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Oxidative carbonylation of phenol to diphenyl carbonate catalyzed by palladium complexes bridged with N,N-ligands over functionalized silica

机译:在功能化二氧化硅上由N,N-配体桥接的钯配合物催化苯酚氧化羰基化为碳酸二苯酯

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摘要

Heterogeneous palladium catalysts anchored on functionalized silica were prepared by sol-gel methods and their catalytic properties for the oxidative carbonylation of phenol to diphenyl carbonate (DPC) were investigated.The catalysts were characterized by means of IR,XPS,EA and BET.The Pd loading in the heterogeneous catalysts and leaching in solution were detected by atomic absorption.The effects of different reaction parameters such as temperature,solvent and inorganic cocatalyst on the yield of DPC and Pd leaching were also studied.It was found that Cu_2O and tetrahydrofuran (THF) were the best partners with these heterogeneous catalysts.In the presence of 3 A molecular sieves as dehydrating agent,the heterogeneous palladium catalyst prepared from 2-acylpyridine revealed excellent catalytic performance and stability at 110 deg C for 5 h,giving 13.7% yield of DPC based on phenol and 4.0% Pd loss in solution.The heterogeneous catalyst was more active and stable compared with traditional supported Pd-C catalyst under the same reaction conditions.
机译:通过溶胶-凝胶法制备了固定在官能化二氧化硅上的多相钯催化剂,研究了其催化酚氧化羰基化为碳酸二苯酯(DPC)的催化性能,并通过IR,XPS,EA和BET对其进行了表征。通过原子吸收检测多相催化剂的负载量和溶液中的浸出。研究了温度,溶剂和无机助催化剂等不同反应参数对DPC和Pd浸出率的影响。发现Cu_2O和四氢呋喃(THF) )是这些多相催化剂的最佳伙伴。在3 A分子筛作为脱水剂的存在下,由2-酰基吡啶制得的多相钯催化剂表现出优异的催化性能和在110℃下5 h的稳定性,得到13.7%的收率。 DPC是基于苯酚和溶液中Pd损失为4.0%的催化剂。与传统催化剂相比,非均相催化剂活性更高且稳定在相同反应条件下负载Pd-C催化剂。

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