Communications Biology
·
2023
·Vol. 6
·期 1
·1-13
·
IF 5.9
Guo Wenbin,Duan Jingjing,Shi Zhengguang,Yu Xue,Shao Zongze
Evidence for microbial biodegradation of polyethylene terephthalate (PET) has been reported, but little is known about the PET biodegradation process and molecular mechanism by marine microorganisms. Here, we show the biodegradation of PET by the membrane-anchored PET esterase from the marine bacterium Rhodococcus pyridinivorans P23, elucidate the properties of this enzyme, and propose the PET biodegradation by this strain in biofilm. We identify the PET-degrading enzyme dubbed PET esterase through activity tracking. In addition to depolymerizing PET, it hydrolyzes MHET into TPA under acid conditions. We prove that it is a low and constitutively transcribed, membrane-anchored protein displayed on the cell surface. Furthermore, we also investigate the microbial groups possessing PET esterase coupled with the TPA degradation pathway, mainly in the phyla Proteobacteria and Actinobacteriota . Clarification of the microbial PET biodegradation in the marine environment will contribute to the understanding of bioremediation of marine PET pollution.
研究领域:
环境微生物学
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生物技术
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海洋污染
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DOI
PubMed
高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 4.446
Zixuan Li,Kun Chen,Linling Yu,Qinghong Shi,Yan Sun
Cost-effective and eco-friendly treatment or recycled use of poly (ethylene terephthalate) (PET) is highly desired. Enzymatic PET degradation is considered a promising approach, but currently available PET hydrolases (PETases) have low activity at ambient temperature. Thus, elevating the reaction system temperature in a cost-effective way becomes a key to the economical enzymatic PET degradation. Herein, we proposed solar-driven enzymatic PET degradation with DuraPETase, a stable mutant of PETase, by using Fe 3 O 4 nanoparticles (NPs) as the solar-to-thermal agent. Simulated solar irradiation could elevate the suspension of Fe 3 O 4 NPs from 25 °C to 46 °C for the effective PET degradation. The enzyme immobilized onto Fe 3 O 4 NPs, [email protected] 3 O 4 , had higher stability than free DuraPETase, but a 10-d PET degradation experiments under simulated solar irradiation revealed that free DuraPETase in the presence of Fe 3 O 4 NPs was approximately three times more effective than the [email protected] 3 O 4 system because of the superiority of free DuraPETase in degrading PET. This implies that enzyme immobilization is unnecessary in such a single-use system. By contrast, the DuraPETase-only system showed only 15.5% efficiency of the Fe 3 O 4 -mediated solar-driven system with free DuraPETase. The research demonstrated the potential of the Fe 3 O 4 -mediated solar-driven enzymatic PET degradation strategy for further development in different practical scenarios
研究领域:
环境科学
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材料科学
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生物技术
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可持续化学
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产品关联
DOI
高影响因子
POLYMER COMPOSITES
·
2023
·
IF 5.2
Yao Peng,Yao Wang,Yingdi Dan,Zengkun Li,Quankai Sun,Yanxin Wang,Wei Wang,Zhonglin Du,Linjun Huang,Matt J. Kipper,Laurence A. Belfiore,Jianguo Tang
In this work, innovative hybrid poly(ethylene terephthalate) (PET) materials with strong luminescence were successfully synthesized by doping PET with silicon-linked poly(ethylene glycol)-PET copolymer nanostructures either with (Si-PEG-PET) or with (ETP@Si-PEG-PET) luminescent Eu 3+ -complexes. The chemical properties and nanostructures of the hybrid materials were characterized by Fourier-transform infrared spectroscopy, nuclear magnetic resonance spectroscopy, x-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy. PET composites ranging from 0.25 to 4 wt% silicon additive were prepared by the melt blending method. The crystal properties, mechanical properties, and fluorescence properties of the composites were systematically studied by differential scanning calorimetry, x-ray diffractometry, tensile testing, and fluorescence spectrometry. When the addition of Si-PEG-PET or ETP@Si-PEG-PET was 0.75 wt%, the relative crystallinity and maximum tensile strength increase substantially. Moreover, the fluorescence intensity of hybrid luminescent PET materials is the strongest at 0.75 wt% loading. ETP@Si-PEG-PET not only endows PET polyester with stronger fluorescence properties and mechanical properties but also acts as an effective nucleation additive for PET. Highlights Silicon-linked poly(ethylene glycol)-poly(ethylene terephthalate) (PEG-PET) nanostructures generate hybrid luminescent PET materials. ETP@Si-PEG-PET improves the crystallization rate and crystallinity of PET. The composite with 0.75% addition showed the best fluorescence performance. Three-dimensional-grid structure of ETP@Si-PEG-PET enhances the mechanical property of PET.
