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Nitrogen-doped carbon@TiO_(2) double-shelled hollow spheres as an electrochemical sensor for simultaneous determination of dopamine and paracetamol in human serum and saliva

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Journal of Pharmaceutical analysis 2022年第3期12卷 436-445页

作者： Hui Yang Gongxun Cao Yongjun Huang Ye Lin Fengying Zheng Luxiu Lin Fengjiao Liu Shunxing Li College of Chemistry Chemical Engineering and EnvironmentMinnan Normal UniversityZhangzhouFujian363000China fujian Provincial key laboratory of Pollution Monitoring and Control Minnan Normal UniversityZhangzhouFujian363000China Fujian Key Laboratory of Separation and Analysis Science and Technology ZhangzhouFujian363000China

As the most commonly used antipyretic and analgesic drug,paracetamol(PA)coexists with neurotransmitter dopamine(DA)in real biological samples.Their simultaneous determination is extremely important for human health,but they also interfere with each other.In order to improve the conductivity,adsorption affinity,sensitivity,and selectivity of TiO_(2)-based electrochemical sensor,N-doped carbon@-TiO_(2) double-shelled hollow sphere(HeC/N@TiO_(2))is designed and synthesized by simple alcoholic and hydrothermal method,using polystyrene sphere(PS)as a template.Meanwhile,TiO_(2) hollow spheres(H eTiO_(2))or N-doped carbon hollow spheres(HeC/N)are also prepared by the same method.HeC/N@TiO_(2) has good conductivity,charge separation,and the highly enhanced and stable current responses for the detection of PA and DA.The detection limit and linear range are 50.0 nmol/L and 0.3-50 mmol/L for PA,40.0 nmol/L and 0.3e50 mmol/L for DA,respectively,which are better than those of carbon-based sensors.Moreover,this electrochemical sensor,with high selectivity,strong anti-interference,high reliability,and long time durability,can be used for the simultaneous detection of PA and DA in human blood serum and saliva.The high electrochemical performance of HeC/N@TiO_(2) is attributed to the multifunctional combination of different layers,because of good conductivity,absorption and electrons transfer ability from in-situ N-doped carbon and electrocatalytic activity from TiO_(2).

关键词： Electrochemical sensor Simultaneous determination Paracetamol Dopamine

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Insights into the conversion of dissolved organic phosphorus favors algal bloom, arsenate biotransformation and microcystins release of Microcystis aeruginosa

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Journal of Environmental sciences 2023年第3期125卷 205-214页

作者： Xiaoyan Zhang Zhenhong Wang Zhuanxi Luo Yan Chen Xuguang Huang College of Chemistry Chemical Engineering and EnvironmentMinnan Normal UniversityKey Laboratory of Modern Separation and Analysis Science and TechnologyKey Laboratory of Pollution Monitoring and ControlZhangzhou 363000China College of Chemical Engineering Huaqiao UniversityXiamen 361021China

Little information is available on influences of the conversion of dissolved organic phosphorus(DOP) to inorganic phosphorus(IP) on algal growth and subsequent behaviors of arsenate(As(V)) in Microcystis aeruginosa(M. aeruginosa). In this study, the influences factors on the conversion of three typical DOP types including adenosine-5-triphosphate disodium salt(ATP), β-glycerophosphate sodium(βP) and D-glucose-6-phosphate disodium salt(GP)were investigated under different extracellular polymeric secretions(EPS) ratios from M.aeruginosa, and As(V) levels. Thus, algal growth, As(V) biotransformation and microcystins(MCs) release of M. aeruginosa were explored in the different converted DOP conditions compared with IP. Results showed that the three DOP to IP without EPS addition became in favor of algal growth during their conversion. Compared with IP, M. aeruginosa growth was thus facilitated in the three converted DOP conditions, subsequently resulting in potential algal bloom particularly at arsenic(As) contaminated water environment. Additionally, DOP after conversion could inhibit As accumulation in M. aeruginosa, thus intracellular As accumulation was lower in the converted DOP conditions than that in IP condition. As(V) biotransformation and MCs release in M. aeruginosa was impacted by different converted DOP with their different types. Specifically, DMA concentrations in media and As(III) ratios in algal cells were promoted in converted βP condition, indicating that the observed dissolved organic compositions from βP conversion could enhance As(V) reduction in M. aeruginosa and then accelerate DMA release. The obtained findings can provide better understanding of cyanobacteria blooms and As biotransformation in different DOP as the main phosphorus source.

