Probing Interfacial Electronic and Catalytic Properties on Well‐Defined Surfaces by Using In Situ Raman Spectroscopy |
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Authors: | Ya‐Hao Wang Miao‐Miao Liang Yue‐Jiao Zhang Shu Chen Petar Radjenovic Dr Hua Zhang Prof Zhi‐Lin Yang Prof Xiao‐Shun Zhou Prof Zhong‐Qun Tian Prof Jian‐Feng Li |
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Institution: | 1. The MOE Key Laboratory of Spectrochemical Analysis and Instrumentation, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China;2. Department of Physics, Research Institute for Biomimetics and Soft Matter, Xiamen University, Xiamen, China;3. Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Life Sciences, Zhejiang Normal University, Jinhua, China;4. Shenzhen Research Institute of Xiamen University, Shenzhen, China |
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Abstract: | Heterogeneous metal interfaces play a key role in determining the mechanism and performance of catalysts. However, in situ characterization of such interfaces at the molecular level is challenging. Herein, two model interfaces, Pd and Pt overlayers on Au single crystals, were constructed. The electronic structures of these interfaces as well as effects of crystallographic orientation on them were analyzed by shell‐isolated nanoparticle‐enhanced Raman spectroscopy (SHINERS) using phenyl isocyanide (PIC) as a probe molecule. A clear red shift in the frequency of the C≡N stretch (νNC) was observed, which is consistent with X‐ray photoelectron spectroscopy (XPS) data and indicates that the ultrathin Pt and Pd layers donate their free electrons to the Au substrates. Furthermore, in situ electrochemical SHINERS studies showed that the electronic effects weaken Pt?C/Pd?C bonds, leading to improved surface activity towards CO electrooxidation. |
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Keywords: | electronic structure gold heterogeneous catalysis nanoparticles shell-isolated nanoparticle-enhanced Raman spectroscopy |
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