高效光热催化废旧聚酯塑料升级回收

doi:10.1016/S1872-2067(23)64435-3

催化学报 ›› 2023, Vol. 49: 113-122.DOI: 10.1016/S1872-2067(23)64435-3

高效光热催化废旧聚酯塑料升级回收

娄向西^a^,^b^,¹, 高璇^b^,¹, 刘钰^b, 褚名宇^b, 张丛洋^b, 邱盈华^b, 杨文秀^c^,^*(), 曹暮寒^b, 王贵领^a^,^*(), 张桥^b, 陈金星^b^,^*()

^a哈尔滨工程大学材料科学与化学工程学院, 超轻材料与表面技术教育部重点实验室, 黑龙江哈尔滨 150001
^b苏州大学功能纳米与软物质研究院, 江苏省碳基功能材料与器件重点实验室, 江苏苏州 215123
^c东南大学分析测试中心, 江苏南京 211189

收稿日期:2023-02-01 接受日期:2023-03-19 出版日期:2023-06-18 发布日期:2023-06-05
通讯作者: ^*电子信箱: 101012725@seu.edu.cn (杨文秀),wangguiling@hrbeu.edu.cn (王贵领),chenjinxing@suda.edu.cn (陈金星).
作者简介:第一联系人：
¹共同第一作者.
基金资助:
国家自然科学基金(51901147);江苏省碳基功能材料与器件重点实验室(ZZ2103);姑苏创新企业领军人才计划(ZXL2022492);苏州大学生创新创业训练计划(202210285038Z)

Highly efficient photothermal catalytic upcycling of polyethylene terephthalate via boosted localized heating

Xiangxi Lou^a^,^b^,¹, Xuan Gao^b^,¹, Yu Liu^b, Mingyu Chu^b, Congyang Zhang^b, Yinghua Qiu^b, Wenxiu Yang^c^,^*(), Muhan Cao^b, Guiling Wang^a^,^*(), Qiao Zhang^b, Jinxing Chen^b^,^*()

^aKey Laboratory of Superlight Materials and Surface Technology of Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, Heilongjiang, China
^bInstitute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, Jiangsu, China
^cAnalysis and Testing Center of Southeast University, Southeast University, Jiulonghu Lake Campus, Nanjing 211189, Jiangsu, China

Received:2023-02-01 Accepted:2023-03-19 Online:2023-06-18 Published:2023-06-05
Contact: ^*E-mail: 101012725@seu.edu.cn (W. Yang), wangguiling@hrbeu.edu.cn (G. Wang), chenjinxing@suda.edu.cn (J. Chen).
About author:First author contact:¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(51901147);Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices(ZZ2103);Gusu Innovation and Entrepreneurship Leading Talent Program(ZXL2022492);111 Project, and the Undergraduate Training Program for Innovation and Entrepreneurship, Soochow University(202210285038Z)

摘要/Abstract

摘要：

太阳能是一种绿色、清洁的能源. 将可再生太阳能转化为热能驱动聚酯醇解反应, 即发展光热催化聚酯醇解方法, 实现废弃塑料转化为高纯度、高附加值单体, 有望解决传统热催化体系效率低、能耗高的问题, 实现废弃塑料的高效增值回收利用. 一方面, 光热催化体系可满足传统热催化所需的反应温度, 同时光热催化过程中存在的局域热效应, 可进一步提升聚酯回收的催化活性, 保障聚酯的高效醇解. 另一方面, 利用太阳能驱动光热催化聚酯醇解反应, 不仅降低能耗, 减少CO₂排放, 还可以充分利用清洁能源, 实现太阳能到化学能的高效转化. 然而, 催化剂的光热转化效率低、局域热效应弱以及催化活性低是限制其发展的挑战问题.

本文采用模板法合成了ZIF-8纳米粒子, 在ZIF-8表面包覆一层SiO₂, 经高温处理后得到一体化光热催化剂. 内部碳材料在吸收太阳光后产生热能, 而外层SiO₂可以阻止内部热的辐射损失, 从而提高局域温度. 此外, SiO₂包覆层可以抑制c-ZIF-8在高温热解过程中的聚集, 使催化剂在催化反应过程中具有更好的分散性. 优化后的光热催化剂(c-ZIF-8@25SiO₂)在0.78 W cm^-2模拟太阳光照射30 min下的PET转化率为84.97%, 是热催化反应性能的3.4倍. 当反应时间延长至45 min时, PET转化率达到100%. 动力学分析表明, 光热催化PET醇解的活化能为59.35 kJ mol^-1, 低于大多文献报道值(通常> 70 kJ mol^-1), 更重要的是, 其活化能也与热催化PET醇解的活化能(61.04 kJ mol^-1)相近反应. 上述结果表明, c-ZIF-8@25SiO₂纳米颗粒光热催化PET醇解和热催化PET醇解的反应路径可能是相同的, 因此排除了光化学活化在光热催化中的贡献. 此外, 这种SiO₂包覆层也使内部催化剂具有较高的稳定性, 其中PET转化率和对苯二甲酸乙二醇酯产率在5次循环后分别保持在初始值的98%和95%. 在室外太阳光照射下进行PET醇解实验以及从混合塑料中选择性回收PET, 进一步证明了c-ZIF-8@25SiO₂在光热催化PET醇解方面具有较好的用前景. 技术经济分析表明, 每回收1万吨PET, 选择光热催化可节电6390000 kW·h, 减少3089.59吨CO₂排放. 综上, 本文策略为增强光热催化中的局部加热效应提供了一种普适性方法, 为构筑高效塑料回收提供理论指导及实验参考.

