Wang Yanzhi, Yao Yinghong, Xu Cong, Tang Deqing, Li Yuting, Qiao Zhen-An, Liang Hai-Wei, Liu Ben
Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu, 610064, China.
College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, 610066, China.
Adv Mater. 2025 Feb;37(6):e2416111. doi: 10.1002/adma.202416111. Epub 2024 Dec 18.
Ordered intermetallic nanocatalysts supported on high-surface-area skeletons are of great importance in catalysis and have disclosed notable catalytic activity and stability that are remarkably better than their random alloy counterparts. Ultrafine intermetallic nanocatalysts are synthetically challenging, especially for universal and scaled-up synthesis, because of inevitable sintering and phase separation under high temperatures that promote atomic alloying and ordering. Herein, a universal solid-phase and scaled-up method is reported for synthesizing ultrafine intermetallic nanocatalysts with uniform size distributions and wide compositional spaces confined in ordered mesoporous carbon (OMC) supports, where the strong physical confinement and chemical interaction between metals and sulfur/mesoporous templates remarkably suppress the high-temperature sintering and phase separation even up to 1000 °C. Libraries of intermetallic nanocatalysts are successfully synthesized including 52 combinations of host platinum/palladium/rhodium with 15 guest elements confined in 4 OMC supports. Taking oxygen reduction and hydrogen evolution reactions as examples, the intermetallic PtFe nanocatalysts hold remarkable performance, whose activities reach up to ten times higher than commercial Pt/C and also are comparable to the best electrocatalysts reported recently. This feasible synthetic strategy offers an intermetallic library spanning from binary to senary materials for industrial synthesis and applications.
负载在高表面积骨架上的有序金属间化合物纳米催化剂在催化领域具有重要意义，并且已展现出显著的催化活性和稳定性，明显优于其无序合金对应物。由于在促进原子合金化和有序化的高温下不可避免地发生烧结和相分离，超细金属间化合物纳米催化剂的合成具有挑战性，尤其是对于通用和规模化合成而言。在此，报道了一种通用的固相和规模化方法，用于合成尺寸分布均匀且组成空间广泛的超细金属间化合物纳米催化剂，这些催化剂被限制在有序介孔碳（OMC）载体中，其中金属与硫/介孔模板之间强烈的物理限制和化学相互作用即使在高达1000℃的温度下也能显著抑制高温烧结和相分离。成功合成了金属间化合物纳米催化剂库，包括52种主体铂/钯/铑与15种客体元素的组合，这些组合被限制在4种OMC载体中。以氧还原和析氢反应为例，金属间化合物PtFe纳米催化剂具有卓越的性能，其活性比商业Pt/C高十倍，并且与最近报道的最佳电催化剂相当。这种可行的合成策略为工业合成和应用提供了一个从二元到六元材料的金属间化合物库。
