.202403127. Epub 2025 May 5.
This study emphasizes the effect of CeO on the Pt nanoparticle (NP) dimension, stability, and activity versus the oxygen reduction reaction. It is demonstrated that the one-pot synthesis of Pt NPs along with CeO NPs over carbon support produces small Pt NPs (2 nm) with higher activity, than the sole Pt NPs, thanks to the cooperative interaction exerted by CeO. This is nicely demonstrated by using synchrotron wide-angle X-ray total scattering and advanced data analysis, monitoring the in situ nucleation and growth of Pt NPs in the presence of preformed CeO NPs or of a Ce precursor. Raman, X-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy analyses are carried out to support the formation of oxygen vacancies responsible for the metal-support interaction. Moreover, the most effective catalyst, PtCeO/C250 (mass activity: MA = 423 Ag; specific activity: SA = 446 µAcm), exhibits activity comparable to the commercial benchmark Pt/C, yet significantly greater stability as demonstrated by accelerated stress tests conducted on gas diffusion electrode. Specifically, PtCeO/C250 retains 62% ± 7% of its MA and 79% ± 9% of its SA, compared to 43% ± 5% and 62% ± 7%, respectively, for the benchmark.
本研究强调了CeO对铂纳米颗粒（NP）尺寸、稳定性以及与氧还原反应相关活性的影响。结果表明，在碳载体上一锅法合成铂纳米颗粒与CeO纳米颗粒，由于CeO的协同作用，生成的小尺寸铂纳米颗粒（2纳米）比单独的铂纳米颗粒具有更高的活性。利用同步辐射广角X射线全散射和先进的数据分析，监测在预先形成的CeO纳米颗粒或Ce前驱体存在下铂纳米颗粒的原位成核和生长，很好地证明了这一点。进行拉曼光谱、X射线光电子能谱和高分辨率透射电子显微镜分析，以支持负责金属-载体相互作用的氧空位的形成。此外，最有效的催化剂PtCeO/C250（质量活性：MA = 423 A/g；比活性：SA = 446 μA/cm²），其活性与商业基准Pt/C相当，但在对气体扩散电极进行的加速应力测试中显示出明显更高的稳定性。具体而言，PtCeO/C250保留了其MA的62%±7%和SA的79%±9%，相比之下，基准Pt/C分别为43%±5%和62%±7%。
