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−preci...
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MDPI AG
2019-06-01
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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−precipitation (DP), and ammonia evaporation (AE). The structural evolution of the Cu species in different states of the ethynylation reaction and the structure−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. |
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language | English |
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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−precipitation (DP), and ammonia evaporation (AE). The structural evolution of the Cu species in different states of the ethynylation reaction and the structure−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 |
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