有机锆聚合物气凝胶的制备及光催化还原CO2
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海南省重点研发计划项目 (ZDYF2020015); 国家自然科学基金 (51761010); 海南大学科研平台建设(ZY2019HN09)


Preparation of organozirconium polymer aerogels and photocatalysis reduction of CO2
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    摘要:

    以2-氨基对苯二甲酸 (NH2-BDC) 为配体、四氯化锆为Zr4+源,采用溶胶-凝胶法制备了4种不同配体/金属离子物质的量比的气凝胶,并通过SEM、BET、FTIR、XPS、UV-Vis、荧光光谱等表征了材料的结构及光电性能。结果表明,这种气凝胶不仅具有大的比表面积与丰富的孔道结构,而且在氙灯照射下具有光电效应,可以在水中催化还原CO2生成甲醇。在300 W 的氙灯照射下,研究了不同配体/金属离子比对光催化还原CO2的影响。结果表明,当气凝胶中n (NH2-BDC): n (Zr4+) 的实际比例为1.10: 1时,4 h 光催化反应后甲醇产率为3.94 mmol/g-cat,催化转换频率为2.41 h-1。相同催化反应条件下以NH2-UiO-66(Zr) 为光催化剂,甲醇的产率为2.33 mmol/g-cat,TOF为1.80 h-1。此外,该气凝胶具有较好的光催化稳定性。

    Abstract:

    Four aerogels with different molar ratios of ligand to metal ion were prepared by sol-gel method using 2-aminoterephthalic acid (NH2-BDC) as ligand and zirconium tetrachloride as Zr4+ source. The structure and photoelectric properties of the materials were characterized by SEM, BET, FTIR, XPS, UV-Vis and fluorescence spectroscopy. The results showed that the aerogels had a large specific surface area and rich pores and exhibited photoelectric effect under Xenon lamp irradiation. They could photocatalyze the reduction of CO2 to produce methanol in water. The effects of different molar ratios of ligand to metal ion on the photocatalytic reduction of CO2 were investigated under 300 W Xenon lamp irradiation. When the photocatalytic reduction of CO2 was performed for 4 h over the aerogel which actual ratio n (NH2-BDC): n (Zr4+) is 1.10∶1, the methanol yield was 3.94 mmol/g-cat and the corresponding turnover frequency (TOF) was 2.41 h-1. While the methanol yield and TOF over NH2-UiO-66(Zr) was 2.33 mmol/g-cat and 1.80 h-1 under the same reaction conditions. In addition, the aerogel had good photocatalytic stability.

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刘青青,张芩宇,贺建雄,姜宏,熊春荣.有机锆聚合物气凝胶的制备及光催化还原CO2[J].精细化工,2021,38(4):

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  • 收稿日期:2020-12-22
  • 最后修改日期:2021-02-23
  • 录用日期:2021-02-24
  • 在线发布日期: 2021-04-06
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