Mechanistic Insights on Sulfide-Adsorption Enhanced Activity of Methanol Electro-Oxidation on Pt Nanoparticles

作者：Park In Su; Atienza Dianne Osena; Hofstead Duffy Augusta M; Chen Dejun; Tong YuYe J^*

来源：ACS Catalysis, 2012, 2(1): 168-174.

DOI：10.1021/cs200546f

• Pt electrocatalyst
• sulfide adsorption
• enhanced methanol electro-oxidation
• parallel reaction pathway

The effect of adsorbed sulfide (S-ada(2-)) on methanol (MeOH) electro-oxidation reaction (MOR) taking place on carbon-supported Pt nanoparticles (NPs) was investigated using electrochemical and attenuated-total-reflection (ATR)-FTIR; spectroscopic techniques. The observed substantial enhancement in MOR activity per active site was rationalized by an enhanced parallel reaction pathway by the S2- adsorption that did not lead to poisonous CO. Moreover, there were delayed/suppressed adsorption of electrolyte anions and oxygen-containing species and increased amount of isolated free water monomers caused by the sulfide adsorption-induced more negatively charged Pt sites, which led to more available active sites, weakened bonding interaction between the Pt NPs and oxygen-containing species, and more active water species for MOR along the parallel reaction pathway.

• 出版日期2012-1