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A core-satellite self-assembled SERS aptasensor containing a“biological-silent region”Raman tag for the accurate and ultrasensitive detection of histamine

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Food Science and Human Wellness 2024年第2期13卷 1029-1039页

作者： Chen Chen Yingfang Zhang Ximo Wang Xuguang Qiao geoffrey i.n.waterhouse Zhixiang Xu Key Laboratory of Food Processing Technology and Quality Control in Shandong Province College of Food Science and EngineeringShandong Agricultural UniversityTai’an 271018China School of Chemical Sciences The University of AucklandAuckland 1142New Zealand

Herein,a novel interference-free surface-enhanced Raman spectroscopy(SERS)strategy based on magnetic nanoparticles(MnPs)and aptamer-driven assemblies was proposed for the ultrasensitive detection of histamine.A core-satellite SERS aptasensor was constructed by combining aptamer-decorated Fe_(3)O_(4)@Au MnPs(as the recognize probe for histamine)and complementary DnA-modified silver nanoparticles carrying 4-mercaptobenzonitrile(4-MBn)(Ag@4-MBn@Ag-c-DnA)as the SERS signal probe for the indirect detection of histamine.Under an applied magnetic field in the absence of histamine,the assembly gave an intense Raman signal at“Raman biological-silent”region due to 4-MBn.in the presence of histamine,the Ag@4-MBn@Ag-c-DnA SERS-tag was released from the Fe_(3)O_(4)@Au MnPs,thus decreasing the SERS signal.Under optimal conditions,an ultra-low limit of detection of 0.65×10^(-3)ng/mL and a linear range 10^(-2)-10^5 ng/mL on the SERS aptasensor were obtained.The histamine content in four food samples were analyzed using the SERS aptasensor,with the results consistent with those determined by high performance liquid chromatography.The present work highlights the merits of indirect strategies for the ultrasensitive and highly selective SERS detection of small biological molecules in complex matrices.

关键词： Surface-enhanced Raman spectroscopy Raman biological-silent region Aptamer Histamine detection Universal SERS-tag

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Covalent organic framework/carbon black/molecularly imprinted polydopamine composites for the selective recognition and electrochemical detection of ciprofloxacin

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Food Science and Human Wellness 2024年

作者： Yufeng Sun Yongfeng Chen Xiaomin Pang geoffrey i.n.waterhouse Xuguang Qiao Zhixiang Xu Key Laboratory of Food Processing Technology and Quality Control in Shandong Province College of Food Science and Engineering Shandong Agricultural University School of Chemical Sciences The University of Auckland

in this work， a novel electrochemical sensor based on covalent organic framework@carbon black@molecularly imprinted polydopamine （COF@CB@MPDA） was developed for selective recognition and determination of ciprofloxacin （CF）. COF@CB@MPDA possessed good water dispersibility and was synthesized by the self-polymerization of dopamine under alkaline conditions in the presence of the COF， CB and CF. The high surface area COF enhanced the adsorption of CF， whilst CB gave the composites high electrical conductivity to improve the sensitivity of the proposed COF@CB@MPDA/GCE sensor. The specific recognition of CF by COF@CB@MPDA involved hydrogen bonding and van der Waals interactions. Under optimized conditions， the sensor showed a good linear relationship with CF concentration over the range 5.0 × 10-7mol/L and 1.0 × 10-4mol/L， with a limit of detection （LOD） of 9.53 × 10-8mol/L. Further， the developed sensor exhibited high selectivity， repeatability and stability for CF detection in milk and milk powders. The method used to fabricate the COF@CB@MPDA/GCE sensor could be easily adapted for the selective recognition and detection of other antibacterial agents and organic pollutants in the environment.

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Bifunctional ZrO@ZiF-90 nanozyme with high phosphohydrolase activity for sensitive electrochemical detection of methyl parathion

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Food Science and Human Wellness 2024年

作者： Xiaomin Pang geoffrey i.n.waterhouse Ruiqiang Wang Xuguang Qiao Yufeng Sun Zhixiang Xu Key Laboratory of Food nutrition and Healthy in Universities of Shandong College of Food Science and Engineering Shandong Agricultural University School of Chemical Sciences the University of Auckland Shandong Cayon Testing Co. Ltd.

