Support Effects in Single-Atom Platinum Catalysts for Electrochemical Oxygen Reduction

作者：Sungeun Yang, Young Joo Tak, Jiwhan Kim, Aloysius Soon, Hyunjoo Lee · 发表于：ACS Catalysis · 年份：2016 · DOI：10.1021/acscatal.6b02899 · 被引用次数：444 · 研究领域：Electrocatalysts for Energy Conversion、Catalytic Processes in Materials Science、Nanomaterials for catalytic reactions

Single-atom catalysts (SACs) provide an ideal platform for reducing noble-metal usage. SACs also exhibit unusual catalytic properties due to the absence of a metal surface. The role of the support may have a significant effect on the catalytic properties, similar to that of the ligand molecules in homogeneous catalysts. Here, the support effect was demonstrated by preparing a single-atom platinum catalyst on two different supports: titanium carbide (Pt1/TiC) and titanium nitride (Pt1/TiN). The formation of single-atom Pt was confirmed by STEM, EXAFS, and in situ IR spectroscopy. Pt1/TiC showed higher activity, selectivity, and stability for electrochemical H 2 O 2 production than Pt1/TiN. Density functional theory calculations presented that oxygen species have strong affinity into Pt1/TiN, possibly acting as surface poisoning species, and Pt1/TiC preserves oxygen–oxygen bonds more with higher selectivity toward H 2 O 2 production. This work clearly shows that the support in SACs actively participates in the surface reaction and does not just act as anchoring sites for single atoms.