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Cascading oxidoreductases-like nanozymes for high selective and sensitive fiuorescent detection of ascorbic acid

Chinese Chemical Letters 2025年第4期36卷 627-632页

作者： Ying Wang Hong Yang Caixia Zhu Qing Hong xuwen cao Kaiyuan Wang Yuan Xu Yanfei Shen Songqin Liu Yuanjian Zhang Jiangsu Engineering Laboratory of Smart Carbon-Rich Materials and Devices Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical ResearchSchool of Chemistry and Chemical EngineeringMedical SchoolSoutheast UniversityNanjing 211189China

Compared with natural enzymes, nanozymes have the advantages of high stability and low cost;however,selectivity and sensitivity are key issues that prevent their further development. In this study, we report a cascade nanozymatic system with significantly improved selectivity and sensitivity that combines more substrate-specific reactions and sensitive fiuorescence detection. Taking detection of ascorbic acid(AA)as an example, a cascade catalytic reaction system consisting of oxidase-like N-doped carbon nanocages(NC) and peroxidase-like copper oxide(Cu O) improved the reaction selectivity in transforming the substrate into the target product by more than 1200 times against the interference of uric acid. The cascade catalytic reaction system was also applicable for transfer from open reactors into a spatially confined microfiuidic device, increasing the slope of the calibration curves by approximately 1000-fold with a linear detection range of 2.5 nmol/L to 100 nmol/L and a low limit of detection of 0.77 nmol/L. This work offers a new strategy that achieves significant improvements in selectivity and sensitivity.

关键词： Nanozyme Fluorescence Selectivity Sensitivity Ascorbic acid

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High-quality chromosome-level genome assembly of the whitespotted conger (Conger myriaster)

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SCIENTIFIC DATA 2025年第1期12卷 1-9页

作者： Han, Shenglei Li, Chen Li, Shuo Chen, Yan Wang, Chenggang Liu, Kaiqiang Liu, Yuyan Wang, Hong-Yan Wang, Qian cao, xuwen Shi, Bao Shao, Changwei Jiangsu Ocean Univ Jiangsu Key Lab Marine Bioresources & Environm Lianyungang 222005 Peoples R China Chinese Acad Fishery Sci Yellow Sea Fisheries Res Inst State Key Lab Mariculture Biobreeding & Sustainabl Qingdao 266071 Shandong Peoples R China Qingdao Marine Sci & Technol Ctr Lab Marine Fisheries Sci & Food Prod Proc Qingdao 266237 Shandong Peoples R China Haiyang Yellow Sea Fisheries Co Ltd Yantai 265100 Peoples R China Chinese Acad Fishery Sci Hebei Key Lab Bohai Sea Fish Germplasm Resources C Beidaihe Cent Expt Stn Qinhuangdao 066100 Peoples R China

The whitespotted conger (Conger myriaster) is an ecologically and economically significant benthic marine species widely distributed across East Asia's coastal waters. Despite this importance, the genomic resources for this species remain limited, hindering evolutionary and aquaculture research. Here, we present the first high-quality chromosome-level genome assembly of C. myriaster using PacBio CLR, WGS, 10X Genomics and Hi-C data. The resulting 1.09 Gb genome assembly exhibits excellent contiguity, with 97.49% of sequences anchored onto 19 chromosomes. The assembled genome achieved a BUSCO completeness stands at 98.00%, containing 34.80% repetitive sequences and 24,063 predicted protein-coding genes. This foundational genomic resource overcomes a major limitation, providing the essential framework for future investigations into the evolutionary adaptations and for the genetic improvement of C. myriaster in aquaculture.

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The marine environmental microbiome mediates physiological outcomes in host nematodes

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BMC BIOLOGY 2024年第1期22卷 1页

作者： Xue, Yiming Xie, Yusu cao, xuwen Zhang, Liusuo Chinese Acad Sci Inst Oceanol CAS Qingdao 266071 Peoples R China Chinese Acad Sci Inst Oceanol Shandong Prov Key Lab Expt Marine Biol Qingdao 266071 Peoples R China Qingdao Natl Lab Marine Sci & Technol Lab Marine Biol & Biotechnol Qingdao 266237 Peoples R China Chinese Acad Sci Ctr Ocean Mega Sci 7 Nanhai Rd Qingdao 266071 Peoples R China Univ Chinese Acad Sci Beijing 100049 Peoples R China

