Diesel emission fluid (DEF) soaking and urea deposits on selective catalytic reduction (SCR) catalysts are critical issues for real diesel engine NH3-SCR systems. To investigate the impact of DEF soaking and urea ...Diesel emission fluid (DEF) soaking and urea deposits on selective catalytic reduction (SCR) catalysts are critical issues for real diesel engine NH3-SCR systems. To investigate the impact of DEF soaking and urea deposits on SCR catalyst performance, fresh Cu-zeolite catalyst samples were drilled from a full-size SCR catalyst. Those samples were impregnated with DEF solutions and subsequently hydrothermally treated to simulate DEF soaking and urea deposits on real SCR catalysts during diesel engine operations. Their SCR performance was then evaluated in a flow reactor with a four-step test protocol. Test results show that the DEF soaking leached some Cu from the SCR catalysts and slightly reduced their Cu loadings. The loss of Cu and associated metal sites on the catalysts weakened their catalytic oxidation abilities and caused lower NO/NI-I3 oxidation and lower high-temperature N20 selectivity. Lower Cu loading also made the catalysts less active to the decomposition of surface ammonium nitrates and decreased low-temperature N20 selectivity. Cu loss during DEF impregnation released more acid sites on the surface of the catalysts and increased their acidities, and more NH3 was able to be adsorbed and involved in SCR reactions at medium and high temperatures. Due to lower NH3 oxidation and higher NH3 storage, the DEF-impregnated SCR catalyst samples showed higher NOx conversion above 400 ℃ compared with the non-soaked one. The negative impact of urea deposits during DEF impregnation was not clearly observed, because the high-temperature hydrothermal treatment helped to remove the urea deposits.展开更多
基金Project supported by the National High-Tech R&D Program(863 Program)of China(No.2013AA065301)the Fundamental Research Funds for the Central Universities,and the State Key Laboratory of Clean Energy Utilization at Zhejiang University(No.ZJUCEU2016006),China
文摘Diesel emission fluid (DEF) soaking and urea deposits on selective catalytic reduction (SCR) catalysts are critical issues for real diesel engine NH3-SCR systems. To investigate the impact of DEF soaking and urea deposits on SCR catalyst performance, fresh Cu-zeolite catalyst samples were drilled from a full-size SCR catalyst. Those samples were impregnated with DEF solutions and subsequently hydrothermally treated to simulate DEF soaking and urea deposits on real SCR catalysts during diesel engine operations. Their SCR performance was then evaluated in a flow reactor with a four-step test protocol. Test results show that the DEF soaking leached some Cu from the SCR catalysts and slightly reduced their Cu loadings. The loss of Cu and associated metal sites on the catalysts weakened their catalytic oxidation abilities and caused lower NO/NI-I3 oxidation and lower high-temperature N20 selectivity. Lower Cu loading also made the catalysts less active to the decomposition of surface ammonium nitrates and decreased low-temperature N20 selectivity. Cu loss during DEF impregnation released more acid sites on the surface of the catalysts and increased their acidities, and more NH3 was able to be adsorbed and involved in SCR reactions at medium and high temperatures. Due to lower NH3 oxidation and higher NH3 storage, the DEF-impregnated SCR catalyst samples showed higher NOx conversion above 400 ℃ compared with the non-soaked one. The negative impact of urea deposits during DEF impregnation was not clearly observed, because the high-temperature hydrothermal treatment helped to remove the urea deposits.