化学
纳米材料基催化剂
合金
催化作用
拉曼光谱
吸附
电子转移
密度泛函理论
纳米颗粒
化学工程
兴奋剂
光化学
纳米技术
物理化学
计算化学
有机化学
工程类
物理
光学
材料科学
光电子学
作者
Huajie Ze,Xing Chen,Xiaoting Wang,Yaohui Wang,Qingqi Chen,Jintong Lin,Yue-Jiao Zhang,Xia‐Guang Zhang,Zhong‐Qun Tian,Jianfeng Li
摘要
PtNi alloy catalysts have excellent catalytic activity and are considered some of the most promising electrocatalysts capable of replacing pure Pt for the oxygen reduction reaction (ORR). For PtNi alloys, Ni-doping can improve performance by changing the electronic and structural properties of the catalyst surface and its interaction with reaction intermediates. However, to date there is no direct spectral evidence detecting or identifying the effect of Ni on the ORR in PtNi alloy catalysts. Herein, we introduce a surface-enhanced Raman spectroscopic (SERS) “borrowing” strategy for investigating ORR processes catalyzed by Au@PtNi nanoparticles (NPs). The bond vibration of adsorbed peroxide intermediate species (*OOH) was obtained, and the effect of Ni on the interaction between surface Pt and *OOH was studied by varying the Ni content in the alloy. The frequency of the *OOH spectral band has an obvious red-shift with increasing Ni content. Combined with density functional theory (DFT) calculations, we show that Ni-doping can optimize *OOH surface binding on the Pt surface, achieving more efficient electron transfer, thus improving the ORR rate. Notably, these results evidence the SERS borrowing strategy as an effective technique for in situ observations of catalytic processes.
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