研究领域:
材料科学
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高分子化学
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纳米技术
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DOI
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Geliang Xie,Guoqiang Zhu,Yifan Kang,Mingxu Zhu,Qianqian Lu,Chao He,Lujiang Xu,Zhen Fang
Realizing the recovery and valorization of waste polyethylene terephthalate (PET) plastics into value-added products have gained significant importance. This study successfully synthesized aromatic nitriles , specifically terephthalonitrile (TPN), from waste polyethylene terephthalate (PET) plastic through in situ catalytic pyrolysis with urea and γ-Al 2 O 3 catalyst. Based on distributed activation energy model, positive interaction between waste PET and urea is responsible for improved thermal decomposition kinetics. The dosage of urea and pyrolysis temperature significantly influenced TPN production. TPN yield reached 32.5% with ca. selectivity of 85% at 550 °C and equivalent urea dosage. Density functional theory calculations validated the role of active ammonia in reducing energy barriers and thus facilitating PET depolymerization . The study highlights the feasibility of recycling waste PET into valuable aromatic nitriles through in situ catalytic pyrolysis with urea and enhances the understanding of the pyrolysis process.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xuhai Fu,Shixiang Fan,Jiaoxue Shi,Shichang Chen
A preparation strategy of chemically bonded fluorescent functionalized PET was proposed. An emitting red light of europium ternary complex with hydroxyl functional groups was prepared by precipitation method, and the PET with carboxyl groups was prepared by using UV grafting technology, then the rare earth complex could be grafted to the surface of PET materials by the reaction of acid and alcohol so that the functional design of bonded fluorescent materials was realized. The structure and morphology of the europium complex and functional PET materials were analyzed and the fluorescence performance of modified PET materials with different grafting contents were evaluated. It was found that the europium complex was successfully bonded onto the surface of PET material by using acrylic-acid reaction as medium. The functional PET emitted strong red fluorescence at 615 nm, and the fluorescence intensity reached a high value of 2.3×10 7 a.u. with the AA grafting rate of 9 %. Additionally, the fluorescent PET showed good temperature burst effect in the range of 40–80 °C and satisfactory response to pH solutions ranging from 2 to 12. This provides an attractive prospect for the design, preparation and application of fluorescent functional PET materials.
研究领域:
材料科学
·
化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Zhi Qu,Yan Sun
The enormous accumulation of poly(ethylene terephthalate) (PET) waste has posed a serious threat to the environment and human health, and biodegradation with PET hydrolase (PETase) can be a possible solution. Herein, we propose site-specifically modifying PETase with amphiphilic polymers to improve the enzyme performance at ambient temperature. For this purpose, we devise a computer-aided strategy to prioritize the conjugation site, and polyethylene glycol (PEG) preparations of 0.55 to 10 kDa are site-specifically conjugated to PETase. The most active conjugate PETase–PEG 5k (PETase-5K) shows an increase of melting temperature (3.88 °C) and significantly improves PET degradation performance (3.5- and 3.1-fold increases at 30 and 40 °C, respectively). Experimental investigation and molecular dynamics simulations reveal that the site-specific PEGylation increases the hydrophobic solvent-accessible surface area and the binding capability to the PET surface, thickens the hydration layer, increases the intramolecular hydrogen bonding, reduces the interactions between water and the conjugated enzyme surface, and rigidifies the enzyme structure via hydrogen bonding and hydrophobic interactions between the polymer and the enzyme, thus leading to improved enzymatic performance of PETase-5K. We further validate the versatility of the site-specific PEGylation in one of the most evolved variants of PETase, FAST-PETase, by 1.8-fold improvement in PET degradation at 30 °C. The presented computer-aided site-specific conjugation strategy has opened a new avenue to enhancing PETase performance at ambient temperature, and the contribution of PEGylation to PETase unraveled in this work laid a foundation for the rational engineering of PET hydrolases.
