淡江大學機構典藏:Item 987654321/127396
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    題名: Conversion of hydrogen/carbon dioxide into formic acid and methanol over Cu/CuCr2O4 catalyst
    作者: Chao-Lung Chiang, Kuen-Song Lin, Hui-Wen Chuang, Chun-Ming Wu
    關鍵詞: Carbon dioxide, Hydrogenation, Formic acid, Copper-chromium catalyst, EXAFS XANES
    日期: 2017-09-14
    上傳時間: 2025-06-04 12:05:27 (UTC+8)
    出版者: Elsevier
    摘要: Cu/CuCr2O4 catalysts were prepared by impregnation method at various calcination temperatures (300, 400, and 500 °C) and then reduced in H2 stream. The aggregated particles and decreasing surface area/pore volumes of the deactivated catalysts during HCOOH and CH3OH formations were also observed. Particularly, the EXAFS data showed that first shells of Cu atoms transforms from Cu–O to Cu–Cu after catalytic reactions, their bond distances and coordination numbers are quite different, respectively. It revealed that metallic Cu atoms are one of the important active species over catalyst surface at different reaction temperatures having many unoccupied binding sites for HCOOH and CH3OH formations. Additionally, the optimal calcination temperature for Cu/CuCr2O4 catalysts was demonstrated at 400 °C that attributed to its strongest acidity and basicity. The catalytic reactions in the duration of HCOOH and CH3OH preparation were proposed that were composed of HCOOH formation, CH3OH formation, and CH3OH decomposition happening at CuCr2O4, Cu, and CuO active sites, respectively. The highest CO2 conversion (14.6%), HCOOH selectivity/yield (87.8/12.8%), and TON/TOF values (4.19/0.84) were obtained at 140 °C and 30 bar in 5 h, respectively. Optimal rate constant (2.57 × 10−2 min−1) and activation energy (16.24 kJ mol−1) of HCOOH formation were evaluated by pseudo first-order model and Arrhenius equation, respectively.
    關聯: International Journal of Hydrogen Energy 42(37),p. 23647-23663
    DOI: 10.1016/j.ijhydene.2017.04.226
    顯示於類別:[化學工程與材料工程學系暨研究所] 期刊論文

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