Enzymatic degradation

酶降解
  • 文章类型: Journal Article
    海藻多糖来源广泛,含量丰富,具有多种生物活性,如抗炎,抗肿瘤,抗凝剂,和降低血压。它们可以应用于食品等领域,农业,和医学。然而,大分子海藻多糖溶解性差限制了其进一步应用。有报道表明,海藻寡糖的某些生物活性更广泛,优于海藻多糖。因此,降低多糖的聚合度将是海藻多糖资源高值化利用的关键。海藻多糖降解成藻寡糖的方法主要有三种,物理,化学和酶降解。其中,酶法降解一直是近年来的研究热点。各种类型的藻多糖水解酶和相关的糖苷酶是制备藻寡糖的有力工具,包括α-琼脂糖酶,β-琼脂糖,与琼脂相关的α-新琼脂糖水解酶和β-半乳糖苷酶,κ-角叉菜酶,与角叉菜胶相关的1-角叉菜胶酶和λ-角叉菜胶酶,与卟啉有关的β-卟啉酶,与真菌相关的真菌水解酶,与藻酸盐相关的藻酸盐裂解酶和与ulvan相关的ulvan裂解酶。本文介绍了琼脂寡糖的生物活性,角叉菜胶寡糖,卟啉寡糖,真菌寡糖,并对酶法制备这六种寡糖的研究进展进行了较为详细的综述。同时,提出了今后藻类寡糖的制备和应用所面临的问题和挑战。
    Seaweed polysaccharides have a wide range of sources and rich content, with various biological activities such as anti-inflammatory, anti-tumor, anticoagulant, and blood pressure lowering. They can be applied in fields such as food, agriculture, and medicine. However, the poor solubility of macromolecular seaweed polysaccharides limits their further application. Reports have shown that some biological activities of seaweed oligosaccharides are more extensive and superior to that of seaweed polysaccharides. Therefore, reducing the degree of polymerization of polysaccharides will be the key to the high value utilization of seaweed polysaccharide resources. There are three main methods for degrading algal polysaccharides into algal oligosaccharides, physical, chemical and enzymatic degradation. Among them, enzymatic degradation has been a hot research topic in recent years. Various types of algal polysaccharide hydrolases and related glycosidases are powerful tools for the preparation of algal oligosaccharides, including α-agarases, β-agaroses, α-neoagarose hydrolases and β-galactosidases that are related to agar, κ-carrageenases, ι-carrageenases and λ-carrageenases that are related to carrageenan, β-porphyranases that are related to porphyran, funoran hydrolases that are related to funoran, alginate lyases that are related to alginate and ulvan lyases related to ulvan. This paper describes the bioactivities of agar oligosaccharide, carrageenan oligosaccharide, porphyran oligosaccharide, funoran oligosaccharide, alginate oligosaccharide and ulvan oligosaccharide and provides a detailed review of the progress of research on the enzymatic preparation of these six oligosaccharides. At the same time, the problems and challenges faced are presented to guide and improve the preparation and application of algal oligosaccharides in the future.
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  • 文章类型: Journal Article
    在本研究中,使用鲍鱼(Haliotisdiscushannai)内脏的粗酶制备了一种新的降解魔芋葡甘露聚糖(DKGM),并对其理化性质进行了研究。酶水解后,KGM的粘度从15,500mPa·s明显下降到398mPa·s。对KGM和DKGM的流变性能分析表明,它们是假塑性流体,和假可塑性,粘弹性,熔化温度,酶水解后胶凝温度显著降低,特别是KGM-180和KGM-240。此外,KGM的分子量从1.80×106Da下降,降解时间240分钟后,多分散指数从1.17增加到1.83。与天然KGM相比,DKGM较小的粒度分布进一步表明酶水解减少了低分子量分子链的聚集。FT-IR和FESEM分析表明,断裂的KMG链不影响分子单体的结构特征;然而,酶水解后,分子间相互作用形成的致密三维网络微观结构变为碎片微观结构。这些结果表明,使用来自鲍鱼内脏的粗酶可以控制并有效改变KGM的粘度和流变特性。该工作为DKGM在食品工业中的应用提供了理论指导。
    In the present study, a new degraded konjac glucomannan (DKGM) was prepared using a crude enzyme from abalone (Haliotis discus hannai) viscera, and its physicochemical properties were investigated. After enzymatic hydrolysis, the viscosity of KGM obviously decreased from 15,500 mPa·s to 398 mPa·s. The rheological properties analysis of KGM and DKGMs revealed that they were pseudoplastic fluids, and pseudoplasticity, viscoelasticity, melting temperature, and gelling temperature significantly decreased after enzymatic hydrolysis, especially for KGM-180 and KGM-240. In addition, the molecular weight of KGM decreased from 1.80 × 106 Da, to 0.45 × 106 Da and the polydispersity index increased from 1.17 to 1.83 after 240 min of degradation time. Compared with natural KGM, the smaller particle size distribution of DKGM further suggests enzyme hydrolysis reduces the aggregation of molecular chains with low molecular weight. FT-IR and FESEM analyses showed that the fragmented KMG chain did not affect the structural characteristics of molecular monomers; however, the dense three-dimensional network microstructure formed by intermolecular interaction changed to fragment microstructure after enzyme hydrolysis. These results revealed that the viscosity and rheological properties of KGM could be controlled and effectively changed using crude enzymes from abalone viscera. This work provides theoretical guidance for the promising application of DKGM in the food industry.