研究领域:
环境科学
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生物化学
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生物技术
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分子生物学
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材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Pengtao Fang,Xingmei Lu,Qing Zhou,Dongxia Yan,Jiayu Xin,Junli Xu,Chunyan Shi,Yongquan Zhou,Shuqian Xia
Controlled degradation of macromolecules or natural macromolecules is important for their subsequent utilization. Normally, it is easier to degrade them to monomers than to oligomers in designated molecular weight range, the controlled degradation is much difficult to achieve and has been challenge for the utilization of macromolecules. Here, we proposed a strategy for simultaneous degradation of the inner and outer layers of PET , which avoid the degradation of polymers from the outside to the inside and achieved the controlled degradation. Under high temperature and micro-pressure conditions, PET is transformed from dense to flocculent structure by the swelling effect, which satisfies the need for simultaneous degradation of the inner and outer layers. In addition, a stable “Dawson” type Polyoxometalates (POMs) α 2 -K 8 P 2 W 17 O 61 X(H 2 O)‧16H 2 O (X = Zn, Mn, Co, Ni, Cu) with limited number of catalytic activity center was synthesized and applied to PET alcoholysis to obtain oligomer with given molecular weight range. Under the optimal conditions, PET: EG: POM catalyst = 1.0: 4.0: 0.02 (wt%), 240 °C, 10 min, PET was completely degraded and obtained the oligomer products (Mn < 2000 g/mol) with 72.1 % yield. By investigating the mechanism of the controlled alcoholysis, the formation of flocculent PET was be the key factor in achieving controlled degradation; hydrogen bonding and coordination of POMs are the key interactions to achieve rapid alcoholysis. Finally, oligomers were applied in the preparation of PET-PLA copolymers to follow sustainable route. The incorporation of bio-based polymers demonstrates better inclusiveness to the environment and contributes to harmonious development.
研究领域:
材料科学
·
环境科学
·
高分子化学
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DOI
高影响因子
PROCESS BIOCHEMISTRY
·
2024
·
IF 3.7
Qingjun Jia,Zixuan Zhang,Lankai Su,Shu Bai,Di Cai,Changjing Chen,Linling Yu,Yan Sun
Enzymatic degradation of poly(ethylene terephthalate) (PET) into its corresponding monomers provides an attractive route for green plastic recycling and environmental remediation applications. However, the binding of PET hydrolases toward the PET surface is a rate-limiting step in PET degradation. Hence, we selected three anchor peptides and four linker peptides to fuse the previously engineered leaf-branch compost cutinase for facilitating enzyme binding and improving degradation of real post-consumer PET wastes of Coca Cola and C′eastbon PET bottles, with using the amorphous PET as a control. The systematical characterization of the seven cutinases revealed that the anchor peptide with moderate hydrophobicity plus chaperone activity and the flexible linker peptide with small hydrophobicity but long length were more suitable for each domain to serve its own role, affording the facilitated PET binding affinities and enhanced PET degradation performance. Thus, the optimal fusion cutinase possessed up to 3.3 times higher catalytic efficiency ( k cat / K m ) and 76 % increased long-term degradation performance than the parental cutinase, respectively. Further, complete degradation of C′eastbon PET wastes and 77 % degradation of Coca Cola PET wastes were achieved by the optimal cutinase of 33.3 nmol·g −1 PET in 96 h, proving its superiority against the real post-consumer PET wastes.
研究领域:
环境科学
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生物技术
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材料科学
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化学工程
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Wenbin Guo,Zhengguang Shi,Xue Yu,Jingjing Duan
An important environmental issue is the pollution caused by poly(ethylene terephthalate) (PET) and the emitted monomers terephthalic acid (TPA) and ethylene glycol (EG). The TPA biodegradation pathway has been well documented for the microbial biodegradation and assimilation of PET; however, the PET biodegradation process by marine microorganisms via the EG biodegradation pathway is less understood. Here, we demonstrate how the marine bacteria Pseudomonas chengduensis BC1815’s membrane-anchored PET esterase (OF113_10420) breaks down PET. We also explain the characteristics of this enzyme and demonstrate that the strain assimilates PET via the EG biodegradation pathway. In addition to depolymerizing PET, PET esterase (OF113_10420) hydrolyzes BHET and MHET to generate EG more efficiently in alkaline circumstances. It has been discovered that P. chengduensis BC1815 cells exhibiting surface-displayed PET esterase (OF113_10420) have the potential to function as cell biocatalysts for the breakdown of PET. Additionally, we look into the microbial communities that have PET esterase linked to the EG biodegradation pathway, primarily those belonging to the phyla Proteobacteria and Actinobacteriota. Consequently, research on the microbial absorption and biodegradation of PET via the EG metabolism route increases our knowledge of the bioremediation of PET pollution in the marine environment and contributes to our understanding of the environmental destiny of PET pollutants in the marine environment.
