Aqueous-phase deoxygenation of glycerol to 1,3-propanediol over Pt/WO3/ZrO2 catalysts in a fixed-bed reactor

Aqueous-phase deoxygenation of glycerol to 1,3-propanediol over Pt/WO3/ZrO2 catalysts in a fixed-bed reactor
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DOI:
10.1039/c0gc00005a
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发表时间:
2010-08-01
期刊:
影响因子:
9.8
通讯作者:
Chen, Chang-Lin
Chen, Chang-Lin
中科院分区:
化学1区
文献类型:
--
作者:
Qin, Li-Zhen;Song, Min-Jie;Chen, Chang-Lin

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Pt/WO 3/ZrO 2低温催化甘油水相脱氧(110-140 ℃)下在2 - 5 MPa的氢气压力下在固定床连续流动反应器中进行,得到1,3-丙二醇(1,3-PDO)和正丙醇(n-PrOH)作为主要产物,表明仲羟基脱氧的选择性高于甘油的伯羟基。在700 ℃下的ZrO 2和30wt%Pt的负载以及10wt%的W含量。反应温度的影响。考察了氢气压力和初始水含量对甘油转化率和1,3-PDO产率的影响。在130 ℃、4 MPa、70.2%转化率条件下,1,3-PDO的收率可达32.0%(1,3-PDO/1,2-PDO = 17.7)。Pt/WO 3/ZrO 2催化剂上甘油氧化反应的机理是一个包含质子和氢离子转移步骤的离子途径
Deoxygenation of glycerol in aqueous medium catalyzed by Pt/WO3/ZrO2 at relatively low temperatures (110-140 degrees C) under hydrogen pressure range from 2 to 5 MPa in a fixed-bed continuous-flow reactor gives 1,3-propanediol (1,3-PDO) and n-propanol (n-PrOH) as the predominant products, indicating high selectivity for deoxygenation of the secondary hydroxyl group over the primary hydroxyl groups of the glycerol The optimum catalyst was prepared by calcination of WO3/ZrO2 at 700 degrees C and loading of 30 wt% Pt with W content of 10 wt%. The effect of reaction temperature. hydrogen pressure and initial water content were evaluated to find the optimum reaction conditions The glycerol conversion and the yield of 1,3-PDO greatly depended on these factors. At 130 degrees C, 4 MPa and 70.2% conversion, the yield of 1,3-PDO was up to 32 0% (1,3-PDO/1,2-PDO = 17 7). The proposed mechanism for glycerol doxygenation in aqueous medium over Pt/WO3/ZrO2 is an ionic pathway involving proton and hydride ion transfer steps