JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2026
·Vol. 74
·期 33
·26532-26543
·
IF 6.7
Chen Yuehua,Liu Peng,Sheng Binbin,Xing Jiaxin,Ouyang Jia,Zheng Zhaojuan
Lignocellulosic
biomass is an abundant renewable resource that
is rich in aldohexoses and aldopentoses. Efficient biocatalysts for
aldopentose oxidation remain limited, and few enzymes exhibit high
catalytic efficiency toward both aldohexoses and aldopentoses. Here,
a naturally promiscuous pyrroloquinoline quinone-dependent glucose
dehydrogenase (PQQ-GDH) from Pseudomonas fragi NL20W was selected as an engineering template and tailored by semirational
design to expand aldopentose oxidation while preserving native d -glucose activity. The V706P/L723 M mutant exhibited markedly
enhanced catalytic efficiency toward d -xylose and l -arabinose, reaching 8.0- and 2.4-fold those of the wild-type, respectively,
while its efficiency toward d -glucose was 1.3-fold that of
the wild-type. Molecular simulations suggested that the improved catalysis
was associated with an optimized substrate positioning and enhanced
conformational flexibility of the active-site region. This study highlights
the significance of natural enzyme scaffold selection in substrate
scope engineering and expands the application potential of PQQ-GDH
in the sustainable valorization of lignocellulosic sugars.
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ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Ning Xia,Fengli Gao,Gang Liu,Yong Chang,Lin Liu
Background Small molecule mimics offer the advantages of easy preparation, good thermodynamic stability, and reproducible catalytic activity. However, most of the reported organic artificial mimics face challenges including low catalytic activity, oxidative self-destruction, and auto-aggregation into inactive dimers. Therefore, novel organic mimics with high catalytic activity as well as good thermal and environmental stability are highly desirable. Results We found that pyrroloquinoline quinone (PQQ), a nutritionally important growth factor, displayed significant peroxidase-like activity to catalyze the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) into blue oxidized TMB (oxTMB) by H 2 O 2 . Its catalytic activity surpassed that of other organic small molecules reported previously, including fluorescein derivatives and adenosine/guanosine triphosphate. Based on the reduction of oxTMB by the enzymatically generated ascorbic acid (AA), the PQQ/TMB-based system was used to monitor alkaline phosphatase (ALP) activity with ascorbic acid 2−phosphate (AAP) as the substrate. This sensing system allowed for the determination of ALP with a detection limit of 1 mU/mL. Furthermore, we discovered that PQQ can coordinate with Cu 2+ to form metal-organic nanoparticles. The building blocks of two active cofactors endowed the nanoparticles with impressive functionalities for biocatalytic applications. With Cu-PQQ nanoparticles as signal labels, colorimetric immunoassays of prostate specific antigen (PSA) were achieved with a lowest detectable concentration down to 0.1 pg/mL. Significance This work is valuable for the design of novel biosensors by utilizing PQQ as an artificial enzyme because of its high catalytic activity, good stability, ease of storage, and simple chemical structure.
研究领域:
生物化学
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分析化学
·
纳米技术
·
生物传感器
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Materials Today Bio
·
2022
·
IF 10.761
Yu-Wei Ge,Min Chu,Zi-Yang Zhu,Qin-Fei Ke,Ya-Ping Guo,Chang-Qing Zhang,Wei-Tao Jia
In situ regeneration of large-segment bone defects is a difficult clinical problem. Here, we innovatively developed magnetically oriented micro-cellulose fibres using nano-hydroxyapatite/chitosan (CEF/Fe 3 O 4 /HA/CS) and loaded an NFκB pathway inhibitor on the surface of magnetically oriented cellulose fibres (CEF/Fe 3 O 4 /HA/CS/PQQ) prepared as a layered bioscaffold. CEF/Fe 3 O 4 /HA/CS/PQQ was constructed by layering HA/CS sheets. Nano-hydroxyapatite was deposited on the surface of cellulose fibres, then the magnetic nanoparticles on the cellulose fibres were aligned on the surface of chitosan under a magnetic field. Oriented cellulose fibres enhanced the compressive properties of the scaffold, with an average maximum compressive strength of 1.63 MPa. The CEF/Fe 3 O 4 /HA/CS/PQQ layered scaffold was filled into the body, and the acute inflammatory response (IL-1β and TNF-α) was suppressed through the early sustained release of PQQ. The CEF/Fe 3 O 4 /HA/CS/PQQ-layered scaffold further inhibited the osteoclasts differentiation. It was further found that the nano-hydroxyapatite on the surface of oriented cellulose fibres promoted the formation and migration of new blood vessels, accelerated the processing of collagen-I fibres to cartilage, and endochondral ossification. Hence, the development of the CEF/Fe 3 O 4 /HA/CS/PQQ layered scaffold with oriented fibres guides bone growth direction and pro-osteogenesis activity and provides a novel strategy for the in situ regeneration of large segmental bone defects.