关键词: 光热催化, 局域热效应, 聚酯升级回收, 聚酯醇解, 金属有机框架

Abstract:

Photothermal catalysis driven by clean solar energy efficiently converts plastic waste into high-value-added products. The catalytic process involves the transformation of solar energy to chemical energy. However, designing photothermal catalysts with a high conversion efficiency and catalytic activity remains considerably challenging. In this study, a c-ZIF-8@SiO₂ nanostructure is fabricated. It acts both as the photothermal reagent and the catalyst, displaying high photothermal conversion efficiency, catalytic activity, and stability in polyethylene terephthalate (PET) glycolysis. SiO₂-coated c-ZIF-8 effectively reduces the thermal radiation loss of the carbon material, thus enhancing the local thermal effect of the catalytic system. Consequently, the conversion efficiency of PET achieved using photothermal catalysis is 3.4 times higher than that of thermal catalysis under the same conditions. An economic efficiency analysis proves that photothermal catalysis can save 6390000 kW·h of electricity and reduce up to 3089.59 tons of CO₂ emissions for every 10000 tons of PET recycled. Therefore, the development of clean energy-driven photothermal catalysis technology could be a potential solution for the upcycling of waste plastics.

Key words: Photothermal catalysis, Localized heating effect, Polyester upcycling, Polyester glycolysis, Metal-organic framework

娄向西, 高璇, 刘钰, 褚名宇, 张丛洋, 邱盈华, 杨文秀, 曹暮寒, 王贵领, 张桥, 陈金星. 高效光热催化废旧聚酯塑料升级回收[J]. 催化学报, 2023, 49: 113-122.

Xiangxi Lou, Xuan Gao, Yu Liu, Mingyu Chu, Congyang Zhang, Yinghua Qiu, Wenxiu Yang, Muhan Cao, Guiling Wang, Qiao Zhang, Jinxing Chen. Highly efficient photothermal catalytic upcycling of polyethylene terephthalate via boosted localized heating[J]. Chinese Journal of Catalysis, 2023, 49: 113-122.

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Fig. 1. Structural characterization. TEM images of ZIF-8 (a), ZIF-8@mSiO2 (b), and c-ZIF-8@25SiO2 (c). HADDF image and EDX spectroscopy mappings of ZIF-8@25SiO2 (d) and c-ZIF-8@25SiO2 (Scale bar: 100 nm) (e). Temperature program (f) and corresponding TEM images (g) after in situ pyrolysis of ZIF-8@25SiO2.

Fig. 2. Photothermal performance of c-ZIF-8@SiO2. (a) Photothermal conversion curves of c-ZIF-8 and c-ZIF-8@25SiO2. (b) Theoretical spectra of the black-body radiation at different temperatures. (c) FTIR spectrum of porous silica shell obtained by removing Zn from c-ZIF-8@SiO2. (d) Schematic representation of the nanoscale insulation effect in c-ZIF-8@SiO2.

Fig. 3. Catalytic performance evaluation. (a) Thermal and photothermal catalysis conversion rate for the PET glycolysis. (b) Arrhenius plot of PET glycolysis for c-ZIF-8@25SiO2 for thermal and photothermal catalysis. (c) 1H NMR spectrum of generated BHET. (d) 13C NMR spectrum of generated BHET.

Fig. 4. Optimization of catalytic performance. (a) Effect of time on the PET conversion and BHET yield over c-ZIF-8@25SiO2. (b) Catalytic performance of recycled c-ZIF-8@25SiO2. (c) Integrated functionalities of c-ZIF-8@SiO2 and the photothermal catalytic mechanism of PET glycolysis over c-ZIF-8@SiO2.

Fig. 5. Practical demonstrations of photothermal catalysis. (a) Portable outdoor test. (b) Real-time reaction parameters of the outdoor experiment, including solar power (top row) and the surrounding (middle row) and system temperature (bottom row). (c) Image of the produced BHET; (d) Selective recycling of PET from PET-PE blends (Conditions: Solar power 0.78 W cm-2, 0.5 g of PE-PET blend, 2.5 g of EG, Cat/mixed plastics = 2%, 2 h). (e) Selective recycling of PET from colored PET waste (Conditions: Solar power 0.78 W cm-2, 0.5 g of color PET, 2.5 g of EG, Cat/mixed plastics = 2%, 1 h).

Fig. 6. Energy and environment impact analysis. (a) Simplified process flow diagram of the PET glycolysis for a typical photothermal/thermal catalysis. (b) Simplified estimation of energy consumption in different equipment for recycling 10000 tons of PET. (c) Impact of photothermal catalysis on reducing gaseous pollutant emission compared to that of thermal catalysis.

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高效光热催化废旧聚酯塑料升级回收

Highly efficient photothermal catalytic upcycling of polyethylene terephthalate via boosted localized heating

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