Eunbi Park , Eunjik Lee , Jungmin Han , Youngjoo Whang , Yongmin Kwon , Narim Kim , Byeong-Seon An , Namgee Jung , Gu-Gon Park
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引用次数: 0
Abstract
In this study, we developed a straightforward and scalable all-dry synthetic process for carbon shell-encapsulated Pt catalysts (Pt@C/C) and analyzed the morphological evolution of the carbon shell at various heat-treatment temperatures. We investigated the impact of these morphological changes on the catalytic activity and durability for the oxygen reduction reaction (ORR). The synthesis process involved ball-milling Pt(acac)2 and carbon black, followed by heat treatment under nitrogen at 200–800 °C. The resulting Pt@C/C samples exhibited an ultrathin carbon shell thickness of less than 1 nm and Pt nanoparticles (2–4 nm) uniformly dispersed on the carbon support. In-situ heating transmission electron microscopy revealed critical morphological transitions: thin amorphous carbon shells (<1 nm) at 200 °C, partial shell decomposition at 400 °C, and dense graphene layers (1–2 layers) at temperatures ≥ 600 °C. Pt@C/C samples prepared at 200 and 400 °C exhibited superior mass and specific ORR activities compared to Pt/C, attributed to the uniform size of Pt nanoparticles and the carbon shell mitigating ionomer poisoning. The carbon shells maintained integrity during 30,000 cycles of accelerated stress test, minimizing Pt particle growth and ensuring superior durability over Pt/C. This method eliminates the need for high temperatures (>600 °C) and additional etching, achieving outstanding catalytic activity and durability at temperatures ≤ 400 °C.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.