关键词： Organic phosphorus Arsenate Phosphate Methylation Extracellular polymeric secretions

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Hybridization induced ion-barrier effect for the label-free and sensitive electrochemical sensing of Hepatocellular Carcinoma biomarker of miRNA-122

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Chinese Chemical Letters 2021年第7期32卷 2192-2196页

作者： Feng Gao Yaru Chu Yijing Ai Weiqiang Yang Zhenyu Lin Qingxiang Wang College of Chemistry and Environment Fujian Provincial Key Laboratory of Modem Analytical Science and Separation TechnologyMinnan Normal UniversityZhangzhou 363000China Ministry of Education key laboratory for Analytical science of Food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350116China

A label-free and sensitive electrochemical biosensing strategy for a hepatocellular carcinoma biomarker of miRNA-122 has been proposed based on hybridization induced ion-barrier effect on the electroactive sensing interface.First,a bifunctional electroactive electrode with the nanocomposite of Prussian blue(PB)and gold nanoparticles(AuNPs)was prepared through a two-step electrodeposition process.The PB endows the electrode excellent K^(+)-dependent voltammetric signal and the AuNPs act as the matrix for the self-assembly immobilization of the thiolated probe DNA.Upon specific hybridization of probe DNA with the target miRNA-122,the formed double duplex induced the ion-barrier effect,which blocked the diffusion of the K^(+)from the bulk solution to the electrode surface.As a result,the voltammetric signal of the PB on the electrode was surpressed,and thus the target miRNA-122 was monitored.The sensing assay showed that the miRNA-122 could be analyzed in the concentration range from 0.1 fmol/L to 1.0 nmol/L,with a detection limit of 0.021 fmol/L.The practical applicability of the biosensor was also verified by the spiking serum assay.

关键词： Prussian blue Label-free Ion-barrier effect MiRNA-122 Electrochemical behavior

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Predesigned covalent organic framework with sulfur coordination: Anchoring Au nanoparticles for sensitive colorimetric detection of Hg(Ⅱ)

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Chinese Chemical Letters 2024年第5期35卷 392-396页

作者： Guorong Li Yijing Wu Chao Zhong Yixin Yang Zian Lin Ministry of Education key laboratory of Analytical science for Food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350108China

Targeted construction of new covalent organic frameworks(COFs)with specific purposes and rationalities to build colorimetric assay platform for environmental pollutant monitoring have attracted increasing interest.However,it is still challenging due to lack of available coordination sites inside COFs pores and only a slight bonding ability for anchoring metal.In this work,a two-dimensional(2D)COFs(termed as Tz-COF)with high crystallinity,excellent chemical stability,and abundant sulfur coordination in its skeletons was synthesized and used for the confined growth of Au NPs.It was found that the Au NPs showed significant dispersibility for the support of Tz-COF.The proposed Tz-COF@Au NPs possessed outstanding Hg^(2+)-activated peroxidase-like activity benefited from physicochemical properties of gold amalgam and synergistic effect between COFs and Au NPs to oxidize chromogenic substrate.Based on highly efficient activity and distinctive color evolution,the strategy for detecting Hg^(2+)was developed and successfully applied to determine the content of Hg^(2+)in real environmental samples.This work manifests that a potential strategy to establish a colorimetric assay platform for environmental pollutant monitoring based on the targeted manufacturing of novel COFs with specific functions.

关键词： Covalent organic frameworks Thiazole Sulfur coordination Au nanoparticles Hg^(2+)-activated peroxidase-like activity

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Recent Advances in Surface-Assisted Laser Desorption/Ionization Mass Spectrometry and Its Imaging for Small Molecules

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Journal of analysis and Testing 2022年第3期6卷 217-234页

作者： Huan Huang Dan Ouyang Zi-An Lin Ministry of Education key laboratory of Analytical science for Food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350108China

Mass spectrometry imaging(MSI)has provided a new perspective on acquiring spatial information of multiple molecules in various samples.Among the different ionization methods,matrix-assisted laser desorption/ionization(MALDI)has been widely utilized for detecting macromolecules,with difficulty for small molecules(m/zanalysis of small molecules.Selecting an appropriate substrate is a precondition for SALDI-MS and offers the possibility for SALDI-MS imaging(SALDI-MSI).In the last 5 years,different kinds of nanomaterials have been widely explored as substrates including metal/metal oxide-based,carbon-based,silicon-based,metal-organic frameworks-based,covalent organic frameworksbased substrates,with growing interests on composite materials and nanomaterials with homogeneous film structure.This review highlights recent advances of various nanomaterials as SALDI substrates,and their emerging imaging applications in botanic,forensic,metabolic and pathological fields.Finally,the merits and limitations of SALDI-MS are sketched out and some recommendations of this technique and its imaging are proposed.

