摘要
采用溶剂热-热回流两步法制备了金属有机框架材料负载Pd催化剂(Pd/HKUST-1),对催化剂进行表征,考察了其催化苯酚氧化羰基化合成碳酸二苯酯(DPC)反应性能及稳定性。结果表明:Pd物种在HKUST-1载体上的分散性好,平均粒径为2.3 nm;当Pd、苯酚的物质的量比n(Pd)/n(BP)为1/425时,在100℃反应8 h,苯酚转化率为53.8%,DPC选择性为71.3%;回收Pd/HKUST-1再次使用时催化性能降低,主要是由于Pd物种流失造成的。Pd/HKUST-1具有较大的比表面积,一方面增大了反应物分子的内扩散阻力,降低了生成DPC的可能性,导致其选择性较低;另一方面,在反应中流失的Pd组分可再次沉积在催化剂表面,因此Pd/HKUST-1具有一定的稳定性。
A metal-organic framework supported Pd catalyst(Pd/HKUST-1)was prepared by solvothermic and thermal reflux method.The catalyst was characterized and its catalytic performance and stability for the oxidation and carbonylation of phenol into diphenyl carbonate(DPC)were investigated.The results showed that the active Pd species were highly dispersed on HKUST-1 with an average particle size of 2.3 nm.When Pd/phenol was 1/425(molar ratio),53.8%phenol conversion with 71.3%DPC selectivity was obtained at 100℃for 8 h.The catalytic activity of Pd/HKUST-1 reduced when reused due to the loss of Pd during the reaction.Pd/HKUST-1 has large specific surface area,which increases the internal diffusion resistance of reactant molecules and reduces the possibility of DPC formation,resulting in low selectivity.On the other hand,the Pd species lost during the reaction can be redeposited on the catalyst surface,so Pd/HKUST-1 has certain stability.
作者
杨瀚森
王志苗
付增杰
王雪芳
薛伟
YANG Hansen;WANG Zhimiao;FU Zengjie;WANG Xuefang;XUE Wei(Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving,School of Chemical Engineering and Technology,Hebei University of Technology,Tianjin 300130,China;School of Economics and Management,Shijiazhuang Tiedao University,Shijiazhuang 050043,China)
出处
《高校化学工程学报》
EI
CAS
CSCD
北大核心
2023年第4期581-590,共10页
Journal of Chemical Engineering of Chinese Universities
基金
河北省社科基金(HB17JY070)。
关键词
碳酸二苯酯
氧化羰基化
金属有机框架材料
负载催化剂
diphenyl carbonate
oxidative carbonylation
metal-organic frameworks
supported catalyst