Background Nematodes are the most abundant metazoans in marine sediments, many of which are bacterivores;however, how habitat bacteria affect physiological outcomes in marine nematodes remains largely unknown. Results Here, we used a Litoditis marina inbred line to assess how native bacteria modulate host nematode physiology. We characterized seasonal dynamic bacterial compositions in L. marina habitats and examined the impacts of 448 habitat bacteria isolates on L. marina development, then focused on HQbiome with 73 native bacteria, of which we generated 72 whole genomes sequences. Unexpectedly, we found that the effects of marine native bacteria on the development of L. marina and its terrestrial relative Caenorhabditis elegans were significantly positively correlated. Next, we reconstructed bacterial metabolic networks and identified several bacterial metabolic pathways positively correlated with L. marina development (e.g., ubiquinol and heme b biosynthesis), while pyridoxal 5'-phosphate biosynthesis pathway was negatively associated. Through single metabolite supplementation, we verified CoQ10, heme b, acetyl-CoA, and acetaldehyde promoted L. marina development, while vitamin B6 attenuated growth. Notably, we found that only four development correlated metabolic pathways were shared between L. marina and C. elegans. Furthermore, we identified two bacterial metabolic pathways correlated with L. marina lifespan, while a distinct one in C. elegans. Strikingly, we found that glycerol supplementation significantly extended L. marina but not C. elegans longevity. Moreover, we comparatively demonstrated the distinct gut microbiota characteristics and their effects on L. marina and C. elegans physiology. Conclusions Given that both bacteria and marine nematodes are dominant taxa in sedimentary ecosystems, the resource presented here will provide novel insights to identify mechanisms underpinning how habitat bacteria affect nematode biology in a more natural context. Ou

关键词： Litoditis marina Full-length 16S rRNA sequencing Marine bacterial collection Host-microbe interactions Metabolic models Gene knockout Gut microbiota

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Identification of Ly2 members as antimicrobial peptides from zebrafish Danio rerio

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BIOSCIENCE REPORTS 2017年第1期37卷 BSR20160265-BSR20160265页

作者： Liu, Xuemin cao, xuwen Wang, Su Ji, Guangdong Zhang, Shicui Li, Hongyan Ocean Univ China Inst Evolut & Marine Biodivers Dept Marine Biol Qingdao 266003 Peoples R China Ocean Univ China Dept Marine Biol Lab Evolut & Dev Qingdao 266003 Peoples R China

The emergence of multidrug-resistant (MDR) microbes caused by overuse of antibiotics leads to urgent demands for novel antibiotics exploration. Our recent data showed that Ly2.1-3 (a novel lymphocyte antigen 6 (Ly6) gene cluster) were proteins with cationic nature and rich in cysteine content, that are characteristic of antimicrobial peptides (AMPs) and their expression were all significantly up-regulated after challenge with lipopolysaccharide (LPS). These strongly suggested that Ly2.1-3 are potential AMPs, but firm evidence are lacking. Here, we clearly showed that the recombinant proteins of Ly2.1-3 were capable of killing Gram-negative bacteria Aeromonas hydrophila and Escherichia coli, while they had little bactericidal activity against the Gram-positive bacteria Staphylococcus aureus and Bacillus subtilis. We also showed that recombinant proteins Ly2.1-3 (rLy2.1-3) were able to bind to the Gram-negative bacteria A. hydrophila, E. coli and the microbial signature molecule LPS, but not to the Gram-positive bacteria S. aureus and B. subtilis as well as the microbial signature molecule LTA. Moreover, the Scatchard analysis revealed that rLy2.1-3 could specifically bind to LPS. Finally, we found that Ly2.1-3 were not cytotoxic to mammalian cells. All these together indicate that Ly2.1-3 can function as AMPs.

关键词： zebrafish Danio rerio Ly6 gene cluster Antimicrobial peptides

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Gill and brain transcriptomic analysis of mandarin fish(Siniperca chuatsi) reveals hypoxia-induced mitochondrial dysfunction and modulation of metabolism

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COMPARATIVE BIOCHEMISTRY AND PHYSIOLOGY D-GENOMICS & PROTEOMICS 2025年 53卷 101367页

作者： Ding, Weidong cao, Liping cao, Zheming Bing, xuwen Chinese Acad Fishery Sci Minist Agr Freshwater Fisheries Res Ctr Key Lab Freshwater Fisheries & Germplasm Resources Wuxi 214081 Peoples R China