in this work， a novel bifunctional zirconium dioxide @ zeolitic imidazolate framework-90 (ZrO2@ZiF-90) nanozyme was successfully developed for the catalytic degradation and electrochemical detection of methyl parathion (MP). The ZrO2@ZiF-90 nanozyme with phosphatase hydrolysis activity can convert MP into p-nitrophenol (p-nP). The addition of ZrO2riched in Lewis acid Zr(iV) sites significantly enhanced the phosphatase hydrolysis activity of ZiF-90. ZrO2@ZiF-90 also displayed satisfactory electrocatalytic performance on account of the high surface area， high porosity and powerful enrichment ability of the ZiF-90 and the excellent ion transfer capacity of ZrO2. A ZrO2@ZiF-90 nanozyme modified glassy carbon electrode (ZrO2@ZiF-90/GCE) was then fabricated to analyze p-nP formed through MP degradation. Under the optimized conditions， the developed sensor displayed satisfactory analytical performance with a low limit of detection of 0.53 μmol L-1and two wide linear ranges (3-10 μmol L-1and 10-200 μmol L-1). ZrO2@ZiF-90 nanozyme accomplished to the degradation and electrochemical detection of MP in river water and spiked fruits. This study identifies a promising new strategy for the design of bifunctional nanozymes for the detection of environmental hazards.

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Facile synthesis of magnetic covalent organic framework nanocomposites for the enrichment and quantification of trace organophosphorus pesticides in fruit juice

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Food Science and Human Wellness 2024年

作者： Quanbin Fu Xin Sun Lu Liu Hailong Jiang geoffrey i.n.waterhouse Shiyun Ai Rusong Zhao School of Chemical Sciences The University of Auckland College of Chemistry and Material Science Shandong Agricultural University Qilu University of Technology (Shandong Academy of Sciences) Shandong Analysis and Test Center Key Laboratory for Applied Technology of Sophisticated Analytical instruments of Shandong Province College of Food Science and Engineering Shandong Agricultural University

Organophosphorus pesticides (OPPs) in foods pose a serious threat to human health， motivating the development of novel analytical methods for their rapid detection and quantification. A magnetic covalent organic framework (M-COF) adsorbent for the magnetic solid-phase extraction (MSPE) of OPPs from foods was reported. M-COF was synthesized by the Schiff base condensation reaction of 1，3，5-tris (4-aminophenyl)benzene and 4，4-biphenyldicarboxaldehyde on the surface of amino-functionalized magnetic nanoparticles. Density–functional theory (DFT) calculations showed that adsorption of OPPs onto the surface of M-COF involved hydrophobic effects， Van der Waals interactions， π–π interactions， halogen-n bonding， and hydrogen bonding. Combined with gas chromatography–mass spectrometry (GC–MS) technology， the MSPE method features low limits of detection for OPPs (0.002–0.015 μg/L)， good reproducibility (1.45%–6.14%)， wide linear detection range (0.01–1 μg/L， R≥ 0.9935)， and satisfactory recoveries (87.3%–110.4%). The method was successfully applied for the trace analysis of OPPs in spiked fruit juices.

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A highly sensitive electrochemical sensing platform based on Zn-CuGaO@CMK-3 signal amplification for simultaneous detection of the sunset yellow and tartrazine in foods

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Food Science and Human Wellness 2024年

作者： Yongfeng Chen Rui Gao Yufeng Sun Ruiqiang Wang geoffrey i.n.waterhouse Xuguang Qiao Zhixiang Xu College of Food Science and Engineering Shandong Agricultural University Shandong Cayon Testing Co. LTD. School of Chemical Sciences The University of Auckland

in this work， a highly sensitive electrochemical sensor based on Zn-doped copper gallium oxide@ordered mesoporous carbon (Zn-CuGaO2@CMK-3) for signal amplification was successfully developed for the simultaneous detection of sunset yellow （SY） and tartrazine （TZ） in foods. Compared with CuGaO2@CMK-3， Zn-CuGaO2@CMK-3 offered enhanced conductivity and catalytic properties owing to the improved carrier density， which was beneficial to the electrooxidation of SY and TZ. Under the optimal testing conditions， the constructed Zn-CuGaO2@CMK-3/GCE sensor offered a wide linear concentration range （0.25 to 100.00 μmol/L） for the detection of both SY and TZ. The limits of detection for SY and TZ were 0.044 μmol/L and 0.059 μmol/L， respectively. Recovery experiments were performed in milk， white vinegar and biscuit samples， yielding satisfactory recoveries （82.70%-114.80%）. Furthermore， the sensor was successfully applied to the determination of the SY and TZ residues in two kinds of carbonated drinks， and the results were nearly consistent with those detected by the high performance liquid chromatography （HPLC） method （P＞0.05）.