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  • 文章类型: Journal Article
    聚对苯二甲酸乙二醇酯(PET)废物的不断积累提出了紧迫的生态挑战,需要有效和经济的处理技术。这里,我们开发了执行化学预处理的化学-生物模块集群,酶促降解,和微生物同化用于PET废物的大规模处理。该模块簇包括(i)化学预处理,涉及通过机械共混以2%的重量比(PET:PCL=98:2)将聚己内酯(PCL)掺入PET中,有效地降低结晶度并增强降解;(ii)使用Thermobifidafusca角质酶变体(4Mz)进行酶促降解,在300g/LPET下实现预处理的PET的完全降解,每克PET的酶负载为1毫克蛋白质;和(iii)微生物同化,华氏红球菌RHA1代谢降解产物,以90%以上的比率同化每个单体。比较生命周期评估表明,我们的模块集群(0.25kgCO2-eq/kgPET)的碳排放量低于其他既定方法的碳排放量。本研究开创了一个无缝结合预处理的闭环系统,降解,和同化过程,从而减轻PET废物对环境的影响并推动循环PET经济的发展。
    The rising accumulation of poly(ethylene terephthalate) (PET) waste presents an urgent ecological challenge, necessitating an efficient and economical treatment technology. Here, we developed chemical-biological module clusters that perform chemical pretreatment, enzymatic degradation, and microbial assimilation for the large-scale treatment of PET waste. This module cluster included (i) a chemical pretreatment that involves incorporating polycaprolactone (PCL) at a weight ratio of 2% (PET:PCL = 98:2) into PET via mechanical blending, which effectively reduces the crystallinity and enhances degradation; (ii) enzymatic degradation using Thermobifida fusca cutinase variant (4Mz), that achieves complete degradation of pretreated PET at 300 g/L PET, with an enzymatic loading of 1 mg protein per gram of PET; and (iii) microbial assimilation, where Rhodococcus jostii RHA1 metabolizes the degradation products, assimilating each monomer at a rate above 90%. A comparative life cycle assessment demonstrated that the carbon emissions from our module clusters (0.25 kg CO2-eq/kg PET) are lower than those from other established approaches. This study pioneers a closed-loop system that seamlessly incorporates pretreatment, degradation, and assimilation processes, thus mitigating the environmental impacts of PET waste and propelling the development of a circular PET economy.
