Zhang Shaohui, Liu Suying, Cao Wei, Luo Juan, Gu Yuke, Liu Xuanzhi, Tan Pengfei, Wang Ziyu, Pan Jun
State Key Laboratory of Powder Metallurgy, Central South University, 932 Lushan Road, Changsha 410083, China.
State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.
J Colloid Interface Sci. 2024 Dec;675:1108-1118. doi: 10.1016/j.jcis.2024.07.171. Epub 2024 Jul 22.
There are currently almost no ternary platinum-based nanosheets used for acidic oxygen reduction reactions (ORR) due to the difficulty in synthesizing ternary nanosheets with high Pt content. In this work, several ultrathin platinum-palladium-copper nanosheets (PtPdCu NSs) with a thickness of around 1.90 nm were prepared via a microwave heating-assisted method. Microwave heating allows a large number of Pt atoms to deposit into PdCu nanosheets, forming Pt-based ternary nanosheets with high Pt content. Among them, PtPdCu NSs catalyst displays the highest mass activity (MA) measured in 0.1 M HClO of 0.932 A/mg which is 8.6 times of that Pt/C. Besides, PtPdCu NSs catalyst also exhibits excellent stability with an extremely low MA attenuation after 80,000 cycles accelerated durability testing (ADT) tests. In the single cell tests, the PtPdCu NSs catalyst manifests higher maximum power density of 796 mW cm than Pt/C of 606 mW cm. Density functional theory (DFT) calculations indicate the weaker adsorption between Pt and O-species in PtPdCu NSs leads to a significant enhancement of ORR activity. This study provides a new strategy to design and prepare ultrathin Pt-based trimetallic nanosheets as efficient and durable ORR catalysts.
由于难以合成具有高铂含量的三元纳米片,目前几乎没有用于酸性氧还原反应(ORR)的三元铂基纳米片。在这项工作中,通过微波加热辅助方法制备了几种厚度约为1.90nm的超薄铂-钯-铜纳米片(PtPdCu NSs)。微波加热使大量铂原子沉积到PdCu纳米片中,形成具有高铂含量的铂基三元纳米片。其中,PtPdCu NSs催化剂在0.1M HClO中测得的最高质量活性(MA)为0.932A/mg,是Pt/C的8.6倍。此外,PtPdCu NSs催化剂在80000次加速耐久性测试(ADT)后也表现出优异的稳定性,MA衰减极低。在单电池测试中,PtPdCu NSs催化剂的最大输出功率密度为796mW/cm²,高于Pt/C的606mW/cm²。密度泛函理论(DFT)计算表明,PtPdCu NSs中Pt与氧物种之间较弱的吸附导致ORR活性显著增强。该研究为设计和制备超薄铂基三金属纳米片作为高效耐用的ORR催化剂提供了一种新策略。