文献类型：期刊文献

英文题名：Two-Dimensional Submonolayer Pt Clusters with Optimal Pt0-Ptδ+ Sites for Efficient Methylcyclohexane Dehydrogenation

作者：Li, Zhengjian[1];Wang, Mingzhi[1];Yang, Huayue[1];Jia, Yanyan[2,3];Liu, Shumin[1];Yang, Shuangli[4];Chen, Mingshu[4];Wang, Pei[5];Dai, Sheng[2,3];Zhou, Linan[6];Zhao, Yun[1];Chen, Guangxu[1]

机构：[1]South China Univ Technol, State Key Lab Luminescent Mat & Devices, Guangdong Prov Key Lab Atmospher Environm & Pollut, Sch Environm & Energy,Natl Engn Lab VOCs Pollut Co, Guangzhou 510006, Peoples R China;[2]East China Univ Sci & Technol, Frontiers Sci Ctr Materiobiol & Dynam Chem, Feringa Arno Pro Nobel Prize Scientist Joint Res C, Inst Fine Chem,Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Feringa Arno Pro Nobel Prize Scientist Joint Res C, Frontiers Sci Ctr Materiobiol & Dynam Chem,Inst Fi, Joint Int Res Lab Precis Chem & Mol Engn,Sch Chem, Shanghai 200237, Peoples R China;[4]Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Fujian, Peoples R China;[5]Huazhong Agr Univ, Coll Sci, Wuhan 430074, Peoples R China;[6]South China Univ Technol, Spin X Inst, Sch Chem & Chem Engn, State Key Lab Luminescent Mat & Devices, Guangzhou 510641, Peoples R China

年份：2025

卷号：19

期号：39

起止页码：35050

外文期刊名：ACS NANO

收录：;EI(收录号：20261520498995);WOS:【SCI-EXPANDED(收录号:WOS:001578840600001)】；

基金：This work was supported by the National Key Research and Development Program of China (2024YFC3908700), the National Natural Science Foundation of China (22476064 and 22106048), the Guangdong Innovative and Entrepreneurial Research Team Program (2019ZT08L075), the Guangdong Pearl River Talent Program (2019QN01L159), the Guangzhou Basic and Applied Basic Research Program (2022A1515012047), and the National Key R&D Program of China (2021YFA1501900). We acknowledge Dr. Wei-Hsiang Huang, National Synchrotron Radiation Research Center, Taiwan, for help during XAFS measurements.

语种：英文

外文关键词：two-dimensional submonolayer Pt clusters; optimal Pt-0-Pt delta+ interfacial sites; Pt/Al2O3 catalyst; methylcyclohexanedehydrogenation; fixed-bed thermocatalysis; interfacialcatalysis

摘要：Methylcyclohexane dehydrogenation (MCHDH) is vital in hydrogen storage and carriage technologies. However, Pt/Al2O3, as a classic practical catalyst for MCHDH, remains ambiguous regarding the catalytic structure of active Pt sites for C-H activation at the atomic scale due to a shortage of subnanometer characterization. Here, based on comprehensive structural characterizations and density functional theory (DFT) calculations, we demonstrate optimal active Pt sites: two-dimensional (2D) submonolayer clusters (SLCs) interfaced with gamma-Al2O3 with an appropriate ratio of Pt delta+ to Pt-0 to form optimal Pt-0-Pt delta+ interfacial sites that have superior activity for the MCHDH reaction. This SLC's catalyst achieves a reaction rate of up to 29,353 mmol g(Pt)(-1) min(-1) at 320 degrees C, with a 99.98% selectivity for toluene over MCHDH, which is significantly better than that of the corresponding Pt single atoms and conventional Pt nanoparticles (NPs) catalysts. The excellent MCHDH performance of Pt 2D SLCs is attributed to their sufficient 5d-electron domination and the optimal Pt-0-Pt delta+ sites, which facilitate the sequential activation of multiple C-H bonds and toluene desorption. In comparison, the presence of too many continuous Pt-0-Pt-0 sites in Pt 2D SLCs can hinder these processes. Our study highlights that constructing atomic-scale 2D submonolayer metal clusters is a promising strategy for optimizing efficient catalysts with abundant M-0-M delta+ (M = metal) sites, enhancing the catalytic performance for selective C-H bond activation