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功能化氧化石墨烯催化CO2的化学固定

卢金凯 张梦 李斌 董丽辉 范闽光

卢金凯, 张梦, 李斌, 董丽辉, 范闽光. 功能化氧化石墨烯催化CO2的化学固定[J]. 华南师范大学学报(自然科学版), 2021, 53(3): 35-42. doi: 10.6054/j.jscnun.2021041
引用本文: 卢金凯, 张梦, 李斌, 董丽辉, 范闽光. 功能化氧化石墨烯催化CO2的化学固定[J]. 华南师范大学学报(自然科学版), 2021, 53(3): 35-42. doi: 10.6054/j.jscnun.2021041
LU Jinkai, ZHANG Meng, LI Bin, DONG Lihui, FAN Minguang. Chemical Fixation of CO2 Catalyzed by Functionalized Graphene Oxide[J]. Journal of South China normal University (Natural Science Edition), 2021, 53(3): 35-42. doi: 10.6054/j.jscnun.2021041
Citation: LU Jinkai, ZHANG Meng, LI Bin, DONG Lihui, FAN Minguang. Chemical Fixation of CO2 Catalyzed by Functionalized Graphene Oxide[J]. Journal of South China normal University (Natural Science Edition), 2021, 53(3): 35-42. doi: 10.6054/j.jscnun.2021041

功能化氧化石墨烯催化CO2的化学固定

doi: 10.6054/j.jscnun.2021041
基金项目: 

国家自然科学基金项目 21968002

广西石化资源加工及过程强化技术重点实验室项目 2019k006

详细信息
    通讯作者:

    范闽光,Email: fanmg@gxu.edu.cn

  • 中图分类号: O643.32

Chemical Fixation of CO2 Catalyzed by Functionalized Graphene Oxide

  • 摘要: 通过一锅法将氨基官能化的咪唑离子液体嫁接在氧化石墨烯(GO)和硅铝酸盐中孔分子筛(SBA-15)上,用来催化合成环状碳酸酯. 通过傅里叶变换红外光谱(FT-IR)、扫描电子显微镜(SEM)、热重分析(TGA)和元素分析(EA)对催化剂的结构、热稳定性以及氨基官能化咪唑离子液体的嫁接量进行了研究. 在环加成反应过程中,GO-NH2的活性高于SBA-15-NH2. 最佳条件: 催化剂用量0.15 g、反应温度130 ℃、CO2压力1.5 MPa和反应时间5 h,碳酸丙烯酯的产率达到96.46%. 此外,催化剂具有可回收性并可以连续5次重复使用.
  • 图  1  SBA-15-NH2和GO-NH2的合成路线

    Figure  1.  The route of SBA-15-NH2 and GO-NH2 synthesis

    图  2  环状碳酸酯的合成

    Figure  2.  The synthesis of cyclic carbonates

    图  3  不同材料的FT-IR光谱

    Figure  3.  The FT-IR spectra of different materials

    图  4  不同材料的SEM图

    Figure  4.  The SEM images of different materials

    图  5  GO和GO-NH2的TGA曲线

    Figure  5.  The TGA curves of GO and GO-NH2

    图  6  SBA-15和SBA-15-NH2的TGA曲线

    Figure  6.  The TGA curves of SBA-15 and SBA-15-NH2

    图  7  各种参数对GO-NH2催化条件下PC产率和选择性的影响

    Figure  7.  The effects of various parameters on the PC yield and selectivity with GO-NH2 as the catalyst

    图  9  GO-NH2催化剂的循环性能

    Figure  9.  The recycling performance of the GO-NH2 catalyst

    表  1  各种样品的元素分析结果

    Table  1.   The elemental analysis results of various samples

    编号 样品 w(C)/% w(N)/% 嫁接量/(mmol·g-1) 嫁接率/%
    1 GO 48.42
    2 GO-NH2 26.04 7.24 1.730 46.78
    3 GO-NH2(循环5次后) 28.63 7.23 1.720 46.77
    4 SBA-15
    5 SBA-15-NH2 12.05 8.29 1.975 53.42
    6 SBA-15-NH2(循环5次后) 12.01 8.27 1.974 53.41
    下载: 导出CSV

    表  2  各种催化剂对CO2环加成生成PC的性能

    Table  2.   The performance of various catalysts for the cycloaddition of CO2 to form PC

    实验序号 催化剂 PC产率/% PC选择性/%
    1 痕量
    2 N-methylimidazole < 3 100
    3 2-Bromoethylamine 19.06 98
    4 GO 15.05 98
    5 GO-NH2 96.46 99
    6 SBA-15 8.51 98
    7 SBA-15-NH2 90.47 99
    注:PO为34.5 mmol,催化剂质量为0.15 g,压力为1.5 MPa,温度为130 ℃,反应时间为5 h.
    下载: 导出CSV

    表  3  GO-NH2与各种同类催化剂的催化活性比较

    Table  3.   The performance of various catalysts for CO2 and PO cycloaddition reaction

    序号 催化剂 温度/℃ 压力/MPa 时间/h 产率/% 参考文献
    1 GO-HEIMBr 140 2 4 99 [24]
    2 EG/HEBIMBr 120 2 4 96 [21]
    3 GO/[BMIM]Br 80 1 6 99 [22]
    4 PS-HEIMBr 120 2.5 4 98 [23]
    5 GO-[SMIM]I 140 2 4 93 [24]
    6 GO-NH2 130 1.5 5 96.4 本文
    下载: 导出CSV
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出版历程
  • 收稿日期:  2021-03-15
  • 网络出版日期:  2021-07-06
  • 刊出日期:  2021-06-25

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