节点文献
Pd/HKUST-1催化苯酚氧化羰基化合成碳酸二苯酯
Oxidative carbonylation of phenol to diphenyl carbonate catalyzed by Pd/HKUST-1
【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。
【Abstract】 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.
【Key words】 diphenyl carbonate; oxidative carbonylation; metal-organic frameworks; supported catalyst;
- 【文献出处】 高校化学工程学报 ,Journal of Chemical Engineering of Chinese Universities , 编辑部邮箱 ,2023年04期
- 【分类号】TQ426;TQ245.24
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