• 論文
主辦單位:煤炭科學研究總院有限公司、中國煤炭學會學術期刊工作委員會
Cu-Zr復合氧化物催化耦合甘油和CO2合成碳酸甘油酯
  • Title

    Synthesis of glycerol carbonate from glycerol and CO2 over Cu-Zr complex oxide

  • 作者

    徐換換柯義虎

  • Author

    XU Huanhuan;KE Yihu

  • 單位

    北方民族大學 國家民委化工技術基礎重點實驗室北方民族大學 寧夏太陽能化學轉化技術重點實驗室

  • Organization
    Key Laboratory of Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University, Yinchuan
    Ningxia Key Laboratory of Solar Chemical Conversion Technology, North Minzu University
  • 摘要
    采用水熱法合成了一系列不同Cu-Zr物質的量比的Cu1?xZrxO2雙金屬氧化物,以此為催化劑,將生物柴油生產過程副產物甘油與溫室氣體CO2耦合反應制備精細化工產品碳酸甘油酯。結果表明,Zr摻雜量不同,催化劑對甘油羰基化反應效果呈現明顯差距,最佳反應條件下,Cu0.99Zr0.01O2催化劑具有最佳催化性能,甘油轉化率和碳酸甘油酯選擇性分別達到64.1%和85.9%。并且發現與純CuO和純ZrO2相比,Cu1?xZrxO2復合氧化物在甘油與CO2耦合反應體系中表現出更強的催化活性,結合X射線粉末衍射(XRD)、掃描電子顯微鏡(SEM)、透射電子顯微鏡(TEM)、X射線光電子能譜(XPS)、N2吸附-脫附、程序升溫還原(H2-TPR)、程序升溫脫附(TPD)、傅里葉變換紅外光譜(FT-IR)等表征手段,推測高活性與Zr在CuO表面的分散程度、催化劑表面氧物種含量及酸堿性位點數量有關。此外,為了研究催化劑的穩定性,以Cu0.99Zr0.01O2催化劑作為基準進行了循環性能測試,結果表明,經過六次循環后,甘油的轉化率和碳酸甘油酯的選擇性未發生明顯變化,說明該催化劑穩定性良好。
  • Abstract
    A series of Cu1?xZrxO2 bimetallic oxides with different Cu-Zr molar ratios for glycerol carbonate synthesis from glycerol and CO2 were prepared by hydrothermal method. The results found that the performance was significantly affected by the Zr doping amounts. Under the optimal reaction conditions, the Cu0.99Zr0.01O2 catalyst had the best catalytic performance. The conversion of glycerol and the selectivity of glycerol carbonate reached 64.1% and 85.9%, respectively. Cu1?xZrxO2 complex oxide exhibited better activity than pure CuO and pure ZrO2. The structures, morphologies and surface properties of the catalysts were characterized by X-ray powder diffraction (XRD), Scanning electron microscopy (SEM), Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), N2 adsorption and desorption, Temperature programmed reduction (H2-TPR), Temperature programmed desorption (TPD) and Fourier Transform Infrared Spectroscopy (FT-IR). It is speculated that the high activity is related to the degree of dispersion of Zr on the surface of CuO, the surface content of oxygen species and the number of acidic-basic sites. In addition, catalytic activity did not change significantly after six cycles, indicating the excellent stability of the catalyst.
  • 關鍵詞

    甘油碳酸甘油酯二氧化碳復合氧化物2-氰基吡啶

  • KeyWords

    glycerol;glycerol carbonate;carbon dioxide;complex oxide;2-cyanopyridine

  • 基金項目(Foundation)
    國家自然科學基金 (21862001),寧夏餐廚廢油資源化利用技術研發創新團隊(2022QCXTD03)和寧夏低品質資源高值化利用技術研發人才小高地資助
  • DOI
  • 引用格式
    徐換換, 柯義虎. Cu-Zr復合氧化物催化耦合甘油和CO2合成碳酸甘油酯[J]. 燃料化學學報(中英文), 2024, 52(2): 171-183.
  • Citation
    XU Huanhuan, KE Yihu. Synthesis of glycerol carbonate from glycerol and CO2 over Cu-Zr complex oxide[J]. Journal of Fuel Chemistry and Technology, 2024, 52(2): 171-183.
  • 圖表
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