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.
State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science, Fudan University, Shanghai 200433, China.
J Colloid Interface Sci. 2023 Sep 15;646:794-801. doi: 10.1016/j.jcis.2023.05.106. Epub 2023 May 21.
While Platinum (Pt)-based electrocatalysts have been extensively studied for the oxygen reduction reaction (ORR), improving their durability remains a challenge. One promising approach is to design structure-defined carbon supports that can uniformly immobilize Pt nanocrystals (NCs). In this study, we present an innovative strategy for constructing three-dimensional ordered, hierarchically porous carbon polyhedrons (3D-OHPCs) as an efficient support for immobilizing Pt NCs. We achieved this by template-confined pyrolysis of a zinc-based zeolite imidazolate framework (ZIF-8) grown within the voids of polystyrene templates, followed by carbonizing the native oleylamine ligands on Pt NCs to produce graphitic carbon shells. This hierarchical structure enables the uniform anchorage of Pt NCs, while enhancing facile mass transfer and local accessibility of active sites. The optimal material with graphitic carbon armor shells on the surface of Pt NCs (CA-Pt), named CA-Pt@3D-OHPCs-1600, shows comparable activities to commercial Pt/C catalysts. Furthermore, it can withstand over 30,000 cycles of accelerated durability tests, owing to the protective carbon shells and hierarchically ordered porous carbon supports. Our study presents a promising approach for designing highly efficient and durable electrocatalysts for energy-based applications and beyond.
虽然基于铂（Pt）的电催化剂已被广泛研究用于氧还原反应（ORR），但其耐久性的提高仍然是一个挑战。一种有前途的方法是设计结构明确的碳载体，可以均匀地固定 Pt 纳米晶体（NCs）。在这项研究中，我们提出了一种构建三维有序、分级多孔碳多面体（3D-OHPCs）的创新策略，作为固定 Pt NCs 的有效载体。我们通过在聚苯乙烯模板的空隙中生长的锌基沸石咪唑酯骨架（ZIF-8）的模板限制热解来实现这一目标，然后碳化 Pt NCs 上的天然油胺配体以生成石墨碳壳。这种分层结构能够均匀地固定 Pt NCs，同时增强了传质的便利性和活性位点的局部可及性。具有 Pt NCs 表面石墨碳装甲壳的最佳材料（CA-Pt），命名为 CA-Pt@3D-OHPCs-1600，与商业 Pt/C 催化剂具有相当的活性。此外，由于保护碳壳和分级有序的多孔碳载体，它可以承受超过 30000 次的加速耐久性测试循环。我们的研究为设计用于能源相关应用及其他领域的高效、耐用的电催化剂提供了一种有前途的方法。
