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Catalytic Dehydration of 1,4‐Butanediol over Mg−Yb Binary Oxides and the Mechanism Study
Author(s) -
Mi Rongli,
Hu Zhun,
Yi Chunhai,
Yang Bolun
Publication year - 2020
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.202000152
Subject(s) - catalysis , selectivity , chemistry , inorganic chemistry , diffuse reflectance infrared fourier transform , methacrolein , infrared spectroscopy , organic chemistry , polymerization , photocatalysis , polymer , methacrylic acid
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 N 2 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 Yb 2 O 3 or MgO. Structures of Mg−O−Yb were generated in the binary oxides via the interchange of Yb or Mg in the MgO or Yb 2 O 3 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.