摘要

Transformation of various oxygen species adsorbed on electrolytic silver surface pretreated by pure oxygen at 423 similar to 973 K under ambient pressure was observed for the first time by in situ confocal microprobe Raman spectroscopy. Ag-O-2 species can transform into Ag[O-O](-) species slowly at temperatures below 423 K. Once the temperature rises to 423 K, the transformation of Ag[O-O](-) to Ag-O(alpha) species takes place. With further increase of temperature, Ag-O(alpha) species first transforms to Ag-O-O-Ag and then to Ag-O(gamma) species which is the most stable oxygen species on the silver surface and can be maintained even above 973 K. As for the practical reaction system, the adsorbed molecular oxygen was found to be present on the silver surface at low temperature. It transforms to Ag-O(alpha) species under similar conditions as those for the partial epoxidation of ethylene, and then transforms to Ag-O(gamma) oxygen species under conditions similar to those for selective oxidation of methanol to formaldehyde. A possible mechanism for the detailed transformation of oxygen species was also proposed.

  • 出版日期2006-2
  • 单位复旦大学; 中国石油化工股份有限公司上海石油化工研究院