The oxygen content in the fish ponds is facing greater challenges than before in the aquaculture of mandarin fish (Siniperca chuatsi) due to the change of climate and eutrophication. Until now, little is known about the molecular mechanisms underlying the harmful effects of hypoxia on this species. In this work, we built transcriptomes for the mandarin fish that were exposed to decreased oxygen concentration at two times points (24 hand 96 h). The respiratory metabolism activities of pyruvate kinase (PK), hexokinase (HK), lactate dehydrogenase (LDH), succinate dehydrogenase (SDH) and malate dehydrogenase (MDH) had different significantly changes during hypoxic treatment. Histological observation of the gill and brain also revealed some damages by hypoxia. A total of 196,355 transcripts were involved in the Gene Ontology analysis, and the numbers of differentially expressed genes (DEGs) in the brain and the gill between the control and experiment groups are 141 and 552 respectively involved in the different hypoxic stress time. The DEGs were then analyzed using KEGG enrichment analysis. The results showed significant differences in the expression of some genes involved in ribosome pathways,biosynthesis of amino acids, hippo signaling pathway, and pentose phosphate pathway,glycolysis/gluconeogenesis pathway and the TCA cycle. The huge number of transcriptome sequences collected in this study has enhanced the mandarin fish gene resources, and the identified DEGs and related pathway analysis give essential information for understanding biological responses to hypoxia.

关键词： Mandarin fish Transcriptome Hypoxia DEGs

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Highly Efficient Wavelength-Resolved Electrochemiluminescence of Carbon Nitride Films for Ultrasensitive Multiplex MicroRNA Detection

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ANALYTICAL CHEMISTRY 2023年第16期95卷 6620-6628页

作者： Fang, Yanfeng Zhou, Zhixin Hou, Yuhua Wang, Chenchen cao, xuwen Liu, Songqin Shen, Yanfei Zhang, Yuanjian Southeast Univ Sch Chem & Chem Engn Med Sch Jiangsu Engn Lab Smart Carbon Rich Mat & DevicesJ Nanjing 211189 Peoples R China

The development of electrochemiluminescence (ECL) emitters of different colors with high ECL efficiency (0ECL) is appealing yet challenging for ultrasensitive multiplexed bioassays. Herein, we report the synthesis of highly efficient polymeric carbon nitride (CN) films with fine-tuned ECL emission from blue to green (410, 450, 470, and 525 nm) using the precursor crystallization method. More importantly, naked eye observable and significantly enhanced ECL emission was achieved, and the cathodic 0ECL values were ca. 112, 394, 353, and 251 times those of the aqueous Ru(bpy)3Cl2/K2S2O8 reference. Mechanism studies showed that the density of surface-trapped electrons, the associated nonradiative decay pathways, and electron-hole recombination kinetics were crucial factors for the high 0ECL of CN. Based on high 0ECL and different colors of ECL emission, the wavelength-resolved multiplexing ECL biosensor was constructed to simultaneously detect miRNA-21 and miRNA-141 with superior low detection limits of 0.13 fM and 25.17 aM, respectively. This work provides a facile method to synthesize wavelength-resolved ECL emitters based on metal-free CN polymers with high 0ECL for multiplexed bioassays.

关键词： Electrochemiluminescence Biosensor MicroRNA Multiplex Carbon nitride

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Insight into Iron Leaching from an Ascorbate-Oxidase-like Fe-N-C Nanozyme and Oxygen Reduction Selectivity

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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 2023年第27期62卷 e202302463-e202302463页

作者： cao, xuwen Zhu, Caixia Hong, Qing Chen, Xinghua Wang, Kaiyuan Shen, Yanfei Liu, Songqin Zhang, Yuanjian Southeast Univ Sch Chem & Chem Engn Jiangsu Engn Lab Smart Carbon Rich Mat & Device Jiangsu Prov Hitech Key Lab Biomed Res Nanjing 211189 Peoples R China Southeast Univ Med Sch Nanjing 210009 Peoples R China

Ascorbate (H(2)A) is a well-known antioxidant to protect cellular components from free radical damage and has also emerged as a pro-oxidant in cancer therapies. However, such "contradictory" mechanisms underlying H(2)A oxidation are not well understood. Herein, we report Fe leaching during catalytic H(2)A oxidation using an Fe-N-C nanozyme as a ferritin mimic and its influence on the selectivity of the oxygen reduction reaction (ORR). Owing to the heterogeneity, the Fe-N-x sites in Fe-N-C primarily catalyzed H(2)A oxidation and 4 e(-) ORR via an iron-oxo intermediate. Nonetheless, trace O-2(center dot-) produced by marginal N-C sites through 2 e(-) ORR accumulated and attacked Fe-N-x sites, leading to the linear leakage of unstable Fe ions up to 420 ppb when the H(2)A concentration increased to 2 mM. As a result, a substantial fraction (ca. 40 %) of the N-C sites on Fe-N-C were activated, and a new 2+2 e(-) ORR path was finally enabled, along with Fenton-type H(2)A oxidation. Consequently, after Fe ions diffused into the bulk solution, the ORR at the N-C sites stopped at H2O2 production, which was the origin of the pro-oxidant effect of H(2)A.

