Single crystal surfaces are ideal substrates for surface science studies, as they exhibit well-defined surface morphology and electronic state and can perfectly match theoretical calculation to uncover the reaction mechanisms and structure-activity relationships at a molecular or atomic level.

We have employed SHINERS technique toin situstudy the electrochemical behavior of different molecules and catalytic reactions at different single crystal surfaces. For example, we havein situinvestigated the adsorption behavior of pyridine, hydrogen, CO at Au(hkl), Pt(hkl), Rh(hkl) single crystal surfaces and revealed the potential dependent electrochemical behaviors of these molecules. We also used thein situSHINERS technique systematically studied the dynamic reaction processes of electrooxidation, ORR, OER and CO₂RR at Au(hkl), Pt(hkl), Cu(hkl) single crystal surfaces and obtained direct spectral evidence of different reaction intermediates. These fundamental insights would greatly deepen the understanding of the catalytic reaction mechanisms at a molecular level. Furthermore, thein situSHINERS technique was applied to study the electronic structure effects at well-defined heterogeneous metal interfaces, such as Pd/Au(hkl) and Pt/Au(hkl).