Lüsi Madis, Erikson Heiki, Käärik Maike, Piirsoo Helle-Mai, Aruväli Jaan, Kikas Arvo, Kisand Vambola, Leis Jaan, Kukli Kaupo, Tammeveski Kaido
Institute of Chemistry, University of Tartu, Ravila 14a, 50411 Tartu, Estonia.
Institute of Physics, University of Tartu, W. Ostwald Str. 1, 50411 Tartu, Estonia.
Nanomaterials (Basel). 2024 Jun 7;14(12):994. doi: 10.3390/nano14120994.
We explored two methods for synthesizing Pd nanoparticles using three different carbide-derived carbon (CDC) support materials, one of which was nitrogen-doped. These materials were studied for oxygen reduction reaction (ORR) in 0.1 M KOH solution, and the resulting CDC/Pd catalysts were characterized using TEM, XRD, and XPS. The citrate method and the polyol method using polyvinylpyrrolidone (PVP) as a capping agent were employed to elucidate the impact of the support material on the final catalyst. The N-doping of the CDC material resulted in smaller Pd nanoparticles, but only in the case of the citrate method. This suggests that the influence of support is weaker when using the polyol method. The citrate method with CDC1, which is predominantly microporous, led to a higher degree of agglomeration and formation of larger particles in comparison to supports, which possessed a higher degree of mesoporosity. We achieved smaller Pd particle sizes using citrate and NaBH compared to the ethylene glycol PVP method. Pd deposited on CDC2 and CDC3 supports showed similar specific activity (SA), suggesting that the N-doping did not significantly influence the ORR process. The highest SA value was observed for CDC1/Pd_Cit, which could be attributed to the formation of larger Pd particles and agglomerates.
我们探索了两种使用三种不同的碳化物衍生碳(CDC)载体材料合成钯纳米颗粒的方法,其中一种是氮掺杂的。研究了这些材料在0.1 M KOH溶液中的氧还原反应(ORR),并使用透射电子显微镜(TEM)、X射线衍射(XRD)和X射线光电子能谱(XPS)对所得的CDC/Pd催化剂进行了表征。采用柠檬酸盐法和以聚乙烯吡咯烷酮(PVP)为封端剂的多元醇法来阐明载体材料对最终催化剂的影响。CDC材料的氮掺杂导致钯纳米颗粒更小,但仅在柠檬酸盐法的情况下如此。这表明使用多元醇法时载体的影响较弱。与具有更高介孔率的载体相比,使用主要为微孔的CDC1的柠檬酸盐法导致更高程度的团聚和更大颗粒的形成。与乙二醇PVP法相比,使用柠檬酸盐和硼氢化钠(NaBH)时我们获得了更小的钯颗粒尺寸。沉积在CDC2和CDC3载体上的钯表现出相似的比活性(SA),这表明氮掺杂并未显著影响ORR过程。观察到CDC1/Pd_Cit的SA值最高,这可能归因于更大的钯颗粒和团聚体的形成。