Synthesis and characterization of H3PW12O40/Ce0.1Ti0.9O2 for dimethyl carbonate formation via Methanol carbonation

doi:10.1016/j.ijhydene.2017.03.120

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Title:	Synthesis and characterization of H3PW12O40/Ce0.1Ti0.9O2 for dimethyl carbonate formation via Methanol carbonation
Authors:	Chiang, Chao-Lung;Lin, Kuen-Song;Yu, Ssu-Han;Lin, Yan-Gu
Keywords:	Carbon dioxide, Methanol carbonation, Dimethyl carbonate, H3PW12O40/Ce0.1Ti0.9O2 catalyst, XANES/EXAFS
Date:	2017/04/08
Issue Date:	2025-06-04 12:05:21 (UTC+8)
Publisher:	Elsevier
Abstract:	Ce0.1Ti0.9O2 and H3PW12O40/Ce0.1Ti0.9O2 catalysts were synthesized with a sol–gel method to form dimethyl carbonate (DMC) at reaction temperatures T = 110, 170, and 220 °C and volumetric flow-rate ratios CO2/N2 = 1/4, 1/7, and 1/9. The zeolite-like properties of H3PW12O40/Ce0.1Ti0.9O2 with an organized Keggin heteropolyacid structure were demonstrated from X-ray diffraction patterns and Fourier transform infrared spectra. 31P nuclear magnetic resonance spectra indicated that the Keggin heteropolyacid structure was formed through the addition of heteropoly acid (H3PW12O40). The bond lengths between titanium (Ti(IV)) and its adjacent atoms in the first shell (Tisingle bondO) of Ce0.1Ti0.9O2 and H3PW12O40/Ce0.1Ti0.9O2 were 1.90 and 1.86 Å, respectively, confirmed with EXAFS spectra. At 170 °C and CO2/N2 = 1/7, the optimal methanol conversion (5.5%), DMC selectivity (91.4%), and DMC yield (5.0%) of H3PW12O40/Ce0.1Ti0.9O2 were greater than those of Ce0.1Ti0.9O2. Linear regressions of the pseudo-first-order model indicated that the largest rate constant (4.16 × 10−3 min−1), turnover number (TON = 29.07), and turnover frequency (TOF = 4.85 × 10−2 min−1) of DMC formation were obtained with H3PW12O40/Ce0.1Ti0.9O2 at 170 °C and CO2/N2 = 1/7. A reaction mechanism induced by oxygen vacancies over the surfaces of Ce0.1Ti0.9O2 and H3PW12O40/Ce0.1Ti0.9O2 is proposed to describe the formation of DMC.
Relation:	International Journal of Hydrogen Energy, 42( 34),p. 22108-22122
DOI:	10.1016/j.ijhydene.2017.03.120
Appears in Collections:	[Graduate Institute & Department of Chemical and Materials Engineering] Journal Article

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