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Effective anti-inflammatory phenolic compounds from dandelion:identification and mechanistic insights using UHPLC-ESi-MS/MS,fluorescence quenching and anisotropy,molecular docking and dynamics simulation

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Food Science and Human Wellness 2023年第6期12卷 2184-2194页

作者： Hui Zou Tingting Ben Ping Wu geoffrey i.n.waterhouse Yilun Chen College of Food Science and Engineering Shandong Agricultural UniversityKey Laboratory of Food Processing Technology and Quality Control in Shandong ProvinceTai’an 271018China School of Chemical Sciences University of AucklandAuckland 1142New Zealand

This novel study identifi es the effective anti-inflammatory phenolic compounds in dandelion and provides mechanistic insights into their interactions with receptor proteins(toll-like receptor 4,TLR4;co-receptor myeloid differentiation protein-2,MD-2)using UHPLC-ESi-MS/MS,lipopolysaccharide(LPS)-stimulated THP-1 cell line,fluorescence quenching and anisotropy,molecular docking(single ligand and multi-ligand docking)and molecular dynamics simulation.A 50%aqueous methanol extract had a greater anti-inflammatory effect and higher chicoric acid content,compared with the 100%water and 100%methanol extracts.Chicoric acid,chlorogenic acid,methylophiopogonone A,caffeic acid,gallic acid monohydrate and 4’-O-demethylbroussonin A had relatively high binding energies and contents in all extracts.Chicoric acid competed with chlorogenic acid,4’-O-demethylbroussonin A and quercetin for MD-2.Among dandelion’s phenolics,chicoric acid most effectively hindered TLR4-MD-2 complex formation,with a quenching constant of 0.62×10^(6) L/mol for MD-2 or TLR4 at 320 K,and binding energies of-6.87 and-5.97 kcal/mol,respectively,for MD-2 and TLR4.

关键词： Dandelion extracts Phenolic compounds binding affinity TLR4-MD-2 antagonist Anti-inflammatory agent

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Dual sensitivity of spiropyran-functionalized carbon dots for full color conversions

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Science China Chemistry 2022年第11期65卷 2274-2282页

作者： Lin Ai Huimin Liu Rui Liu Haoqiang Song Ziqi Song Mingjun nie geoffrey i.n.waterhouse Siyu Lu Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450000China College of Chemistry and Chemical Engineering Jishou UniversityJishou 416000China School of Chemical Sciences The University of AucklandAuckland 142New Zealand

Multicolor phosphors that respond rapidly to external stimuli are highly desirable for many applications, including lighting,optical displays and sensors. Herein, spiropyran(SP)-functionalized carbon dots(CDs) were synthesized with a broad-spectrum output that were responsive to both ultraviolet(UV)/visible light and pH. The SP-CDs possessed strong ester linkages between the UV-absorbing/blue-emitting CDs and blue-absorbing/red-emitting surface SP groups, allowing efficient F?rster resonance energy transfer(FRET) between the donor and acceptor. UV irradiation or acid addition cause the SP ring opening to merocyanine(MC) or protonated MCH+forms, respectively, together with the formation of sheet-like aggregates. These processes enhanced the red emissions by the SP groups and attenuated blue emissions from the CDs. These changes were fully reversible under visible light or basic conditions, respectively, allowing dynamic regulation of the fluorescence properties(emission colors from blue to red, photoluminescence(PL) intensity) under photoirradiation on the timescale of minutes. As proof-of concept, we demonstrate that the emission properties of the SP-CDs can be used to construct UV and pH sensing materials as well as light emitting diode(LED) with different colors.

关键词： carbon dots dual-sensitivity full color emission spiropyran F?rster resonance energy transfer

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Disulfide Crosslinking-induced Aggregation:Towards Solid-State Fluorescent Carbon Dots with Vastly Different Emission Colors

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Chinese Journal of Chemistry 2023年第9期41卷 1007-1014页

作者： Rui Fu Haoqiang Song Xingjiang Liu Yongqiang Zhang Guanjun Xiao Bo Zou geoffrey i.n.waterhouse Siyu Lu Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhouHenan 450000China State Key Laboratory of Superhard Materials College of PhysicsJilin UniversityChangchunJilin 130012China School of Chemical Sciences The University of AucklandAuckland 1142New Zealand

Solid-state fluorescent multi-color carbon dots(SFM-CDs),prepared using the same precursor(s)without the need for dispersion in a solid matrix,are highly demanded for a wide range of applications.Herein,we report a microwave-assisted strategy for the prepara-tion of SFM-CDs with blue,yellow and red emissions within 5 min from the same precursors.The as-prepared B-CDs,Y-CDs,and R-CDs possessed bright fluorescence at 425 nm,550 nm,and 640 nm,and photoluminescence quantum yields(PLQYs)of 54.68%,17.93%,and 2.88%,respectively.The structure of SFM-CDs consisted of 5-oxo-3,5-dihydro-2H-thiazolo[3,2-a]pyridine-7-carboxylic acid(TPCA)immobilized on the surface of a carbon core,with the size of the carbon core and degree of disulfide crosslinking between CDs both increasing on going from the B-CDs to the R-CDs,as verified by mechanochromic experiments.The excellent solid-state fluorescence performance of the SFM-CDs allowed their utilization as the fluorescent converter layer in multi-color LEDs and white LEDs with a high color rendering index.