研究领域:
环境科学
·
微生物学
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生物化学
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产品关联
DOI
PubMed
高影响因子
Applied Nanoscience
·
2015
·Vol. 6
·期 4
·575-580
·
IF 0
Wang E. Y.,Li Xuezhao,Duan Y. N.
A new process to fabricate copper pattern on PET substrate is developed in the experiment. Functional ink with ion-adsorption nanoparticles was printed on PET substrate to form the pattern adsorption film. Catalytic ion was adsorbed by amino groups in the adsorption film to catalyze the electroless plating process of copper. The mercapto groups were introduced to the film to enhance the reliability of patterns. In addition, the specific solvent was used in the ink to increase the surface roughness of adsorption film which leads to a better adhesion of the patterns. The conductivity of prepared copper patterns is the same as bulk copper and the patterns show good adhesion on PET substrate.
研究领域:
材料科学
·
纳米技术
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产品关联
DOI
ACS Sensors
·
2025
·
IF 9.1
Zuhua Zeng,Ying Tan,Tiantian Luo,Zhengwei Li,Guihao Hu,Yao Liu,Ling He,Haiyu Wang,Lei Zhong,Haiying Wang,Tianwei Liu,Jiang Zhu
Melanoma is one of the most aggressive forms of skin cancer. Accurate and early diagnosis of melanoma is crucial for improving patient outcomes. This study develops two TYR-activatable molecular probes, Mn-TyrEDTA and Al-18F-TyrEDTA, for the selective detection of melanoma in vivo. In vitro studies reveal that Mn-TyrEDTA exhibits TYR activity-dependent relaxivity enhancement, undergoing TYR-mediated oxidative polymerization, resulting in the formation of paramagnetic oligomers. UV–vis analysis supports this mechanism, showing time- and TYR concentration-dependent increases in broad band absorbance in the UV–vis region, specifically around 475 nm, due to the formation of o-quinone intermediates and melanin-like oligomers. HPLC analysis further confirmed the presence of polar oligomeric products in Mn-TyrEDTA solutions incubated with TYR/O2. MRI studies demonstrate Mn-TyrEDTA’s selective retention and signal enhancement in TYR-expressing melanoma tissues. Furthermore, PET imaging with Al-18F-TyrEDTA conducted using a dual-xenograft mouse model reveals significantly higher uptake and retention of Al-18F-TyrEDTA in TYR-expressing melanoma compared to TYR-negative tumors. This selective retention could be attributed to a TYR-mediated proximity labeling mechanism, where highly reactive quinones form covalent bonds with nearby tumor proteins. In summary, our findings establish Mn-TyrEDTA and Al-18F-TyrEDTA as promising TYR-activatable imaging probes, offering a novel strategy for the early diagnosis and prognosis of melanoma.
研究领域:
医学影像学
·
肿瘤学
·
分子生物学
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产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Renwen Tian,Yan Sun
Extensive use of polyethylene terephthalate (PET) has brought about global environmental problems. A recently reported PET hydrolase (PETase) discovered from Ideonella sakaiensis showed high potential for degrading PET at moderate temperatures, but its activity and stability need further improvement for practical applications. Herein, we proposed to use α-synuclein (αS) as a fusion chaperone and created six PETase-αS fusion enzymes with linkers of different types and lengths. All the fusion enzymes exhibited improved enzymatic performance, presenting 1.5 to 2.6-fold higher activity towards bis-2(hydroxyethyl) terephthalate than PETase, as well as significantly increased stabilities. Fluorescence spectroscopy indicated that the chaperone fusion tightened the overall conformation and resulted in the opening of the substrate binding pocket, which led to the improved thermal stability and catalytic activity of the fusion enzymes. Remarkably, one of the fusion proteins, PETase-[(GS)(EK)] 10 -αS, showed 3.2 to 5.1 times higher PET degradation capability than PETase. The significantly boosted PET degradation performance was not only attributed to the enhanced enzymatic activity and stability, but also possibly due to the binding affinity of the fused αS domain for PET. These findings demonstrated that αS was an effective fusion chaperone for significantly enhancing the enzymatic performance of PETase.
研究领域:
酶学
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生物技术
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环境科学
·
蛋白质工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）