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  • 文章类型: Journal Article
    为了将天然受霉菌毒素污染的小麦谷物重新引入食品价值链,本研究制定了净化策略.为此,第一步,使用冷针穿孔对全麦籽粒进行预处理。通过扫描电子显微镜评估孔径,并使用荧光标记在酶(5nm)和微生物(10μm)的大小范围内确定酶和微生物的可及性,和荧光显微镜。穿孔的小麦籽粒,以及非穿孔颗粒作为对照,然后与选定的微生物(巨大芽孢杆菌Myk145和地衣芽孢杆菌MA572)或与酶ZHD518孵育。两株杆菌均不能显著降低玉米赤霉烯酮(ZEA)的含量,与对照相比,穿孔小麦籽粒和未穿孔小麦籽粒均不存在。相比之下,与对照相比,酶ZHD518显着降低了穿孔和非穿孔小麦籽粒中ZEA的初始浓度。此外,ZHD518与ZEA的体外孵育显示存在ZEA的两种非雌激素降解产物:水解玉米赤霉烯酮(HZEA)和脱羧水解ZEA(DHZEA)。此外,物理预处理导致一部分样品中可检测到的霉菌毒素含量降低。总的来说,这项研究强调了将物理预处理方法与生物净化解决方案相结合的潜力,以解决霉菌毒素污染和减少食物垃圾的相关问题。
    With the aim of reintroducing wheat grains naturally contaminated with mycotoxins into the food value chain, a decontamination strategy was developed in this study. For this purpose, in a first step, the whole wheat kernels were pre-treated using cold needle perforation. The pore size was evaluated by scanning electron microscopy and the accessibility of enzymes and microorganisms determined using fluorescent markers in the size range of enzymes (5 nm) and microorganisms (10 μm), and fluorescent microscopy. The perforated wheat grains, as well as non-perforated grains as controls, were then incubated with selected microorganisms (Bacillus megaterium Myk145 and B. licheniformis MA572) or with the enzyme ZHD518. The two bacilli strains were not able to significantly reduce the amount of zearalenone (ZEA), neither in the perforated nor in the non-perforated wheat kernels in comparison with the controls. In contrast, the enzyme ZHD518 significantly reduced the initial concentration of ZEA in the perforated and non-perforated wheat kernels in comparison with controls. Moreover, in vitro incubation of ZHD518 with ZEA showed the presence of two non-estrogenic degradation products of ZEA: hydrolysed zearalenone (HZEA) and decarboxylated hydrolysed ZEA (DHZEA). In addition, the physical pre-treatment led to a reduction in detectable mycotoxin contents in a subset of samples. Overall, this study emphasizes the promising potential of combining physical pre-treatment approaches with biological decontamination solutions in order to address the associated problem of mycotoxin contamination and food waste reduction.
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  • 文章类型: Journal Article
    木聚糖的独特性能使其对各种行业具有吸引力,包括纸张,食物,和生化生产。虽然对于某些应用来说,保护其自然结构至关重要,对其他人来说,降解成单糖是必不可少的。对于完整的细分,需要使用几种酶,由于其结构的复杂性。事实上,酶催化反应的特异性由表面引导,限制或调节可及性,并提供指导酶作用的结构编码输入。这里,我们使用表面等离子体共振光谱研究富含木聚糖的表面上的酶。通过酶表面动力学模拟研究了扩散和底物形态变化的影响,产生反应速率和常数。我们提出了动力学模型,可以应用于多层生物聚合物膜的降解。最先进的模型已成功应用于用聚羟基丁酸酯-解聚酶处理的聚羟基丁酸酯薄膜的降解,从而得到了验证。本文导出的模型可用于量化各种酶在异质环境中生物聚合物上的降解动力学。通常在工业过程中普遍存在。确定影响反应速率的关键因素,例如抑制,将有助于量化复杂系统中的复杂动力学。
    Xylans\' unique properties make it attractive for a variety of industries, including paper, food, and biochemical production. While for some applications the preservation of its natural structure is crucial, for others the degradation into monosaccharides is essential. For the complete breakdown, the use of several enzymes is required, due to its structural complexity. In fact, the specificity of enzymatically-catalyzed reactions is guided by the surface, limiting or regulating accessibility and serving structurally encoded input guiding the actions of the enzymes. Here, we investigate enzymes at surfaces rich in xylan using surface plasmon resonance spectroscopy. The influence of diffusion and changes in substrate morphology is studied via enzyme surface kinetics simulations, yielding reaction rates and constants. We propose kinetic models, which can be applied to the degradation of multilayer biopolymer films. The most advanced model was verified by its successful application to the degradation of a thin film of polyhydroxybutyrate treated with a polyhydroxybutyrate-depolymerase. The herein derived models can be employed to quantify the degradation kinetics of various enzymes on biopolymers in heterogeneous environments, often prevalent in industrial processes. The identification of key factors influencing reaction rates such as inhibition will contribute to the quantification of intricate dynamics in complex systems.
