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

被引：25

作者：

Chiang, Chao-Lung ^{[1
]}

Lin, Kuen-Song ^{[1
]}

Yu, Ssu-Han ^{[1
]}

Lin, Yan-Gu ^{[2
]}

机构：

[1] Yuan Ze Univ, Environm Technol Res Ctr, Dept Chem Engn & Mat Sci, Taoyuan 32003, Taiwan

[2] Natl Synchrotron Radiat Res Ctr, Sci Res Div, Mat Sci Grp, Hsinchu Sci Pk, Hsinchu 30076, Taiwan

来源：

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY | 2017年 / 42卷 / 34期

关键词：

Carbon dioxide; Methanol carbonation; Dimethyl carbonate; H3PW12O40/Ce0.1Ti0.9O2; catalyst; XANES/EXAFS; HETEROGENEOUS CATALYSTS; OXIDE CATALYSTS; DIOXIDE; CO2; ACIDITY; NANOPARTICLES; CONVERSION; CHEMICALS; H3PW12O40; BASICITY;

D O I：

10.1016/j.ijhydene.2017.03.120

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Ce(0.1)Ti(0.9)O(2)and H3PW12O40/Ce0.2Ti0.9O2 catalysts were synthesized with a sol-gel method to form dimethyl carbonate (DMC) at reaction temperatures T = 110, 170, and 220 degrees C and volumetric flow-rate ratios CO2/N-2 = 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. P-31 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 (Ti -O) of Ce0.1Ti0.9O2 and H3PW12O40/Ce0.1Ti0.9O2 were 1.90 and 1.86 (A) over circleA, respectively, confirmed with EXAFS spectra. At 170 degrees C and CO2/N-2 = 1/7, the optimal methanol conversion (5.5%), DMC selectivity (91.4%), and DMC yield (5.0%) of H3PW12O40/Ce0.2Ti0.9O2 were greater than those of Ce0.1Ti0.9O2. Linear regressions of the pseudo -first -order model indicated that the largest rate constant (4.16 x 10(-3) min (-1)), turnover number (TON = 29.07), and turnover frequency (TOF = 4.85 x 10(-2) min (-1)) of DMC formation were obtained with H3PW12O40/Ce0.1Ti0.9O2 at 170 C and CO2/N-2 = 1/7. A reaction mechanism induced by oxygen vacancies over the surfaces of Ce0.2Ti0.9O2 and H3PW12O40/Ce0.1Ti0.9O2 is proposed to describe the formation of DMC. (C)2017 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

引用

页码：22108 / 22122

页数：15

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