Heterogeneous CaO-ZrO2 acid-base bifunctional catalysts for vapor-phase selective dehydration of 1,4-butanediol to 3-buten-1-ol
Heterogeneous CaO-ZrO2 acid-base bifunctional catalysts for vapor-phase selective dehydration of 1,4-butanediol to 3-buten-1-ol
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DOI：
10.1016/j.apcata.2013.06.020
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发表时间：
2013-09
影响因子：
5.5
通讯作者：
Qian Zhang;Yin Zhang;Haitao Li;Chunguang Gao;Yongxiang Zhao
中科院分区：
文献类型：
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作者：
Qian Zhang;Yin Zhang;Haitao Li;Chunguang Gao;Yongxiang Zhao
采用浸渍法制备了一系列酸碱双功能CaO-ZrO2催化剂，并将其用于1，4-丁二醇(BDO)的气相脱水反应。考察了CaO含量和焙烧温度对CaO-ZrO2催化剂催化性能的影响。结果表明，在焙烧温度为650℃、CaO含量为12.5wt%时，该催化剂对BDO选择性脱水合成3-丁烯-1-醇(BTO)具有良好的催化性能和稳定性。最大BTO选择性和BDO转化率分别达到68.9%和94.6%。副产物四氢呋喃的生成受到明显抑制。用氮气物理吸附、X射线衍射、红外光谱、NH3-TPD和CO2-TPD对催化剂进行了表征。结果表明，由于CaO的引入形成了Ca-O-Zr杂键，使CaO-ZrO2催化剂表现出较高的碱性密度和相近的酸性密度。催化剂的催化性能取决于催化剂表面酸性中心和碱性中心的共存。
A series of acid–base bifunctional CaO-ZrO2catalysts was prepared simply by the impregnation method and evaluated for the vapour-phase dehydration of 1,4-butanediol (BDO). The effects of CaO content and calcination temperature on the catalytic properties of the CaO-ZrO2catalysts were investigated. It was found that the catalyst with 12.5 wt% CaO and at a calcination temperature of 650 °C exhibited favorable catalytic performance and good stability for the selective dehydration of BDO to 3-buten-1-ol (BTO). The maximum BTO selectivity and BDO conversion reached 68.9% and 94.6%, respectively. The formation of by-product, THF, was markedly suppressed. These catalysts were characterized by N2physisorption, XRD, FT-IR spectra, NH3-TPD and CO2-TPD. The results indicated that the CaO-ZrO2catalysts showed higher basicity density and similar acidity density compared to unmodified ZrO2due to the formation of Ca–O–Zr Hetero-linkage by CaO introduction. The catalytic performance depended on the coexistence of acidic and basic sites on the surface of catalysts.