关键词： Solid-state fluorescence Multicolor Cross-linked aggregation Disulfide bond Carbon dots

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Creating burdock polysaccharide-oleanolic acid-ursolic acid nanoparticles to deliver enhanced anti-inflammatory effects:fabrication,structural characterization and property evaluation

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Food Science and Human Wellness 2023年第2期12卷 454-466页

作者： Shanshan Zhu Zhichang Qiu Xuguang Qiao geoffrey i.n.waterhouse Wenqing Zhu Wenting Zhao Qiuxia He Zhenjia Zheng Key Laboratory of Food Processing Technology and Quality Control of Shandong Higher Education institutes College of Food Science and EngineeringShandong Agricultural UniversityTai’an 271018China The School of Chemical Sciences The University of AucklandAuckland 1025New Zealand institute of Agri-food Processing and nutrition Vegetable Research CenterBeijing Academy of Agriculture and Forestry SciencesBeijing 100097China Biology institute Qilu University of Technology(Shandong Academy of Sciences)Jinan 250103China

This study explored the potential of polysaccharides from Actium lappa(ALPs)as natural wall materials for producing ALP-based nanoparticles to deliver poorly water-soluble oleanolic acid(OA)and ursolic acid(UA).Encapsulating OA+UA with ALPs(ALP:OA+UA,50:1;OA:UA,1:1)changed the crystalline nature to a more amorphous state through hydrogen bonding and involving O-H/C-O/O-C-O groups.ALP-OA/UA nanoparticles had a particle size and zeta potential(in water)of 199.1 nm/-7.15 mV,with a narrow unimodal size distribution,and excellent pH,salt solution,temperature and storage stability.Compared with ALPs,ALPOA/UA nanoparticles showed enhanced anti-inflammatory activity(especially at a dose of 100μg/mL)in a CuSO-induced zebrafish inflammation model via down-regulating the nF-κB signalling pathway and gene expression of associated transcription factors and cytokines(TnF-α,iL-1βand iL-8).Therefore,ALP-based nanoparticles are natural and anti-inflammatory carriers for hydrophobic bioactive molecules.

关键词： Encapsulation Structural features Particle size Zeta potential Thermodynamic properties in vivo verification

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Targeted alleviation of ischemic stroke reperfusion via atorvastatin-ferritin Gd-layered double hydroxide

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Bioactive Materials 2023年第2期20卷 126-136页

作者： Li Wang Baorui Zhang Xueting Yang Shuaitian Guo geoffrey i.n.waterhouse Guangrong Song Shanyue Guan Aihua Liu Liang Cheng Shuyun Zhou Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing100190China Beijing neurosurgical institute and Beijing Tiantan Hospital Capital Medical UniversityChina National Clinical Research Center for Neurological DiseasesBeijing100070China institute of Functional nano&Soft Materials(FUnSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China School of Chemical Sciences The University of AucklandAuckland1142New Zealand

in acute ischemic stroke therapy,potent neuroprotective agents are needed that prevent neural injuries caused by reactive oxygen species(ROS)during ischemic reperfusion.Herein,a novel 2D neuroprotective agent(AFGd-LDH)is reported,comprising Gd-containing layered double hydroxide nanosheets(Gd-LDH,as a drug nanocarrier/MRi contrast agent),atorvastatin(ATO,as a neuroprotective drug)and the ferritin heavy subunit(FTH,as a blood brain barrier transport agent).Experiments revealed AFGd-LDH to possess outstanding antioxidant activity,neuroprotective properties,blood‒brain barrier transit properties,and biocompatibility.in vitro studies demonstrated the ROS scavenging efficiency of AFGd‒LDH to be~90%,surpassing CeO_(2)(50%,a ROS scavenger)and edaravone(52%,a clinical neuroprotective drug).ischemia‒reperfusion model studies in mice showed AFGd‒LDH could dramatically decrease apoptosis induced by reperfusion,reducing the infarct area by 67%and lowering the neurological deficit score from 3.2 to 0.9.AFGd-LDH also offered outstanding MRi performance,thus enabling simultaneous imaging and ischemia reperfusion therapy.

关键词： Layered double hydroxide ROS scavenger Atorvastatin ischemic stroke Multimodal imaging

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