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开发可重复使用的 Ni/γ-AlO 催化剂,用于催化水解废 PET 瓶为对苯二甲酸。

Development of reusable Ni/γ-AlO catalyst for catalytic hydrolysis of waste PET bottles into terephthalic acid.

机构信息

Institute of Energy and Power Engineering, Zhejiang University of Technology, Hangzhou, 310014, China.

Zhejiang Carbon Neutral Innovation Institute, Zhejiang University of Technology, Hangzhou, 310014, China.

出版信息

Environ Sci Pollut Res Int. 2023 Oct;30(46):102560-102573. doi: 10.1007/s11356-023-29596-1. Epub 2023 Sep 5.

Abstract

In order to efficiently recycle waste polyethylene terephthalate (PET) bottles, this study aimed to enhance the hydrolysis process to convert PET bottle into valuable terephthalic acid (TPA) by developing effective and reusable Ni/γ-AlO catalysts. A series of Ni/γ-AlO catalyst was prepared by the impregnation method with different Ni loadings (5-15 wt%) and was characterized by various techniques including XRD, SEM-EDX, and N adsorption-desorption. The prepared catalysts were employed in the catalytic hydrolysis of PET under varied influencing factors, namely reaction temperature (220-280 °C), reaction time (20-60 min), and Ni loading. The response surface methodology (RSM) was used to optimize the operating condition to produce the maximum TPA yield, and the optimal values were determined as follows: reaction temperature = 267.07 °C, reaction time = 48.54 min, and Ni loading = 12.90 wt%, giving the highest TPA yield of 97.06%. The R, F-value, and P-value of the analysis of variance (ANOVA) were 0.9982, 424.96, and <0.0001, respectively, indicating a good fit of the model. The results from XRD and FTIR measurement of the produced TPA indicated the high purity and comparable chemical structures to the TPA standard. In addition, the 12.9Ni/Al catalyst exhibited high catalytic activity in repeated cycles of hydrolysis process of PET and could be regenerated by calcination to restore its catalytic activity. This finding could be a promising alternative for an effective TPA recovery from waste plastic bottles.

摘要

为了高效回收废弃的聚对苯二甲酸乙二醇酯(PET)瓶,本研究旨在通过开发高效且可重复使用的 Ni/γ-Al2O3 催化剂来增强水解过程,将 PET 瓶转化为有价值的对苯二甲酸(TPA)。采用浸渍法制备了一系列不同 Ni 负载量(5-15wt%)的 Ni/γ-Al2O3 催化剂,并通过 XRD、SEM-EDX 和 N2 吸附-脱附等多种技术进行了表征。将制备的催化剂用于在不同影响因素下催化 PET 的水解,即反应温度(220-280°C)、反应时间(20-60min)和 Ni 负载量。采用响应面法(RSM)优化操作条件以获得最大的 TPA 产率,确定的最佳值如下:反应温度=267.07°C,反应时间=48.54min,Ni 负载量=12.90wt%,得到的 TPA 产率最高,为 97.06%。方差分析(ANOVA)的 R、F 值和 P 值分别为 0.9982、424.96 和<0.0001,表明模型拟合良好。对生成的 TPA 的 XRD 和 FTIR 测量结果表明,其具有高纯度和与 TPA 标准相当的化学结构。此外,12.9Ni/Al 催化剂在 PET 水解过程的重复循环中表现出高催化活性,并且可以通过煅烧再生以恢复其催化活性。这一发现为从废塑料瓶中有效回收 TPA 提供了一种有前途的替代方法。

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