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用于乙醇脱氢偶联制正丁醇的银负载层状双氧化物中的界面位点

Interfacial Sites in Ag Supported Layered Double Oxide for Dehydrogenation Coupling of Ethanol to n-Butanol.

作者信息

Zhang Jian, Shi Kai, Zhu Yanru, An Zhe, Wang Wanning, Ma Xiaodan, Shu Xin, Song Hongyan, Xiang Xu, He Jing

机构信息

State Key Laboratory of Chemical Resource Engineering & Beijing, Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Box 98, 15 Beisanhuan Donglu, Beijing, 100029, China.

出版信息

ChemistryOpen. 2021 Nov;10(11):1095-1103. doi: 10.1002/open.202000295. Epub 2021 Jan 26.

DOI:10.1002/open.202000295
PMID:33496388
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8562315/
Abstract

Upgrading of ethanol to n-butanol through dehydrogenation coupling has received increasing attention due to the wide application of n-butanol. But the enhancement of ethanol dehydrogenation and followed coupling to produce high selectivity to n-butanol is still highly desired. Our previous work has reported an acid-base-Ag synergistic catalysis, with Ag particles supported on Mg and Al-containing layered double oxides (Ag/MgAl-LDO). Here, Ag-LDO interfaces have been manipulated for dehydrogenation coupling of ethanol to n-butanol by tailoring the size of Ag particles and the interactions between Ag and LDO. It has been revealed that increasing the population of surface Ag sites at Ag-LDO interfaces promotes not only the dehydrogenation of ethanol to acetaldehyde but also the subsequent aldol condensation of generated acetaldehyde. A selectivity of up to 76 % to n-butanol with an ethanol conversion of 44 % has been achieved on Ag/LDO with abundant interfacial Ag sites, much superior to the state-of-the-art catalysts.

摘要

由于正丁醇的广泛应用，通过脱氢偶联将乙醇升级为正丁醇受到了越来越多的关注。但是，提高乙醇脱氢以及随后的偶联反应以对正丁醇产生高选择性仍然是人们非常渴望的。我们之前的工作报道了一种酸碱 - 银协同催化作用，其中银颗粒负载在含镁和铝的层状双氢氧化物（Ag/MgAl-LDO）上。在这里，通过调整银颗粒的尺寸以及银与LDO之间的相互作用，对Ag-LDO界面进行了调控，用于乙醇脱氢偶联生成正丁醇。研究表明，增加Ag-LDO界面处表面银位点的数量不仅促进了乙醇脱氢生成乙醛，还促进了生成的乙醛随后的羟醛缩合反应。在具有丰富界面银位点的Ag/LDO上，实现了对正丁醇76%的选择性和44%的乙醇转化率，远优于现有催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/39d87bd821e1/OPEN-10-1095-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/43e6797d6661/OPEN-10-1095-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/74fdf79c3b4c/OPEN-10-1095-g011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/ab837e55b2b4/OPEN-10-1095-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/876a1cdd6f74/OPEN-10-1095-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/6d1f9d010801/OPEN-10-1095-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/7c6e958168f0/OPEN-10-1095-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/267e969c4680/OPEN-10-1095-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/2b67088a2ba1/OPEN-10-1095-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/0681a1aaeb2b/OPEN-10-1095-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/39d87bd821e1/OPEN-10-1095-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/43e6797d6661/OPEN-10-1095-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/74fdf79c3b4c/OPEN-10-1095-g011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/ab837e55b2b4/OPEN-10-1095-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/876a1cdd6f74/OPEN-10-1095-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/6d1f9d010801/OPEN-10-1095-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/7c6e958168f0/OPEN-10-1095-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/267e969c4680/OPEN-10-1095-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/2b67088a2ba1/OPEN-10-1095-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/0681a1aaeb2b/OPEN-10-1095-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a19f/8562315/39d87bd821e1/OPEN-10-1095-g004.jpg

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