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  • 文章类型: Journal Article
    背景:树脂-牙本质界面的稳定性仍然非常可疑。这项研究的目的是评估Salvadorapersica对树脂-牙本质粘结耐久性的影响。
    方法:提取的人类第三磨牙用于提供中冠状牙本质,酸蚀后用20%的Salvadorapersica提取物处理1分钟。在24小时和6个月后评估微拉伸粘结强度和界面纳米渗漏。在用Salvadorapersica提取物处理之前和之后,使用三点弯曲测试来测量完全脱矿质的牙本质棒的刚度。羟脯氨酸释放试验也用于测量内源性牙本质蛋白酶对胶原的降解。使用双向ANOVA进行统计分析,然后进行事后Bonferroni检验和非配对t检验。P值<0.05被认为具有统计学意义。
    结果:使用Salvadorapersica作为带有蚀刻和冲洗粘合剂的附加底漆不会影响即时粘合强度和纳米泄漏(p>0.05)。六个月后,对照组的粘结强度降低(p=0.007),和纳米存储量增加(p=0.006),而Salvadorapersica组与24h组相比,其结合强度和纳米体积没有显着差异(p>0.05)。与对照组相比,Salvadorapersica增加了牙本质硬度并减少了胶原蛋白降解(p<0.001)。
    结论:Salvadorapersica提取物预处理酸蚀牙本质保存树脂-牙本质结合界面6个月。
    结论:树脂-牙本质结合界面的耐久性仍然非常可疑。内源性牙本质基质金属蛋白酶在这些界面内的牙本质胶原的降解中起重要作用。Salvadorapersica可能会在更长的时间内保留树脂-牙本质界面,从而提高树脂复合材料修复体的临床成功率和寿命。
    BACKGROUND: The stability of resin-dentin interfaces is still highly questionable. The aim of this study was to evaluate the effect of Salvadora persica on resin-dentin bond durability.
    METHODS: Extracted human third molars were used to provide mid-coronal dentin, which was treated with 20% Salvadora persica extract for 1 min after acid-etching. Microtensile bond strength and interfacial nanoleakage were evaluated after 24 h and 6 months. A three-point flexure test was used to measure the stiffness of completely demineralized dentin sticks before and after treatment with Salvadora persica extract. The hydroxyproline release test was also used to measure collagen degradation by endogenous dentin proteases. Statistical analysis was performed using two-way ANOVA followed by post hoc Bonferroni test and unpaired t-test. P-values < 0.05 were considered statistically significant.
    RESULTS: The use of Salvadora persica as an additional primer with etch-and-rinse adhesive did not affect the immediate bond strengths and nanoleakage (p > 0.05). After 6 months, the bond strength of the control group decreased (p = 0.007), and nanoleakage increased (p = 0.006), while Salvadora persica group showed no significant difference in bond strength and nanoleakage compared to their 24 h groups (p > 0.05). Salvadora persica increased dentin stiffness and decreased collagen degradation (p < 0.001) compared to their controls.
    CONCLUSIONS: Salvadora persica extract pretreatment of acid-etched dentin preserved resin-dentin bonded interface for 6 months.
    CONCLUSIONS: Durability of resin-dentin bonded interfaces is still highly questionable. Endogenous dentinal matrix metalloproteinases play an important role in degradation of dentinal collagen within such interfaces. Salvadora persica may preserve resin-dentin interfaces for longer periods of time contributing to greater clinical success and longevity of resin composite restorations.
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  • 文章类型: Journal Article
    已开发出一种使用肟的通用且强大的端基衍生方法,用于检测合成聚异戊二烯和聚丁二烯的氧化降解。该方法具有广泛的适用性,通过与凝胶渗透色谱耦合的紫外(UV)检测,有效地监测宽分子量范围内的降解。重要的是,它可以通过衍生化诱导的紫外线最大位移来有效监测降解,即使存在过量的未降解多烯,克服了以前报道的折射率检测器的限制。值得注意的是,这种基于肟的衍生方法用于合成聚异戊二烯的酶促降解实验,其特征在于橡胶加氧酶LcpK30的顺式:反式比例。它揭示了分子量超过1000gmol-1的聚异戊二烯的衍生酶降解产物中的大量紫外线吸收-该酶对此类合成聚异戊二烯的活性的空前启示。这种创新方法有望成为推进合成聚异戊二烯和聚丁二烯降解研究的宝贵工具,特别是在低有机催化或酶促降解活性的条件下。凭借其广泛的适用性和揭示先前隐藏的退化过程的能力,它代表了对可持续聚合物化学的显著贡献。
    A versatile and robust end-group derivatization approach using oximes has been developed for the detection of oxidative degradation of synthetic polyisoprenes and polybutadiene. This method demonstrates broad applicability, effectively monitoring degradation across a wide molecular weight range through ultraviolet (UV)-detection coupled to gel permeation chromatography. Importantly, it enables the effective monitoring of degradation via derivatization-induced UV-maximum shifts, even in the presence of an excess of undegraded polyene, overcoming limitations previously reported with refractive index detectors. Notably, this oxime-based derivatization methodology is used in enzymatic degradation experiments of synthetic polyisoprenes characterized by a cis: trans ratio with the rubber oxygenase LcpK30. It reveals substantial UV absorption in derivatized enzymatic degradation products of polyisoprene with molecular weights exceeding 1000 g mol-1 - an unprecedented revelation for this enzyme\'s activity on such synthetic polyisoprenes. This innovative approach holds promise as a valuable tool for advancing research into the degradation of synthetic polyisoprenes and polybutadiene, particularly under conditions of low organocatalytic or enzymatic degradation activity. With its broad applicability and capacity to reveal previously hidden degradation processes, it represents a noteworthy contribution to sustainable polymer chemistry.
