Catalysis Science & Technology
·
2025
·
IF 4.2
Chengyang Sun,Yong Guo,Xiaohui Liu,Yanqin Wang
The upcycling of C–C bond linked polyolefins has drawn wide attention in recent years and a lot of studies have been focused on the conversion of polyolefins to hydrocarbons, while the further valorization to more value-added products has barely been developed. In this work, we developed an efficient strategy to upgrade polystyrene (PS) plastics into a single N-containing product, benzonitrile, over a NiO/CeO2 catalyst via a one-pot, two-step process. The first step is the oxidative-amination of PS to a mixture of benzamide and benzonitrile and the second step is the dehydration of benzamide to benzonitrile; finally, a single N-containing product, benzonitrile with a 50.3% yield, was achieved. Mechanism studies via control experiments in the first oxidative-amination step showed that benzaldehyde was the important intermediate, which can undergo two parallel pathways generating benzamide and benzonitrile, respectively. Following the dehydration of benzamide to benzonitrile in the second step, benzonitrile was produced as the only product. This strategy can also be extended to real-life PS plastics and a high yield of benzonitrile was achieved. This novel study provides an efficient approach for upgrading waste plastics to a single high-value product.
研究领域:
化学工程
·
环境科学
·
催化科学
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Jianye Gao,Jun Zhao,Zerong Xing,Minghui Guo,Haijiao Xie,Wangjing Ma,Jing Liu
Upcycling waste plastics is highly promising to tackle global white pollution while achieving sustainable development. However, prevailing approaches often encounter challenges in scalable engineering practices due to either insufficient plastic upcycling capability or arduousness in the separation, recovery, and purification of catalysts, which inevitably augments the cost of plastic upcycling. Here, the microwave-powered liquid metal synergetic depolymerization is presented to facilitate low-cost plastic upcycling. By leveraging the fluidity of liquid metals and their exceptional chemical-bond activation ability under microwave field, this method efficiently converts various polyolefins into narrowband hydrocarbon oil (Oil yield: 81 wt.% for polypropylene (PP), 85.9 wt.% for polyethylene (PE)) and high-value olefin monomers (C 2-4 selectivity: 50% for PE, 65.3% for PP) over 30 successive cycles, resulting in a high turnover frequency of 2.83 kg Plastic mL Liquid metal −1 . These captivating advantages offered by electromagnetically-powered liquid metals are also supported by their self-separation features, thereby paving the way for large-scale engineering solutions in waste plastic upcycling.
研究领域:
环境科学
·
材料科学
·
化学工程
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产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Songliang Liu,Kun Ma,Huaifang Teng,Weixin Miao,Xiaotong Zhou,Xuejing Cui,Xin Zhou,Luhua Jiang,Shaojun Guo
Innovating nanocatalysts with both high intrinsic catalytic activity and high selectivity is crucial for multi-electron reactions, however, their low mass/electron transport at industrial-level currents is often overlooked, which usually leads to low comprehensive performance at the device level. Herein, a Cl − /O 2 etching-assisted self-assembly strategy is reported for synthesizing a self-assembled gap-rich PdMn nanofibers with high mass/electron transport highway for greatly enhancing the electrocatalytic reforming of waste plastics at industrial-level currents. The self-assembled PdMn nanofiber shows excellent catalytic activity in upcycling waste plastics into glycolic acid, with a high current density of 223 mA cm −2 @0.75 V ( vs RHE), high selectivity (95.6%), and Faraday efficiency (94.3%) to glycolic acid in a flow electrolyzer. Density functional theory calculation, X-ray absorption spectroscopy combined with in situ electrochemical Fourier transform infrared spectroscopy reveals that the introduction of highly oxophilic Mn induces a downshift of the d -band center of Pd, which optimizes the adsorption energy of the reaction intermediates on PdMn surface, thereby facilitating the desorption of glycolic acid as a high-value product. Computational fluid dynamics simulations confirm that the gap-rich nanofiber structure is conducive for mass transfer to deliver an industrial-level current.
研究领域:
材料科学
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环境科学
·
催化化学
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产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2025
·
IF 5.1
Yanqin Zheng,Fuwang Wen,Hai Li,Fu Fangbao,Xihong Zu,Yanwei Wang,Almagul Mentbayeva,Wenli Zhang
The recycling of commercial plastics can decrease dependence on fossil fuels. The preparation of carbon electrode materials from commercial plastics can enable the upgrading of waste plastics. Converting low-recycled commercial plastics to value-added porous carbon materials showed great potential toward low-carbon development. However, the conversion of commercial plastics to porous carbon has low yields during pyrolysis and chemical activation. We employed the CuCl2 chemical activator and typical commercial plastics to prepare porous carbon, which achieved high yields exceeding 45%. The release of hydrocarbons during the pyrolysis of commercial plastics is inhibited by the dehydrogenation effect of the CuCl2 activator, while the carbon-rich structure is stabilized by the aromatization reactions of the decomposition species. The porous carbon materials prepared by CuCl2 activation have rich micropores and mesopores. These porous carbons exhibit excellent supercapacitor performance in aqueous electrolytes.
研究领域:
材料科学
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环境科学
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能源化学
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高分子化学
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电化学
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资源循环利用
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产品关联
DOI
PubMed
高影响因子
ChemSusChem
·
2022
·Vol. 16
·期 2
·e202201935
·
IF 9.14
Panpan He,Zhen Hu,Zhikun Dai,Huiying Bai,Zifen Fan,Ran Niu,Jiang Gong,Qiang Zhao,Tao Tang
Graphical MOF mill : A mechanochemical milling strategy effectively transforms waste poly(ethylene terephthalate) into a series of metal–organic frameworks (MOFs). The resultant MOFs show definite crystal structure with agglomerated nanoparticles. This strategy is green and sustainable, with the advantages of solvent-free conditions, ambient reaction temperature, short running time, and easy scale-up for large-scale production of MOFs. Converting poly(ethylene terephthalate) (PET) into metal–organic frameworks (MOFs) has emerged as a promising innovation for upcycling of waste plastics. However, previous solvothermal methods suffer from toxic solvent consumption, long reaction time, high pressure, and high temperature. Herein, a mechanochemical milling strategy was reported to transform waste PET into a series of MOFs with high yields. This strategy had the merits of solvent-free conditions, ambient reaction temperature, short running time, and easy scale-up for large-scale production of MOFs. The as-prepared MOFs exhibited definite crystal structure and porous morphology composed of agglomerated nanoparticles. It was proven that, under mechanochemical milling, PET was firstly decomposed into 1,4-benzenedicarboxylate, which acted as linkers to coordinate with metal ions for forming fragments, followed by the gradual arrangement of fragments into MOFs. This work not only promotes high value-added conversion of waste polyesters but also offers a new opportunity to produce MOFs in a green and scalable manner.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子