首页|Al2O3负载Pt基催化剂表面动态变化的谱学研究

Al2O3负载Pt基催化剂表面动态变化的谱学研究

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明确多相催化剂表面在反应过程的动态变化对催化剂的优化、设计有重要意义.我们通过控制Pt的不同负载量制备了一系列Al2O3负载的Pt/Al2O3催化剂,利用X-射线衍射、X-光电子能谱、球差扫描电镜、CO-探针的红外光谱、低能离子散射谱、程序升温氧化和拉曼光谱等研究Pt/Al2O3的表面结构和反应过程中的变化,以丙烷直接脱氢(PDH)反应为探针,考察反应过程存在"诱导"期的表面动态变化,特别是表面积碳、表面形貌、活性位点等的演化.进而与其催化反应性能关联,发现Pt纳米粒子(NP)和团簇上丙烷易深度脱氢或断裂C-C键生成CH4的同时形成积碳、随后失去活性;而孤立的Pt单原子位点(SAC)上不易生成积碳、是丙烯生成的关键活性位.
Spectroscopic Study of Surface Dynamics of Al2O3 Supported Pt-Catalysts
Understanding the dynamic changes of heterogeneous catalyst under reaction conditions is very important for improving the catalyst and designing a new catalyst.In present study,a series of A12O3 supported Pt/Al2O3 catalysts were prepared with various Pt loadings.Surface structures and changes were studied by the X-ray diffraction(XRD),X-ray photoemission spectroscopy(XPS),high-angle annular dark field scanning transmission electron microscopy(HAADF-STEM),CO probed Fourier transform infrared spectroscopy(CO-FTIR),low energy ion scattering spectroscopy(LEIS),temperature programmed oxidation of carbon(TPOC)and Raman spectroscopy.Propane dehydrogenation(PDH)was used as a probe reaction.Surface dynamics,especially coke formation,surface morphology and active sites were investigated,and correlated with catalytic performance.It was found that Pt/Al2O3 catalysts underwent an'induction'period for PDH.Propane was easy to deeply dehydrogenate,broke C-C bond on Pt nanoparticles(NP)and clusters to form CH4 and coke,resulted in a lower activity.In contrast,the isolated Pt single-atom central sites(SAC)were not easy to form coke,and would mainly be the active sites for propylene formation.

surface dynamicsin-situ characterizationpropane dehydrogenationPt-based catalystsingle-atom site catalyst

何念秋、郑燕萍、陈明树

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厦门大学化学化工学院固体表面物理化学国家重点实验室,福建厦门 361005

表面动态过程 原位表征 丙烷脱氢 Pt基催化剂 单原子催化剂

国家重点研发计划国家重点研发计划国家自然科学基金国家自然科学基金

2020YFB06064012021YFA15028012213200412241502

2024

分子催化
中国科学院兰州化学物理研究所

分子催化

CSTPCD北大核心
影响因子:2.622
ISSN:1001-3555
年,卷(期):2024.38(1)
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