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  • 文章类型: Journal Article
    冠状动脉支架是救命设备,每年植入数百万种这种装置来治疗冠心病。目前治疗的金标准是药物洗脱支架,其涂覆有可生物降解的聚合物层,所述聚合物层洗脱抗增殖药物以防止由于新生内膜增生引起的再狭窄。支架通常与全身性抗血小板治疗配对以防止支架血栓形成。尽管他们在临床上取得了成功,目前的支架具有显著的局限性,包括诱导局部炎症,导致增生;缺乏促进血栓形成的血液相容性,抗血小板治疗的需求增加;内皮化有限,这是治愈过程中的关键步骤。在这项研究中,我们设计了一种新的材料作为下一代药物洗脱支架涂层,解决了上述局限性.具体来说,我们开发了一种用REDV细胞粘附配体功能化的重组蜘蛛丝材料,在心血管环境中促进内皮细胞特异性粘附的肽基序。我们说明了这种REDV修饰的蜘蛛丝变体[eADF4(C16)-REDV]是一种内皮细胞特异性材料,可以促进近汇合的内皮形成。我们还使用人全血进行了血液相容性测定,并证明蜘蛛丝材料在静态和流动条件下都表现出优异的血液相容性。此外,我们表明该材料表现出缓慢的酶介导降解。最后,我们说明了从重组蜘蛛丝涂层中加载和释放临床相关药物依维莫司的能力,其数量和速度与商业设备相似。这些结果支持使用REDV官能化的重组蜘蛛丝作为药物洗脱支架的涂层。
    Coronary artery stents are life-saving devices, and millions of these devices are implanted annually to treat coronary heart disease. The current gold standard in treatment is drug-eluting stents, which are coated with a biodegradable polymer layer that elutes antiproliferative drugs to prevent restenosis due to neointimal hyperplasia. Stenting is commonly paired with systemic antiplatelet therapy to prevent stent thrombosis. Despite their clinical success, current stents have significant limitations including inducing local inflammation that drives hyperplasia; a lack of hemocompatibility that promotes thrombosis, increasing need for antiplatelet therapy; and limited endothelialization, which is a critical step in the healing process. In this research, we designed a novel material for use as a next-generation coating for drug-eluting stents that addresses the limitations described above. Specifically, we developed a recombinant spider silk material that is functionalized with an REDV cell-adhesive ligand, a peptide motif that promotes specific adhesion of endothelial cells in the cardiovascular environment. We illustrated that this REDV-modified spider silk variant [eADF4(C16)-REDV] is an endothelial-cell-specific material that can promote the formation of a near-confluent endothelium. We additionally performed hemocompatibility assays using human whole blood and demonstrated that spider silk materials exhibit excellent hemocompatibility under both static and flow conditions. Furthermore, we showed that the material displayed slow enzyme-mediated degradation. Finally, we illustrated the ability to load and release the clinically relevant drug everolimus from recombinant spider silk coatings in a quantity and at a rate similar to that of commercial devices. These results support the use of REDV-functionalized recombinant spider silk as a coating for drug-eluting stents.
