| 溶剂热浸渍法制备高稳定性Zn(OAc)2/SiO2催化剂及其催化合成苯氨基甲酸甲酯 |
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| 引用本文： | 彭向聪,王志苗,李红芹,薛伟,李芳,王延吉.溶剂热浸渍法制备高稳定性Zn(OAc)2/SiO2催化剂及其催化合成苯氨基甲酸甲酯[J].化工进展,2019,38(3):1396-1402. |
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| 作者姓名： | 彭向聪 王志苗 李红芹 薛伟 李芳 王延吉 |
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| 作者单位： | 河北工业大学化工学院, 绿色化工与高效节能河北省重点实验室, 天津 300130;河北工业大学化工学院, 绿色化工与高效节能河北省重点实验室, 天津 300130;河北工业大学化工学院, 绿色化工与高效节能河北省重点实验室, 天津 300130;河北工业大学化工学院, 绿色化工与高效节能河北省重点实验室, 天津 300130;河北工业大学化工学院, 绿色化工与高效节能河北省重点实验室, 天津 300130;河北工业大学化工学院, 绿色化工与高效节能河北省重点实验室, 天津 300130 |
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| 基金项目： | 国家自然科学基金(21236001，21776057);天津市自然科学基金(17JCYBJC20100) |
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| 摘 要： | Zn(OAc)2对由碳酸二甲酯（DMC）和苯胺合成苯氨基甲酸甲酯（MPC）的反应具有优异的催化性能，但存在易失活、不能重复使用的缺点。为此，以DMC为溶剂，利用溶剂热浸渍法制备Zn(OAc)2/SiO2催化剂，并对其催化性能进行了研究。利用XRD、FTIR和TG-DTA等方法对其进行了表征，结果表明，Zn(OAc)2/SiO2催化剂表面存在Zn(OAc)2和ZnO，且其在SiO2表面分散较好；优化了Zn(OAc)2/SiO2催化剂的反应条件，当反应温度为190℃、反应时间为5h、苯胺与DMC的摩尔比为1∶20、催化剂与苯胺质量比为0.2时，苯胺的转化率为97.2%，MPC的选择性为89.4%。和等体积浸渍法制备的催化剂相比，溶剂热浸渍法制备的Zn(OAc)2/SiO2催化剂具有较好的稳定性，重复使用7次，苯胺的转化率下降至79.1%，MPC的选择性下降至79.2%。Zn(OAc)2/SiO2活性下降的原因是由于ZnO的生成，并对其进行了再生，再生后的催化剂活性与新鲜催化剂接近。
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| 关 键 词： | 碳酸二甲酯 苯氨基甲酸甲酯 苯胺 Zn(OAc)2/SiO2 溶剂热浸渍 催化剂 稳定性 再生 |
| 收稿时间： | 2018-03-01 |
Preparation of Zn(OAc)2/SiO2 catalyst with better stability prepared by solvothermal impregnation method and its application in methyl N-phenyl carbamate |
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| Xiangcong PENG,Zhimiao WANG,Hongqin LI,Wei XUE,Fang LI,Yanji WANG.Preparation of Zn(OAc)2/SiO2 catalyst with better stability prepared by solvothermal impregnation method and its application in methyl N-phenyl carbamate[J].Chemical Industry and Engineering Progress,2019,38(3):1396-1402. |
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| Authors: | Xiangcong PENG Zhimiao WANG Hongqin LI Wei XUE Fang LI Yanji WANG |
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| Affiliation: | Hebei Provincial Key Lab of Green Chemical Technology & High Efficient Energy Saving, School of Chemical Engineering & Technology, Hebei University of Technology, Tianjin 300130，China |
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| Abstract: | Zn(OAc)2 exhibits excellent catalytic performance in the methyl N-phenyl carbamate (MPC) synthesis using aniline and dimethyl carbonate (DMC), but it cannot be reused. Zn(OAc)2/SiO2 catalyst was prepared by solvothermal impregnation with DMC as the solvent in this paper. Zn(OAc)2/SiO2 was characterized by XRD、FTIR and TG-DTA. The results suggested that Zn(OAc)2 and ZnO were well dispersed on SiO2 surface. At reaction temperature of 190℃, reaction time of 5h, n DMC∶n aniline of 20∶1 and m aniline:m of 0.2, Zn(OAc)2/SiO2 showed the best catalytic performance, giving an aniline conversion of 97.2% and a MPC selectivity of 89.4%. The obtained Zn(OAc)2/SiO2 showed better stability than that prepared by incipient impregnation. After the Zn(OAc)2/SiO2 was used for the seventh time, aniline conversion and MPC selectivity were found to be 79.1% and 79.2%, respectively and the catalytic activity decrease is attributed to the formation of ZnO. The deactivated Zn(OAc)2/SiO2 can be regenerated with the catalytic activity almost the same as that of the fresh catalyst. |
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| Keywords: | dimethyl carbonate methyl N-phenyl carbamate aniline zinc acetate/silica solvothermal impregnation catalyst stability regeneration |
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