研究领域:
生物材料学
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组织工程学
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再生医学
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Nanomaterials
·
2021
·Vol. 11
·期 7
·1757
·
IF 5.076
Xiaohua Ma,Dehua Deng,Ning Xia,Yuanqiang Hao,Lin Liu
Nanocatalysts are a promising alternative to natural enzymes as the signal labels of electrochemical biosensors. However, the surface modification of nanocatalysts and sensor electrodes with recognition elements and blockers may form a barrier to direct electron transfer, thus limiting the application of nanocatalysts in electrochemical immunoassays. Electron mediators can accelerate the electron transfer between nanocatalysts and electrodes. Nevertheless, it is hard to simultaneously achieve fast electron exchange between nanocatalysts and redox mediators as well as substrates. This work presents a scheme for the design of electrochemical immunosensors with nanocatalysts as signal labels, in which pyrroloquinoline quinone (PQQ) is the redox-active center of the nanocatalyst. PQQ was decorated on the surface of carbon nanotubes to catalyze the electrochemical oxidation of tris(2-carboxyethyl)phosphine (TCEP) with ferrocenylmethanol (FcM) as the electron mediator. With prostate-specific antigen (PSA) as the model analyte, the detection limit of the sandwich-type immunosensor was found to be 5 pg/mL. The keys to success for this scheme are the slow chemical reaction between TCEP and ferricinum ions, and the high turnover frequency between ferricinum ions, PQQ. and TCEP. This work should be valuable for designing of novel nanolabels and nanocatalytic schemes for electrochemical biosensors.Keywords:electrochemical immunosensor;nanocatalyst;redox cycling;quinone
研究领域:
生物传感
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分析化学
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International Journal of Polymeric Materials and Polymeric Biomaterials
·
2025
·
IF 2.6
Shengnan Zheng,Chuzhou Wen,Jiaxue Tang,Changkai Sun,Fengtao Wang,Shui Guan
Pyrroloquinoline quinone (PQQ) is a redox cofactor that has been shown to have strong antioxidant capacity and neuroprotective effects and has been extensively studied in recent years. However, PQQ small molecule compounds have poorly stability and low bioavailability in vivo, making it difficult to exert drug activity for long periods of time. In this study, we employed the EDC/NHS method to graft PQQ onto carboxymethyl chitosan (CMCS) to improve the utilization of PQQ. The obtained PQQ-g-CMCS product was a water-soluble copolymer, and the grafting rate could be controlled by adjusting the pH and the raw material feeding ratio. The PQQ-g-CMCS samples were characterized using FT-IR, UR-Vis, NMR, and XRD spectroscopy, suggesting a conjugation reaction between the amino groups of CMCS and the carboxyl groups of PQQ. Specifically, the in vitro antioxidant experiments showed that the Fe2+ chelating activity of the grafted copolymer was significantly enhanced. In addition, the PQQ-g-CMCS copolymer also exhibited good biocompatibility and significant protective effect against H2O2-induced oxidative damage in SH-SY5Y cells. These results preliminarily indicate that PQQ-g-CMCS may be a promising antioxidant material for applications such as drug release and tissue engineering.