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  • 文章类型: Journal Article
    脱氧雪腐镰刀菌烯醇(DON)是全球范围内危害人类和动物健康的最广泛的真菌毒素污染物。它是关键的毒力因子,可以刺激致病性镰刀菌在小麦植株中的传播。控制DON和镰刀菌病极大地有助于食品安全,依赖于化学杀菌剂。这里,我们报道了一种新型土壤细菌对DON的生物降解,IavosiaFS10-7及其对镰刀菌冠腐病(FCR)的生物防治作用。我们证明菌株FS10-7通过形成3-酮-DON中间体将DON降解为3-epi-DON。在有氧条件下,这种降解活性可以保持在宽范围的pH(4-10)和温度(16-42°C)值下。值得注意的是,在实验室条件下的体外培养皿试验和温室条件下的盆栽实验中,菌株FS10-7对由赤霉病和假赤霉病引起的FCR病表现出实际的抑制作用。初步研究了菌株FS10-7的生物防治能力的潜在机制,认为其与其高DON降解活性有关,而不是直接拮抗作用。这些结果为进一步开发能够生物降解谷物和衍生产品中霉菌毒素的生物制剂奠定了基础,因此,由产生DON的病原体引起的生物防治植物病害。
    Deoxynivalenol (DON) is the most widespread mycotoxin contaminant hazardous to human and animal health globally. It acts as a crucial virulence factor to stimulate the spread of pathogenic Fusarium within wheat plants. Control of DON and Fusarium disease contributes enormously to food safety, which relies on chemical fungicides. Here, we report the biodegradation of DON using a novel soil bacterium, Devosia insulae FS10-7, and its biocontrol effect against Fusarium crown rot. We demonstrated that strain FS10-7 degraded DON to 3-epi-DON by forming a 3-keto-DON intermediate. Such degradation activity can be maintained at a wide range of pH (4 to 10) and temperature (16 to 42°C) values under aerobic conditions. Notably, strain FS10-7 exhibited practical inhibitory effects on Fusarium crown rot disease caused by F. graminearum and F. pseudograminearum in the in vitro Petri dish test under laboratory conditions and the pot experiment under greenhouse conditions. The mechanisms underlying the biocontrol ability of strain FS10-7 were preliminarily investigated to be associated with its high DON-degrading activity rather than direct antagonism. These results establish the foundation to develop further bioagents capable of biodegrading mycotoxins in cereals and derived products and, accordingly, biocontrol plant diseases caused by DON-producing pathogens.
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  • 文章类型: Journal Article
    全氟烷基酸(PFAA)被认为是永远的化学品,越来越多地关注它们的危险影响。然而,PFAA的生态效应尚不清楚。环境DNA(eDNA)作为环境基因库,通常收集用于评估污染物的生态毒理学影响。在这项研究中,我们发现所有调查过的PFAA,包括全氟己酸,全氟辛酸,全氟壬酸,全氟辛烷磺酸,即使在低浓度(0.02和0.05mg/L),以非线性剂量效应关系加速DNA的酶促降解,DNA降解片段大小在降解15分钟和30分钟后低于1,000bp和200bp,分别。这种现象归因于PFAA与DNA中AT碱基之间通过凹槽结合的结合相互作用。范德华力(特别是分散力)和氢键是主要的结合力。DNA与PFAA结合导致碱基堆积和右手螺旋度降低,导致松散的DNA结构暴露了更多降解酶的消化位点,加速DNA的酶降解.全球生态风险评价结果表明,在来自11个污染热点国家(如美国,加拿大,和中国)。这项研究的发现显示了对PFAA对生物大分子环境命运的影响的新见解,并揭示了PFAA在环境中隐藏的分子生态效应。
    Perfluoroalkyl acids (PFAAs) are considered forever chemicals, gaining increasing attention for their hazardous impacts. However, the ecological effects of PFAAs remain unclear. Environmental DNA (eDNA), as the environmental gene pool, is often collected for evaluating the ecotoxicological effects of pollutants. In this study, we found that all PFAAs investigated, including perfluorohexanoic acid, perfluorooctanoic acid, perfluorononanoic acid, and perfluorooctane sulfonate, even at low concentrations (0.02 and 0.05 mg/L), expedited the enzymatic degradation of DNA in a nonlinear dose-effect relationship, with DNA degradation fragment sizes being lower than 1,000 bp and 200 bp after 15 and 30 min of degradation, respectively. This phenomenon was attributed to the binding interaction between PFAAs and AT bases in DNA via groove binding. van der Waals force (especially dispersion force) and hydrogen bonding are the main binding forces. DNA binding with PFAAs led to decreased base stacking and right-handed helicity, resulting in loose DNA structure exposing more digestion sites for degrading enzymes, and accelerating the enzymatic degradation of DNA. The global ecological risk evaluation results indicated that PFAA contamination could cause medium and high molecular ecological risk in 497 samples from 11 contamination-hot countries (such as the USA, Canada, and China). The findings of this study show new insights into the influence of PFAAs on the environmental fates of biomacromolecules and reveal the hidden molecular ecological effects of PFAAs in the environment.
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