关键词： Nanomaterials Surface-assisted laser desorption ionization(SALDI) Mass spectrometry imaging(MSI) Small molecules

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Selecting small molecule DNA aptamers with significant conformational changes for constructing transcriptional switches and biosensors

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science China Chemistry 2023年第5期66卷 1529-1536页

作者： Shaobin Guo Jingjing Lin Lujie Lin Wen Xu Yan Guo Zipeng Xu Chunhua Lu Xianai Shi Lanlan Chen Huanghao Yang College of Biological science and Engineering Fuzhou UniversityFuzhou 350108China School of Pharmacy Fujian University of Traditional Chinese MedicineFuzhou 350122China key laboratory for Analytical science of Food Safety and Biology of Ministry of Education Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyState Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou 350108China fujian key laboratory of Medical Instrument and Pharmaceutical technology Fuzhou UniversityFuzhou 350108China

Small molecule aptamers discovered by traditional selection methods usually lack conformational changes upon target binding.This limits the use of aptamers as molecular probes for small molecule detection and regulatory elements of genetic circuits.Here,we report a new method called capture and in vitro transcription-systematic evolution of ligands by exponential enrichment(CIVT-SELEX)to select DNA aptamers that can not only bind to small molecule ligands but also undergo significant conformational changes.Through this method,we select a structure-switching aptamer of uridine-5′-diphosphate(UDP).Taking advantage of its conformational changes,we first construct a UDP-responsive transcriptional switch by inserting the aptamer in a genetic circuit and demonstrate that it can respond to the addition of UDP and regulate the transcription of downstream genes.We also build a UDP aptamer-based biosensor that can be used for active glycosyltransferase screening.We believe this method can provide a universal platform for selecting small molecule aptamers with conformational changes and expand the use of aptamers in small molecule detection and genetic regulation.

关键词： aptamers conformational change CIVT-SELEX small molecule biosensors

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Copper(Ⅱ) ions-immobilized virus-like hollow covalent organic frameworks for highly efficient capture and sensitive analysis of amyloid beta-peptide 1–42 by MALDI-MS

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Chinese Chemical Letters 2022年第12期33卷 5174-5179页

作者： Wende Ma Chao Zhong Juan Lin Zhuling Chen Guorong Li Wei Tong Yijing Wu Lan Zhang Zian Lin Ministry of Education key laboratory of Analytical science for Food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350108China Department of Cardiology Fujian Provincial Governmental HospitalFuzhou 350003China

Amyloid beta-peptide 1-42(Aβ1-42)is one of the biomarkers of Alzheimer's disease,and its selective capture and quantitative detection are important for diagnosis and treatment of Alzheimer's disease.Herein,copper(Ⅱ)ions-immobilized virus-like hollow covalent organic frameworks(V-HCOFs@Cu^(2+))were synthesized by a facile approach.The as-prepared V-HCOFs@Cu^(2+)showed unique morphology,ultra-high specific surface(2552 m^(2)/g),uniform mesoporous structure(3.2 nm),superior chemical stability and abundant binding sites.Based on these excellent properties,the V-HCOFs@Cu^(2+)could be adopted as an ideal enrichment probe for highly efficient capture of Aβ1-42,exhibiting high adsorption capacity(320 mg/g),and fast adsorption equilibration time(3 min).In addition,an attractive approach of the V-HCOFs@Cu^(2+)-based matrix-assisted laser desorption/ionization mass spectrometry(MALDI-MS)was developed for the rapid screening and quantitative analysis of Aβ1-42 in human serum by using C-peptide as an internal standard,which exhibited low limit of detection(LOD,0.2 fmol/μL),and satisfactory recovery.This work provides an alternative solution for enrichment of biomarkers and also offers the potential applications of COFs in clinical analysis.

关键词： Virus-like hollow covalent organic frameworks Metal ion immobilization Amyloidβ-peptide 1–42 Capture Matrix-assisted laser desorption ionization mass spectrometry

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Target-triggered inhibiting oxidase-mimicking activity of platinum nanoparticles for ultrasensitive colorimetric detection of silver ion

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Chinese Chemical Letters 2019年第9期30卷 1659-1662页

作者： Haohua Deng Shaobin He Xiuling Lin Lu Yang Zhen Lin Ruiting Chen Huaping Peng Wei Chen Higher Educational key laboratory for Nano Biomedical technology of fujian Province Department of Pharmaceutical Analysis Fujian Medical University

