Hydroamination of n-butanol on Cu-containing anion-modified catalysts

Q4 Chemistry
V.V. Bilov, V. Markov, V.V. Shipilo
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引用次数: 0

Abstract

The purpose of the work is to establish the relationship between the composition of new Cu-containing anion-modified compositions and their catalytic potential in the synthesis of dibutylamine, which is an important intermediate for the production of such significant products as medicines, insecticides, vulcanization accelerators for rubber compounds, multifunctional corrosion inhibitors, etc. Composite materials were prepared by thermal decomposition of a copper-ammonia-carbonate solution in the presence of chromate, molybdate, aluminum tungstate, aluminum metahydroxide, and lanthanum carbonate salts. The active state of the new catalysts was formed under the conditions of low-temperature heat treatment (2500C) and reduction (2400C), which ensure incomplete removal of modifying OH– and СО32– anions. The study of the catalytic efficiency of new samples in the process of vapor-phase hydroamination of n-butanol was carried out in a flow reactor at the n-butanol:ammonia:hydrogen molar ratio equal to 1.0:2.0:6.0, an alcohol load of 0.4 h–1 and temperatures of 200–2400C. Among the catalysts tested, the sample whose precursor was a mixed "compound" salt hydroxocarbonate copper-aluminum chromate showed the highest performance as follows: alcohol conversion and selectivity to the target dibutylamine of 86.3% and 82.7%, respectively (at 2200C). The least active was the sample, the precursor of which was a mixed "compound" salt hydroxocarbonate copper-lanthanum carbonate. Factors that can affect the catalytic efficiency of new materials were analyzed.
含cu阴离子改性催化剂上正丁醇的氨基化反应
二丁胺是生产医药、杀虫剂、橡胶硫化促进剂、多功能缓蚀剂等重要产品的重要中间体,研究了新型含铜阴离子改性组合物的组成与其合成二丁胺的催化潜力之间的关系。在铬酸盐、钼酸盐、钨酸铝、氢氧化铝和碳酸镧盐的存在下,对铜-氨-碳酸盐岩溶液进行热分解制备复合材料。新型催化剂在低温热处理(2500C)和还原(2400C)条件下形成活性态,保证了改性OH -和СО32 -阴离子的不完全去除。在正丁醇:氨:氢的摩尔比为1.0:2.0:6.0,酒精负荷为0.4 h-1,温度为200 - 2400℃的流动反应器中,对新样品在正丁醇气相加氢胺化过程中的催化效率进行了研究。在所测试的催化剂中,以混合“复合”氢氧碳酸盐铜铝铬酸盐为前驱体的样品表现出最高的性能:醇转化率和对目标二丁胺的选择性分别为86.3%和82.7% (2200C)。活性最低的是样品,其前体是一种混合的“化合物”盐氢氧碳酸盐铜-碳酸镧。分析了影响新材料催化效率的因素。
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来源期刊
Voprosy Khimii i Khimicheskoi Tekhnologii
Voprosy Khimii i Khimicheskoi Tekhnologii Chemical Engineering-Chemical Engineering (all)
CiteScore
0.90
自引率
0.00%
发文量
62
期刊介绍: Voprosy Khimii i Khimicheskoi Tekhnologii (Issues of Chemistry and Chemical Technology) is published bimonthly by the Ukrainian State University of Chemical Technology and accepts Ukrainian- or English language high-quality original articles and reviews concerning various fields of research in chemistry and chemical engineering. Our unusual title “Voprosy khimii i khimicheskoi tekhnologii” originates from the transliterated initial Russian title “Issues of Chemistry and Chemical Technology“. The fact of the matter is that Voprosy khimii i khimicheskoi tekhnologii was founded in 1965 as a scientific journal mainly for Russian-reading and Russian-speaking readership when «the Iron Curtain» existed. Since 1991, after Ukraine declared its independence, our Journal began to publish the articles in Ukrainian and English. Multilingualism is our established tradition. We remember and cherish our traditions, but we follow the latest trends in modern science. Papers that are multidisciplinary or address new or emerging areas of chemistry and chemical engineering are particularly encouraged. Thus, the scope is dynamic. It includes but is not limited to the traditional areas of general, inorganic, organic, analytical, physical chemistry and electrochemistry, as well as all conventional areas of chemical engineering (chemistry of high molecular compounds, technology of inorganic and organic substances, processing of combustible minerals, chemical technology of silicates, processes and apparatus of chemical productions, etc.). The Journal publishes papers dealing with newer interdisciplinary areas such as materials science, nano-science, catalysis, computational and theoretical chemistry, surface phenomenon and colloidal systems, environmental chemistry, green chemistry.
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