Precursor-EngineeredStrategy for Constructing SupportedTetra-Atom Pt Clusters to Boost Propane Dehydrogenation under DirectResistive Heating

作者：Panpan Li (484033), Guangsheng Liu, Najie Zhuang, Jingjing Tu (16849542), Taotao Gao (2888879), Xiaoyang Ren, Ruhao Wang (10903733), Haifeng Jiang (298743), Yanru Zhu (4443175), Wan-Lu Li (1412359), J He, Shubo Tian · 发表于：Figshare · 年份：2026 · DOI：10.1021/acsnano.6c06516.s001 · 研究领域：Catalysis and Oxidation Reactions、Catalytic Processes in Materials Science、Catalysts for Methane Reforming

The commercial platinum-based catalysts used in propane dehydrogenation (PDH) reactions face challenges such as ambiguous active sites, low stability, and poor propylene selectivity. Atomically precise platinum catalysts, featuring well-defined active structures and controllable electronic properties, offer an effective approach to addressing these issues. Herein, we successfully constructed atomically precise Pt 4 nanoclusters stabilized on oxygen-functionalized carbon nanotubes (Pt 4 /OCNT) through a precursor-engineered strategy. Combined advanced characterization and density functional theory (DFT) calculations revealed that the Pt 4 clusters are consistent with the tetrahedral model stabilized by Pt–C/O bonds with the support. Under direct resistive heating for PDH at 500 °C, Pt 4 /OCNT reached 99.6% propylene selectivity while exhibiting the highest space-time conversion, demonstrating superior performance compared to both atomically dispersed Pt 1 /OCNT and industrial Pt/C catalysts. In situ infrared characterization combined with DFT calculations further demonstrated that Pt 4 /OCNT effectively stabilizes key dehydrogenation intermediates and transition states through multisite cooperative interactions, thereby lowering the activation barrier for PDH. Furthermore, the weak adsorption of propylene on Pt 4 /OCNT suppresses side reactions and enhances selectivity. This work presents a precursor-engineered strategy for constructing atomically precise supported Pt 4 /OCN...