Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200438, China.
PLA Naval Medical Center, 5 Panshan Rd, Shanghai 200052, China.
J Colloid Interface Sci. 2023 Oct 15;648:719-726. doi: 10.1016/j.jcis.2023.06.036. Epub 2023 Jun 10.
Self-assembled superstructures composed of nanocrystals (NCs) have shown immense potential for enhancing the performance in electrocatalytic applications. However, there has been limited research on the self-assembly of platinum (Pt) into low-dimensional superstructures as efficient electrocatalysts for oxygen reduction reaction (ORR). In this study, we designed a unique tubular superstructure composed of monolayer or sub-monolayer carbon-armored platinum nanocrystals (Pt NCs) using a template-assisted epitaxial assembly approach. The organic ligands on the surface of Pt NCs were in situ carbonized, resulting in few-layer graphitic carbon shells that encapsulate Pt NCs. Due to their monolayer assembly and tubular geometry, the Pt utilization of the supertubes was 1.5 times higher than that of conventional carbon-supported Pt NCs. As a result, such Pt supertubes exhibit remarkable electrocatalytic performance for the ORR in acidic media, with a high half-wave potential of 0.918 V and a high mass activity of 181 A g at 0.9 V, which are comparable to commercial carbon-supported Pt (Pt/C) catalysts. Furthermore, the Pt supertubes demonstrate robust catalytic stability, as confirmed by long-term accelerated durability tests and identical-location transmission electron microscopy. This study presents a new approach to designing Pt superstructures for highly efficient and stable electrocatalysis.
自组装的纳米晶体（NCs）超结构在增强电催化应用性能方面显示出了巨大的潜力。然而，将铂（Pt）自组装成低维超结构作为高效氧还原反应（ORR）电催化剂的研究还很有限。在这项研究中，我们使用模板辅助外延组装方法设计了一种由单层或亚单层碳包覆铂纳米晶体（Pt NCs）组成的独特管状超结构。Pt NCs 表面的有机配体原位碳化，形成了包裹 Pt NCs 的少层石墨碳壳。由于其单层组装和管状几何形状，超管的 Pt 利用率比传统的碳载 Pt NCs 高 1.5 倍。因此，这种 Pt 超管在酸性介质中对 ORR 表现出显著的电催化性能，半波电位为 0.918 V，在 0.9 V 时质量活性为 181 A g，可与商业碳载 Pt（Pt/C）催化剂相媲美。此外，Pt 超管通过长期加速耐久性测试和同位置透射电子显微镜证实了其具有强大的催化稳定性。本研究提出了一种设计高效稳定电催化剂的 Pt 超结构的新方法。
