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Probing the Local Bonding at the Pt/γ-Al2O3 Interface
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-04-13 , DOI: 10.1021/acs.jpcc.9b12029
Henry O. Ayoola 1 , Cecile S. Bonifacio 1 , Qing Zhu 1, 2 , Cheng-Han Li 3 , Stephen D. House 1, 4 , Joshua J. Kas 5 , Joerg Jinschek 3 , John J. Rehr 5 , Wissam A. Saidi 2 , Judith C. Yang 1, 4, 6
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-04-13 , DOI: 10.1021/acs.jpcc.9b12029
Henry O. Ayoola 1 , Cecile S. Bonifacio 1 , Qing Zhu 1, 2 , Cheng-Han Li 3 , Stephen D. House 1, 4 , Joshua J. Kas 5 , Joerg Jinschek 3 , John J. Rehr 5 , Wissam A. Saidi 2 , Judith C. Yang 1, 4, 6
Affiliation
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Metal–support interactions significantly affect the performance of heterogeneous catalysts, of which Pt supported on γ-Al2O3 is one of the most widely used. Characterizing the bonding of Pt on the γ-Al2O3 surface is key to fully understanding the catalyst–support interaction. Herein aberration-corrected and monochromated scanning transmission electron microscopy-based electron energy-loss spectroscopy (STEM-EELS) were employed on a model Pt/γ-Al2O3(111) catalyst to locally investigate the bonding between Pt and the γ-Al2O3 support. Differences in the aluminum L2,3-edge and oxygen K-edge EELS near-edge fine structure between spectra acquired at the Pt/γ-Al2O3(111) interface and the bulk γ-Al2O3 served as signatures of the interfacial bonding environment. Fine structure in the interface-localized Al-L2,3 edge suggested a larger fraction of tetrahedrally coordinated Al atoms at the Pt/γ-Al2O3(111) interface, which was confirmed by DFT simulations. The interface-localized O–K edge EELS revealed a prepeak associated with several types of oxygen bonding. To determine the specific interfacial O bonding, O–K edge EELS spectra were simulated from an array of Pt/γ-Al2O3(111) bonding configuration models. The simulated EELS from the interfacial bonding models revealed an O bonding motif consistent with the experimental O–K edge EELS fine structure.
中文翻译：
在铂探测局部粘合/γ-Al系2 ö 3接口
金属-载体相互作用显著影响多相催化剂，其中铂负载于γ-Al的性能2 Ó 3是最广泛使用的一种。表征Pt构成的接合用的γ-Al上2 ö 3表面的关键是充分了解的催化剂-载体的相互作用。本文像差校正和单色扫描透射电子显微镜为基础的电子能量损失光谱法（STEM-EELS）被雇用在模型上的Pt /γ-Al系2 ö 3（111）催化剂，以局部地调查了Pt和γ-之间的结合Al 2 O 3支持。铝L 2,3的差异〜边缘和氧K边缘EELS在了Pt /γ-Al系获得的光谱之间的近边缘精细结构2 ö 3（111）界面和体的γ-Al 2 ö 3担任的界面结合环境的签名。在接口本地化的Al-L精细结构2,3边缘建议在的Pt /γ-Al系四面体配位的Al原子的较大部分2 ö 3（111）的接口，其通过DFT模拟证实。界面局部的O-K边缘EELS揭示了与几种类型的氧键相关的预峰。以确定特定的界面O键，O--K边缘EELS光谱选自Pt的阵列/γ-Al系模拟2 ö 3（111）绑定配置模型。界面键合模型的模拟EELS揭示了与实验的O-K边缘EELS精细结构一致的O键基序。
更新日期：2020-04-13
中文翻译：
在铂探测局部粘合/γ-Al系2 ö 3接口
金属-载体相互作用显著影响多相催化剂，其中铂负载于γ-Al的性能2 Ó 3是最广泛使用的一种。表征Pt构成的接合用的γ-Al上2 ö 3表面的关键是充分了解的催化剂-载体的相互作用。本文像差校正和单色扫描透射电子显微镜为基础的电子能量损失光谱法（STEM-EELS）被雇用在模型上的Pt /γ-Al系2 ö 3（111）催化剂，以局部地调查了Pt和γ-之间的结合Al 2 O 3支持。铝L 2,3的差异〜边缘和氧K边缘EELS在了Pt /γ-Al系获得的光谱之间的近边缘精细结构2 ö 3（111）界面和体的γ-Al 2 ö 3担任的界面结合环境的签名。在接口本地化的Al-L精细结构2,3边缘建议在的Pt /γ-Al系四面体配位的Al原子的较大部分2 ö 3（111）的接口，其通过DFT模拟证实。界面局部的O-K边缘EELS揭示了与几种类型的氧键相关的预峰。以确定特定的界面O键，O--K边缘EELS光谱选自Pt的阵列/γ-Al系模拟2 ö 3（111）绑定配置模型。界面键合模型的模拟EELS揭示了与实验的O-K边缘EELS精细结构一致的O键基序。
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