Catalytic Dehydration of 1,4‐Butanediol over Mg−Yb Binary Oxides and the Mechanism Study.

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Title: Catalytic Dehydration of 1,4‐Butanediol over Mg−Yb Binary Oxides and the Mechanism Study.
Authors: Mi, Rongli1 (AUTHOR), Hu, Zhun1 (AUTHOR), Yi, Chunhai1 (AUTHOR), Yang, Bolun1,2 (AUTHOR) blunyang@mail.xjtu.edu.cn
Source: ChemCatChem. 5/20/2020, Vol. 12 Issue 10, p2859-2871. 13p.
Subjects: Butanediol, Fourier transform infrared spectroscopy, Oxides, Dehydration
Abstract: In this study, Mg−Yb binary oxides were synthesized using different MgO concentrations and investigated for the catalytic dehydration of 1,4‐butanediol (BDO) into 3‐buten‐1‐ol (BTO). The physicochemical properties of the catalysts were characterized by N2 physisorption, X‐ray diffraction, Raman spectroscopy, temperature‐programmed techniques, and diffuse reflectance infrared Fourier transform spectroscopy. The Mg−Yb binary oxides exhibited superior catalytic activity and better BTO selectivity compared with the pristine Yb2O3 or MgO. Structures of Mg−O−Yb were generated in the binary oxides via the interchange of Yb or Mg in the MgO or Yb2O3 crystalline phases. Extra basic and acidic sites were formed over the Mg−Yb binary oxides because of the formation of surface defects and the presence of Mg−O−Yb structures, respectively. The acidic as well as basic sites were observed to influence the catalytic performance: BDO reactivity was enhanced by the more acidic sites, while BTO selectivity was favored by the basic sites. The highest BTO yield of 71.1 % was achieved over the Mg7Yb3 catalyst with 90.4 % BDO conversion and 78.6 % BTO selectivity at 350 °C. The in situ DRIFTS results indicated that BDO was first adsorbed on the catalyst and then reacted with the acidic sites to generate butoxides. The β‐H of the surface butoxides was abstracted by the basic oxygen anions to produce aldehyde species, which dissociated to form BTO. [ABSTRACT FROM AUTHOR]
Copyright of ChemCatChem is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Group: Ti
  Data: Catalytic Dehydration of 1,4‐Butanediol over Mg−Yb Binary Oxides and the Mechanism Study.
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  Data: <searchLink fieldCode="AR" term="%22Mi%2C+Rongli%22">Mi, Rongli</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Hu%2C+Zhun%22">Hu, Zhun</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Yi%2C+Chunhai%22">Yi, Chunhai</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Yang%2C+Bolun%22">Yang, Bolun</searchLink><relatesTo>1,2</relatesTo> (AUTHOR)<i> blunyang@mail.xjtu.edu.cn</i>
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  Data: <searchLink fieldCode="JN" term="%22ChemCatChem%22">ChemCatChem</searchLink>. 5/20/2020, Vol. 12 Issue 10, p2859-2871. 13p.
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  Data: <searchLink fieldCode="DE" term="%22Butanediol%22">Butanediol</searchLink><br /><searchLink fieldCode="DE" term="%22Fourier+transform+infrared+spectroscopy%22">Fourier transform infrared spectroscopy</searchLink><br /><searchLink fieldCode="DE" term="%22Oxides%22">Oxides</searchLink><br /><searchLink fieldCode="DE" term="%22Dehydration%22">Dehydration</searchLink>
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  Data: In this study, Mg−Yb binary oxides were synthesized using different MgO concentrations and investigated for the catalytic dehydration of 1,4‐butanediol (BDO) into 3‐buten‐1‐ol (BTO). The physicochemical properties of the catalysts were characterized by N2 physisorption, X‐ray diffraction, Raman spectroscopy, temperature‐programmed techniques, and diffuse reflectance infrared Fourier transform spectroscopy. The Mg−Yb binary oxides exhibited superior catalytic activity and better BTO selectivity compared with the pristine Yb2O3 or MgO. Structures of Mg−O−Yb were generated in the binary oxides via the interchange of Yb or Mg in the MgO or Yb2O3 crystalline phases. Extra basic and acidic sites were formed over the Mg−Yb binary oxides because of the formation of surface defects and the presence of Mg−O−Yb structures, respectively. The acidic as well as basic sites were observed to influence the catalytic performance: BDO reactivity was enhanced by the more acidic sites, while BTO selectivity was favored by the basic sites. The highest BTO yield of 71.1 % was achieved over the Mg7Yb3 catalyst with 90.4 % BDO conversion and 78.6 % BTO selectivity at 350 °C. The in situ DRIFTS results indicated that BDO was first adsorbed on the catalyst and then reacted with the acidic sites to generate butoxides. The β‐H of the surface butoxides was abstracted by the basic oxygen anions to produce aldehyde species, which dissociated to form BTO. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of ChemCatChem is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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RecordInfo BibRecord:
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      – Type: doi
        Value: 10.1002/cctc.202000152
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      – Code: eng
        Text: English
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        PageCount: 13
        StartPage: 2859
    Subjects:
      – SubjectFull: Butanediol
        Type: general
      – SubjectFull: Fourier transform infrared spectroscopy
        Type: general
      – SubjectFull: Oxides
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      – SubjectFull: Dehydration
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      – TitleFull: Catalytic Dehydration of 1,4‐Butanediol over Mg−Yb Binary Oxides and the Mechanism Study.
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            NameFull: Yang, Bolun
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            – D: 20
              M: 05
              Text: 5/20/2020
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              Y: 2020
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