研究领域:
高分子化学
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神经科学
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药学
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材料科学
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生物化学
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Food Bioscience
·
2024
·
IF 4.8
Shan Li,Xiong Xiang,Yinglu Qing,Yanbo Wang,Min Wang,Jiaoyan Ren
Cell morphology and motility are crucial trait of somatic cell phenotype, closely linked to cellular function and susceptibility to external stimuli. Oxidative damage impacts cell functionality, ultimately influencing cell morphology and motility. In this study, the changes in cell state were characterized and quantified through dynamic analysis of cell morphodynamic parameters, thereby reflecting the impairment of cellular function. The protective effects of antioxidants on oxygen-damaged cells were assessed in terms of cellular morphology and motility, based on the aforementioned findings. In this study, the protective effect of pyrroloquinoline quinone (PQQ) on cells in d -galactose-induced oxidative damage model was evaluated using the long-term live cell imaging technique, focusing on cell morphodynamic parameters. Additionally, cell proliferation and metabolic activity were assessed at the end to investigate the relationship between cell function and morphodynamics. The results showed that oxidative damage compromised cellular proliferation ( p < 0.001) and metabolic function, while also inducing alterations in cellular morphology and motility. Morphological parameters (cellular branches, surface, nuclear area, shape factor and quotient) and motility parameters (cell migration velocity and directionality) effectively characterized and quantified the observed trends in cellular morphology and motility. Meanwhile, real-time analysis showed that PQQ improved oxygen-induced morphological changes in cells, protected cellular motility effectively ( p < 0.01), and exhibited significant protective effects during the initial stages of injury. Phase relationship analysis data revealed the correlation between cell morphology, motility, and function. This implies that quantifying cell morphodynamics could offer a novel perspective for assessing how antioxidants shield cells against oxidative damage.
研究领域:
细胞生物学
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分子生物学
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生物医学工程
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Food Bioscience
·
2023
·
IF 5.2
Xiong Xiang,Amakye William Kwame,Yinglu Qing,Shan Li,Min Wang,Jiaoyan Ren
Effect of antioxidants in oxidative stress-induced cell damage has been extensively studied, but its effects on cell macroscopic phenomena have rarely been explored. Cell morphology and motility are two interrelated cellular processes reflecting cellular function phenotype, and the real-time imaging technology is key for the study of these processes. In this study, we used two known antioxidants, pyrroloquinoline quinone (PQQ) and rutin , to explore the antioxidant effects on cell morphology and motility in rotenone-damaged NIH3T3 cells, as well as roles in their antioxidant function based on Cytation 7 Cell Imaging Multi-Mode Reader. First, NIH-3T3 cells were pretreated with PQQ and rutin for 4 h and then rotenone was used to induce oxidative damage. It was found that PQQ (2 μM) and rutin (300 μM) had similar protective effects on the proliferation activity of rotenone-damaged cells. Subsequently, the morphology and motility of the treated cells were quantified. Results showed that both PQQ and rutin could significantly inhibit morphological changes including cell shape index and cell surface of the damaged cells, however PQQ had a stronger effect on cell motility under the specific experimental concentrations. Using principal component analysis (PCA), we further demonstrated that the quantified cell morphology and motility were consistent with the cell proliferation activity. Consequently, quantification of cell morphology and motility as evaluation indices may serve as potential reference values for the evaluation of biological activity of antioxidants.
研究领域:
细胞生物学
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药理学
·
生物医学工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Bin Ma,Jiafeng Niu,Hao Zhu,Huibing Chi,Zhaoxin Lu,Fengxia Lu,Ping Zhu
The oxidative reaction of Fusarium mycotoxin deoxynivalenol (DON) using the dehydrogenase is a desirable strategy and environmentally friendly to mitigate its toxicity. However, a critical issue for these dehydrogenases shows widespread substrate promiscuity. In this study, we conducted pocket reshaping of Devosia strain A6-243 pyrroloquinoline quinone (PQQ)-dependent dehydrogenase (DADH) on the basis of protein structure and kinetic analysis of substrate libraries to improve preference for particular substrate DON (10a). The variant presented an increased preference for substrate 10a and enhanced catalytic efficiency. A 4.7-fold increase in preference for substrate 10a was observed. Kinetic profiling and molecular dynamics (MD) simulations provided insights into the enhanced substrate specificity and activity. Moreover, the variant exhibited stronger conversion of substrate 10a to 3-keto-DON compared to the wild DADH. Overall, this study provides a feasible protocol for the redesign of PQQ-dependent dehydrogenases with favourable substrate specificity and catalytic activity, which is desperately needed for DON antidote development.
研究领域:
生物技术
·
酶学
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毒理学
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分子生物学
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