Regulation of Cu Species in CuO/SiO<sub>2</sub> and Its Structural Evolution in Ethynylation Reaction

A Cu-based nano-catalyst has been widely used in the ethynylation of formaldehyde; however, the effects of the presence of Cu on the reaction have not yet been reported. CuO/SiO<sub>2</sub> catalysts with different Cu species were prepared by impregnation (IM), deposition&#8722;preci...

Full description

Bibliographic Details
Main Authors: Haitao Li, Lijun Ban, Zhipeng Wang, Pingfan Meng, Yin Zhang, Ruifang Wu, Yongxiang Zhao
Format: Article
Language:English
Published: MDPI AG 2019-06-01
Series:Nanomaterials
Subjects:
Online Access:https://www.mdpi.com/2079-4991/9/6/842
_version_ 1818178512530440192
author Haitao Li
Lijun Ban
Zhipeng Wang
Pingfan Meng
Yin Zhang
Ruifang Wu
Yongxiang Zhao
author_facet Haitao Li
Lijun Ban
Zhipeng Wang
Pingfan Meng
Yin Zhang
Ruifang Wu
Yongxiang Zhao
author_sort Haitao Li
collection DOAJ
description A Cu-based nano-catalyst has been widely used in the ethynylation of formaldehyde; however, the effects of the presence of Cu on the reaction have not yet been reported. CuO/SiO<sub>2</sub> catalysts with different Cu species were prepared by impregnation (IM), deposition&#8722;precipitation (DP), and ammonia evaporation (AE). The structural evolution of the Cu species in different states of the ethynylation reaction and the structure&#8722;activity relationship between the existence state of the Cu species and the catalytic properties of the ethynylation reaction were studied. The results show that the Cu species in the CuO/SiO<sub>2</sub> (IM), prepared using the impregnation method, are in the form of bulk CuO, with large particles and no interactions with the support. The bulk CuO species are transformed into Cu<sup>+</sup> with a low exposure surface at the beginning of the reaction, which is easily lost. Thus, this approach shows the lowest initial activity and poor cycle stability. A high dispersion of CuO and copper phyllosilicate exists in CuO/SiO<sub>2</sub> (DP). The former makes the catalyst have the best initial activity, while the latter slows release, maintaining the stability of the catalyst. There is mainly copper phyllosilicate in CuO/SiO<sub>2</sub> (AE), which is slowly transformed into a highly dispersed and stable Cu<sup>+</sup> center in the in situ reaction. Although the initial activity of the catalyst is not optimal, it has the optimal service stability.
first_indexed 2024-12-11T20:49:10Z
format Article
id doaj.art-8a7e26ab39b14c03929845fb21a18ddb
institution Directory Open Access Journal
issn 2079-4991
language English
last_indexed 2024-12-11T20:49:10Z
publishDate 2019-06-01
publisher MDPI AG
record_format Article
series Nanomaterials
spelling doaj.art-8a7e26ab39b14c03929845fb21a18ddb2022-12-22T00:51:17ZengMDPI AGNanomaterials2079-49912019-06-019684210.3390/nano9060842nano9060842Regulation of Cu Species in CuO/SiO<sub>2</sub> and Its Structural Evolution in Ethynylation ReactionHaitao Li0Lijun Ban1Zhipeng Wang2Pingfan Meng3Yin Zhang4Ruifang Wu5Yongxiang Zhao6Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaEngineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, ChinaA Cu-based nano-catalyst has been widely used in the ethynylation of formaldehyde; however, the effects of the presence of Cu on the reaction have not yet been reported. CuO/SiO<sub>2</sub> catalysts with different Cu species were prepared by impregnation (IM), deposition&#8722;precipitation (DP), and ammonia evaporation (AE). The structural evolution of the Cu species in different states of the ethynylation reaction and the structure&#8722;activity relationship between the existence state of the Cu species and the catalytic properties of the ethynylation reaction were studied. The results show that the Cu species in the CuO/SiO<sub>2</sub> (IM), prepared using the impregnation method, are in the form of bulk CuO, with large particles and no interactions with the support. The bulk CuO species are transformed into Cu<sup>+</sup> with a low exposure surface at the beginning of the reaction, which is easily lost. Thus, this approach shows the lowest initial activity and poor cycle stability. A high dispersion of CuO and copper phyllosilicate exists in CuO/SiO<sub>2</sub> (DP). The former makes the catalyst have the best initial activity, while the latter slows release, maintaining the stability of the catalyst. There is mainly copper phyllosilicate in CuO/SiO<sub>2</sub> (AE), which is slowly transformed into a highly dispersed and stable Cu<sup>+</sup> center in the in situ reaction. Although the initial activity of the catalyst is not optimal, it has the optimal service stability.https://www.mdpi.com/2079-4991/9/6/842copper phyllosilicatedifferent statesformaldehyde ethynylation1,4-butynediol
spellingShingle Haitao Li
Lijun Ban
Zhipeng Wang
Pingfan Meng
Yin Zhang
Ruifang Wu
Yongxiang Zhao
Regulation of Cu Species in CuO/SiO<sub>2</sub> and Its Structural Evolution in Ethynylation Reaction
Nanomaterials
copper phyllosilicate
different states
formaldehyde ethynylation
1,4-butynediol
title Regulation of Cu Species in CuO/SiO<sub>2</sub> and Its Structural Evolution in Ethynylation Reaction
title_full Regulation of Cu Species in CuO/SiO<sub>2</sub> and Its Structural Evolution in Ethynylation Reaction
title_fullStr Regulation of Cu Species in CuO/SiO<sub>2</sub> and Its Structural Evolution in Ethynylation Reaction
title_full_unstemmed Regulation of Cu Species in CuO/SiO<sub>2</sub> and Its Structural Evolution in Ethynylation Reaction
title_short Regulation of Cu Species in CuO/SiO<sub>2</sub> and Its Structural Evolution in Ethynylation Reaction
title_sort regulation of cu species in cuo sio sub 2 sub and its structural evolution in ethynylation reaction
topic copper phyllosilicate
different states
formaldehyde ethynylation
1,4-butynediol
url https://www.mdpi.com/2079-4991/9/6/842
work_keys_str_mv AT haitaoli regulationofcuspeciesincuosiosub2subanditsstructuralevolutioninethynylationreaction
AT lijunban regulationofcuspeciesincuosiosub2subanditsstructuralevolutioninethynylationreaction
AT zhipengwang regulationofcuspeciesincuosiosub2subanditsstructuralevolutioninethynylationreaction
AT pingfanmeng regulationofcuspeciesincuosiosub2subanditsstructuralevolutioninethynylationreaction
AT yinzhang regulationofcuspeciesincuosiosub2subanditsstructuralevolutioninethynylationreaction
AT ruifangwu regulationofcuspeciesincuosiosub2subanditsstructuralevolutioninethynylationreaction
AT yongxiangzhao regulationofcuspeciesincuosiosub2subanditsstructuralevolutioninethynylationreaction