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SBA-15负载型铜催化剂上草酸二乙酯选择性加氢制乙醇的研究

发表时间:2015-02-15  浏览量:1351  下载量:625
全部作者: 龙培,郑鑫磊,郑建伟,陈金,段新平,袁友珠
作者单位: 厦门大学化学化工学院,固体表面物理化学国家重点实验室,醇醚酯化工清洁生产国家 工程实验室
摘 要: 采用蒸氨法制备了以介孔分子筛SBA-15和硅胶等为载体的负载型催化剂(25Cu/SBA-15和25Cu/SiO2-sol等),并考察它们对草酸二乙酯(DEO)制乙醇的催化性能。结果表明:25Cu/SBA-15与25Cu/SiO2-sol的催化性能相似,但前者有更好的耐热性;在533 K,氢气压力3.0 MPa和DEO液时空速(weight liquid hourly space velocity, WLHSV)2.0 h"1的最优反应条件下,DEO转化率接近100%,乙醇选择性87.3%. 表征结果显示:在催化剂制备过程中,铜离子与载体表面氧化硅物种的相互作用形成了页硅酸铜物种,这有利于还原态催化剂中铜纳米粒子的高分散与稳定化,而SBA-15载体的高比表面积和孔道限域效应等特性使这些作用得到了强化,进而表现出更为优异的催化性能。
关 键 词: 物理化学;25Cu/SBA-15;草酸二乙酯;乙醇;加氢
Title: Study on selective hydrogenation of diethyl oxalate to ethanol over SBA-15-supported Cu catalysts
Author: LONG Pei, ZHENG Xinlei, ZHENG Jianwei, CHEN Jin, DUAN Xinping, YUAN Youzhu
Organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University
Abstract: 25Cu/SBA-15 and 25Cu/SiO2-sol catalysts were prepared by an ammonia-evaporation method for the selective hydrogenation of diethyl oxalate (DEO) to ethanol. The results indicated that 25Cu/SBA-15 and 25Cu/SiO2-sol showed similar catalytic performance initially, but Cu/SBA-15 displayed a better thermal-resistant ability. Nearly 100% conversion of DEO and 87.3% selectivity to ethanol could be obtained under the optimized conditions [553 K, 3.0 MPa and 2.0 h�1 weight liquid hourly space velocity (WLHSV)]. Characterization studies revealed that dispersion and stability of copper nanoparticles were benefited from the formation of copper phyllosilicate species on the surfaces. The high surface area and the pore confinement of SBA-15 support have important contributions to the performance enhancement.
Key words: physical chemistry; 25Cu/SBA-15; diethyl oxalate; ethanol; hydrogenation
发表期数: 2015年2月第3期
引用格式: 龙培,郑鑫磊,郑建伟,等. SBA-15负载型铜催化剂上草酸二乙酯选择性加氢制乙醇的研究 [J]. 中国科技论文在线精品论文,2015,8(3):251-257.
 
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