Synthesis and characterization of H3PW12O40/Ce0.1Ti0.9O2 for dimethyl carbonate formation via Methanol carbonation
學年 106
學期 1
出版（發表）日期 2017-08-24
作品名稱 Synthesis and characterization of H3PW12O40/Ce0.1Ti0.9O2 for dimethyl carbonate formation via Methanol carbonation
作品名稱（其他語言）
著者 Chao-Lung Chiang; Kuen-Song Lin; Ssu-Han Yu; Yan-Gu Lin
單位
出版者
著錄名稱、卷期、頁數 International Journal of Hydrogen Energy, 42( 34),p. 22108-22122
摘要 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.
關鍵字 Carbon dioxide, Methanol carbonation, Dimethyl carbonate, H3PW12O40/Ce0.1Ti0.9O2 catalyst, XANES/EXAFS
語言 en_US
ISSN
期刊性質 國內
收錄於 SCI Scopus
產學合作
通訊作者
審稿制度 是
國別 NLD
公開徵稿
出版型式 ,電子版
SDGS 氣候行動,可負擔的潔淨能源,產業創新與基礎設施