The development of efficient methods for the detection of hazardous and toxic elements is extremely important for environmental security and public health. In this work, we developed a facile colorimetric assaying system for Ag+ detection in aqueous solution. Chitosan-stabilized platinum nanoparticles(ChPtNPs) were synthesized and severed as an artificial oxidase to catalyze the oxidation of the substrate3,30,5,50-tetramethylbenzidine(TMB) and generate color signal. In the presence of Ag+, due to the strong metallophilic interactions between Ag+ and Pt2+ on the surface of Ch-PtNPs, Ag+ can weaken the affinity to the substrates and inactivate the catalytic activity of Ch-PtNPs, leading to decreased absorbance signal to varying degrees depending on Ag+ amount. Combing the specific binding between Ch-PtNPs and Ag+ with signal amplification procedure based on the Ch-PtNPs-catalyzed TMB oxidation, a sensitive,selective, simple, cost-effective, and rapid detection method for Ag+ can be realized. Ag+ ions in tap and lake waters have been successfully detected. We ensured that the proposed method can be a potential alternative for Ag+ determination in environmental samples.

关键词： Colorimetric detection Oxidase-like activity Platinum nanoparticle Tetramethylbenzidine Silver ion

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Dual inhibition of glycolysis and oxidative phosphorylation by aptamer-based artificial enzyme for synergistic cancer therapy

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Nano Research 2022年第7期15卷 6278-6287页

作者： Xiao Fang Meng Yuan Junduan Dai Qianying Lin Yuhong Lin Wenli Wang Yifan Jiang Haihui Wang Fang Zhao Junye Wu Shumeng Bai Chunhua Lu Huanghao Yang MOE key laboratory for Analytical science of Food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyState Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou 350108China College of Biological science and Engineering Fuzhou UniversityFuzhou 350108China

Dual inhibition of glycolysis and oxidative phosphorylation(OXPHOS)can break the metabolic plasticity of cancer cells to inhibit most energy supply and lead to effective cancer therapy.However,the pharmacokinetic difference among drugs hinders these two inhibitions to realize a uniform temporal and spatial distribution.Herein,we report an aptamer-based artificial enzyme for simultaneous dual inhibition of glycolysis and OXPHOS,which is constructed by arginine aptamer modified carbon-dots-doped graphitic carbon nitride(AptCCN).AptCCN can circularly capture intracellular arginine attribute to the specific binding ability of arginine aptamers to arginine,and further catalyze the oxidation of enriched arginine to nitric oxide(NO)under red light irradiation.In vitro and in vivo experiments showed that arginine depletion and NO stress could inhibit glycolysis and OXPHOS,leading to energy blockage and apoptosis of cancer cells.The presented aptamer-based artificial enzyme strategy provides a new path for cell pathway regulation and synergistic cancer therapy.

关键词： aptamers artificial enzymes photochemistry energy blockage cancer therapy

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Thiophene-based covalent organic frameworks for highly efficient iodine capture

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Chinese Chemical Letters 2023年第1期34卷 550-554页

作者： Xi Yan Yixin Yang Guorong Li Jianhua Zhang Yu He Ran Wang Zian Lin Zongwei Cai Ministry of Education key laboratory of Analytical science for Food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350108China State key laboratory of Environmental and Biological analysis Department of ChemistryHong Kong Baptist UniversityHong KongChina Radiation Environment Supervision Station of fujian Province Fuzhou 350001China

Development of adsorbent materials for highly efficient iodine capture is high demand from the perspective of ecological environment and human health. Herein, the two kinds of thiophene-based covalent organic frameworks(COFs) with different morphologies were synthesized by solvothermal reaction using thieno[3,2-b]thiophene-2,5-dicarbaldehyde(TT) as the aldehyde monomer and tri(4-aminophenyl)benzene(PB) or tris(4-aminophenyl)amine(PA) as the amino monomer(denoted as PB-TT COF and PA-TT COF) and the as-prepared two heteroatoms-rich COFs possessed many excellent properties,including high thermal stability and abundant binding sites. Among them, PB-TT COF exhibited ultra-high iodine uptake up to 5.97 g/g in vapor, surpassing most of adsorbents previously reported, which was ascribed to its high specific surface(1305.3 m2/g). Interestingly, PA-TT COF with low specific surface(48.6m2/g) showed good adsorption ability for iodine in cyclohexane solution with uptake value of 750 mg/g,which was 2.38 times higher than that obtained with PB-TT COF due to its unique sheet-like morphology.Besides, the two COFs possessed good reusability, high selectivity and iodine retention ability. Based on experimental results, the adsorption mechanisms of both COFs were studied, revealing that iodine was captured by the physical-chemical adsorption. Furthermore, the both COFs showed excellent adsorption ability in real radioactive seawater treated safely, demonstrating their great potential in real environment.

关键词： Thiophene-based covalent organic frameworks Iodine Morphology Adsorption mechanisms Radioactive seawater

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