The effect of the amount of precipitant ammonia on the Cu0/Cu+ratio of Cu/Si O2 prepared by the deposition–precipitation method is investigated. Species at different preparation stages, resulted from the amount of a...The effect of the amount of precipitant ammonia on the Cu0/Cu+ratio of Cu/Si O2 prepared by the deposition–precipitation method is investigated. Species at different preparation stages, resulted from the amount of ammonia used, are identified by the XRD and FTIR techniques. Chrysocolla together with either copper nitrate hydroxide or copper hydroxide coexist in the uncalcined catalysts. Upon calcination, the latter two species are converted to Cu O particles while chrysocolla remains. Following reduction, Cu O is transformed to metallic Cu and chrysocolla is converted to Cu2 O. The value of Cu0/Cu+ratio can be evaluated using the peak areas in their TPR profiles. Hydrogenation of dimethyl oxalate(DMO) to ethylene glycol(EG) shows that the selectivity of EG depends on the Cu0/Cu+ratio. Catalyst prepared with the addition of ammonia solution at n(NH3)/n(Cu2+) = 0.9 for precipitation–deposition gains a more suitable Cu0/Cu+ratio upon reduction and thus has a higher selectivity for EG.展开更多
基金Funding for the present study from the National Basic Research Program of China(973 Program,No.2011CB710800)the Opening Foundation(2014)of Zhejiang Zanyu Technology Co.,Ltd
文摘The effect of the amount of precipitant ammonia on the Cu0/Cu+ratio of Cu/Si O2 prepared by the deposition–precipitation method is investigated. Species at different preparation stages, resulted from the amount of ammonia used, are identified by the XRD and FTIR techniques. Chrysocolla together with either copper nitrate hydroxide or copper hydroxide coexist in the uncalcined catalysts. Upon calcination, the latter two species are converted to Cu O particles while chrysocolla remains. Following reduction, Cu O is transformed to metallic Cu and chrysocolla is converted to Cu2 O. The value of Cu0/Cu+ratio can be evaluated using the peak areas in their TPR profiles. Hydrogenation of dimethyl oxalate(DMO) to ethylene glycol(EG) shows that the selectivity of EG depends on the Cu0/Cu+ratio. Catalyst prepared with the addition of ammonia solution at n(NH3)/n(Cu2+) = 0.9 for precipitation–deposition gains a more suitable Cu0/Cu+ratio upon reduction and thus has a higher selectivity for EG.