锆基MOFs的合成和表征及催化制备生物柴油
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TQ 021.8

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海南省重点项目(ZDYF2018134)


Synthesis and Characterization of Zirconium-Based MOFs and Catalytic Preparation of Biodiesel
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Hainan Provincial Key Project (ZDYF2018134)

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    摘要:

    采用不同有机配体(对苯二甲酸,2-硝基对苯二甲酸、2-氨基对苯二甲酸、2-羟基对苯二甲酸),利用剂热合成法合成锆基MOFs结构UiO-66及其衍生物,添加不同的调节剂(甲酸、乙酸、苯甲酸和盐酸)调节锆基MOFs结构。采用XRD、SEM和FT-IR等对锆基MOFs材料进行表征,研究不同的调节剂和添加量对锆基MOFs形貌特征和结构性质的影响。研究发现调节剂的不同对锆基MOFs结构形成产生不同影响,盐酸和乙酸混合调节剂能显著提高UiO-66的结晶度,当n(调节剂)∶n(ZrCl4)=30∶1时,苯甲酸调节剂可以获得尺寸为500 nm结构规整的UiO-66八面体晶体,甲酸调节剂将UiO-66的比表面积由1173.3 m2/g提高到1973.8 m2/g。选择3种锆基MOFs作为酯化反应催化剂,UiO-66-NH2催化活性较好,其游离脂肪酸转化率为50.7%,用KOH催化酯化油反应得到的生物柴油产率为51.6%,脂肪酸甲酯含量达99%以上。

    Abstract:

    UiO-66 and its derivatives were synthesized by solvothermal synthesis of different organic ligands, such as terephthalic acid, 2-nitroterephthalic acid, 2-aminoterephthalic acid and 2-hydroxyterephthalic acid. In the synthesis, formic acid, acetic acid, benzoic acid and hydrochloric acid were used as different modulators to modulate the structure of zirconium-based MOFs. The zirconium-based MOFs were characterized by XRD, SEM and FT-IR. The effects of different modulators and additions on the morphology and structure of zirconium-based MOFs were investigated. It was found that the different modulators have different effects on the formation of zirconium-based MOFs. The hydrochloric acid and acetic acid mixture modulators can significantly improve the crystallinity of UiO-66. When the molar ratio of the regulator to ZrCl4 was 30, the benzoic acid modulator can obtain uniform UiO-66 octahedral crystal with dimensions of 500 nm, the formic acid modulators increased the specific surface area of UiO-66 from 1173.3 m2/g to 1973.8 m2/g. Three kinds of zirconium-based MOFs were selected as esterification reaction catalysts to obtain esterified oil. UiO-66-NH2 has good catalytic activity, and its free fatty acid conversion rate was 50.7%. The yield of biodiesel obtained by the reaction of KOH catalyzed esterification oil was 51.6%, and the methyl ester rate was as high as 99% or more.

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杨子飞,曹阳,李进.锆基MOFs的合成和表征及催化制备生物柴油[J].精细化工,2020,37(2):0

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  • 收稿日期:2019-05-06
  • 最后修改日期:2019-07-06
  • 录用日期:2019-07-09
  • 在线发布日期: 2019-11-27
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