Probing Interfacial Electronic and Catalytic Properties on Well-Defined Surfaces by Using InSitu Raman Spectroscopy

被引:76
作者
Wang, Ya-Hao [1 ]
Liang, Miao-Miao [2 ]
Zhang, Yue-Jiao [1 ]
Chen, Shu [2 ]
Radjenovic, Petar [1 ]
Zhang, Hua [1 ]
Yang, Zhi-Lin [2 ]
Zhou, Xiao-Shun [3 ]
Tian, Zhong-Qun [1 ]
Li, Jian-Feng [1 ,2 ,4 ]
机构
[1] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, iChEM,MOE Key Lab Spectrochem Anal & Instrumentat, Xiamen 361005, Peoples R China
[2] Xiamen Univ, Dept Phys, Res Inst Biomimet & Soft Matter, Xiamen 361005, Peoples R China
[3] Zhejiang Normal Univ, Coll Chem & Life Sci, Key Lab, Minist Educ Adv Catalysis Mat, Jinhua 321004, Peoples R China
[4] Xiamen Univ, Shenzhen Res Inst, Shenzhen 518000, Peoples R China
关键词
electronic structure; gold; heterogeneous catalysis; nanoparticles; shell-isolated nanoparticle-enhanced Raman spectroscopy; METHANOL OXIDATION REACTION; SINGLE-CRYSTAL SURFACES; OXYGEN REDUCTION; FORMIC-ACID; PLATINUM SURFACES; INITIAL-STAGES; AU-CORE; ELECTROOXIDATION; NANOPARTICLES; DEPOSITION;
D O I
10.1002/anie.201805464
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Heterogeneous metal interfaces play a key role in determining the mechanism and performance of catalysts. However, insitu 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 CN stretch ((NC)) 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, insitu electrochemical SHINERS studies showed that the electronic effects weaken Pt-C/Pd-C bonds, leading to improved surface activity towards CO electrooxidation.
引用
收藏
页码:11257 / 11261
页数:5
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