In situ Raman spectroscopic evidence for oxygen reduction reaction intermediates at platinum single-crystal surfaces

Jin-Chao Dong, Xia-Guang Zhang, Valentín Briega-Martos, Xi Jin, Ji Yang, Shu Chen, Zhi-Lin Yang, Wu De-Yin, Juan Miguel Feliu (), Christopher T. Williams, Zhong-Qun Tian and Jian-Feng Li ()
Additional contact information
Jin-Chao Dong: Xiamen University
Xia-Guang Zhang: Xiamen University
Valentín Briega-Martos: Universidad de Alicante
Xi Jin: Xiamen University
Ji Yang: Xiamen University
Shu Chen: Xiamen University
Zhi-Lin Yang: Xiamen University
Wu De-Yin: Xiamen University
Juan Miguel Feliu: Universidad de Alicante
Christopher T. Williams: University of South Carolina
Zhong-Qun Tian: Xiamen University
Jian-Feng Li: Xiamen University

Nature Energy, 2019, vol. 4, issue 1, 60-67

Abstract: Abstract Developing an understanding of structure–activity relationships and reaction mechanisms of catalytic processes is critical to the successful design of highly efficient catalysts. As a fundamental reaction in fuel cells, elucidation of the oxygen reduction reaction (ORR) mechanism at Pt(hkl) surfaces has remained a significant challenge for researchers. Here, we employ in situ electrochemical surface-enhanced Raman spectroscopy (SERS) and density functional theory (DFT) calculation techniques to examine the ORR process at Pt(hkl) surfaces. Direct spectroscopic evidence for ORR intermediates indicates that, under acidic conditions, the pathway of ORR at Pt(111) occurs through the formation of HO2*, whereas at Pt(110) and Pt(100) it occurs via the generation of OH*. However, we propose that the pathway of the ORR under alkaline conditions at Pt(hkl) surfaces mainly occurs through the formation of O2−. Notably, these results demonstrate that the SERS technique offers an effective and reliable way for real-time investigation of catalytic processes at atomically flat surfaces not normally amenable to study with Raman spectroscopy.

Date: 2019
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DOI: 10.1038/s41560-018-0292-z

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