关键词： Antioxidants Iron Nanozymes Oxygen Reduction Selectivity Pro-Oxidants

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Quantitative evaluation of O2 activation half-reaction for Fe-N-C in oxidase-like activity enhancement

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CATALYSIS SCIENCE & TECHNOLOGY 2021年第22期11卷 7255-7259页

作者： Chen, Xinghua Zhu, Caixia Xu, Yuan Wang, Kaiyuan cao, xuwen Shen, Yanfei Liu, Songqin Zhang, Yuanjian Southeast Univ Sch Chem & Chem Engn Jiangsu Engn Lab Smart Carbon Rich Mat & Device Jiangsu Prov Hitech Key Lab Biomed ResState Key Nanjing 211189 Peoples R China Southeast Univ Med Sch Nanjing 210009 Peoples R China

The oxidase-like activity of high-performance Fe-N-C was enhanced by up to 55% by using a secondary N-containing precursor in pyrolysis. Moreover, the exploration of the O-2 activation half-reaction using electrochemical methods was disclosed to be a practically facile approach to quantitatively evaluate the factors associated with the activity.

关键词： Iron compounds

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Decoupling of the Confused Complex in Oxidation of 3,3′,5,5′-Tetramethylbenzidine for the Reliable Chromogenic Bioassay

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ANALYTICAL CHEMISTRY 2023年第44期95卷 16407-16417页

作者： Zhu, Caixia Yang, Hong cao, xuwen Hong, Qing Xu, Yuan Wang, Kaiyuan Shen, Yanfei Liu, Songqin Zhang, Yuanjian Southeast Univ Sch Chem & Chem Engn Med Sch Jiangsu Engn Lab Smart Carbon Rich Mat & DevicesJ Nanjing Peoples R China

Regulation of the reaction pathways is a perennial theme in the field of chemistry. As a typical chromogenic substrate, 3,3 ',5,5 '-tetramethylbenzidine (TMB) generally undertakes one-electron oxidation, but the product (TMBox1) is essentially a confused complex and is unstable, which significantly hampers the clinic chromogenic bioassays for more than 50 years. Herein, we report that sodium dodecyl sulfate (SDS)-based micelles could drive the direct two-electron oxidation of TMB to the final stable TMBox2. Rather than activation of H2O2 oxidant in the one-electron TMB oxidation by common natural peroxidase, activation of the TMB substrate by SDS micelles decoupled the thermodynamically favorable complex between TMBox2 with unreacted TMB, leading to an unusual direct two-electron oxidation pathway. Mechanism studies demonstrated that the complementary spatial and electrostatic isolation effects, caused by the confined hydrophobic cavities and negatively charged outer surfaces of SDS micelles, were crucial. Further cascading with glucose oxidase, as a proof-of-concept application, allowed glucose to be more reliably measured, even in a broader range of concentrations without any conventional strong acid termination.

关键词： Carbohydrates Micelles Oxidation Oxidation reactions Reaction products

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Cascade nanozymatic network mimicking cells with selective and linear perception of H2O2

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CHEMICAL SCIENCE 2023年第24期14卷 6780-6791页

作者： Zhu, Caixia Zhou, Zhixin Gao, Xuejiao J. Tao, Yanhong cao, xuwen Xu, Yuan Shen, Yanfei Liu, Songqin Zhang, Yuanjian Southeast Univ Sch Chem & Chem Engn Med Sch Jiangsu Engn Lab Smart Carbon Rich Mat & DeviceJi Nanjing Peoples R China Jiangxi Normal Univ Coll Chem & Chem Engn Nanchang 330022 Peoples R China

A single stimulus leading to multiple responses is an essential function of many biological networks, which enable complex life activities. However, it is challenging to duplicate a similar chemical reaction network (CRN) using non-living chemicals, aiming at the disclosure of the origin of life. Herein, we report a nanozyme-based CRN with feedback and feedforward functions for the first time. It demonstrates multiple responses at different modes and intensities upon a single H2O2 stimulus. In the two-electron cascade oxidation of 3,3 ',5,5 '-tetramethylbenzidine (TMB), the endogenous product H2O2 competitively inhibited substrates in the first one-electron oxidation reaction on a single-atom nanozyme (Co-N-CNTs) and strikingly accelerated the second one-electron oxidation reaction under a micellar nanozyme. As a proof-of-concept, we further confined the nanozymatic network to a microfluidic chip as a simplified artificial cell. It exhibited remarkable selectivity and linearity in the perception of H2O2 stimulus against more than 20 interferences in a wide range of concentrations (0.01-100 mM) and offered an instructive platform for studying primordial life-like processes.

关键词： Oxidation

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