Mercury ion(Hg^(2+)),as one of the most toxic heavy metal ions,accumulates easily in the environment,which can generate potential hazards to the ecosystem and human health.To effectively detect and remove Hg^(2+),we f...Mercury ion(Hg^(2+)),as one of the most toxic heavy metal ions,accumulates easily in the environment,which can generate potential hazards to the ecosystem and human health.To effectively detect and remove Hg^(2+),we fabricated four types of carbon dots(CDs)using carboxymethyl nanocellulose as a carbon source doped with different elements using a hydrothermal method.All the CDs exhibited a strong fluorescence emission,excitation-dependent emission and possessed good water dispersibility.Moreover,the four fluorescent CDs were used for Hg^(2+)recognition in aqueous solution,where the CDs-N exhibited better sensitivity and selectivity for Hg^(2+)detection,with a low limit of detection of 8.29×10^(-6)mol/L.It was determined that the fluorescence quenching could be ascribed to a photoinduced charge-transfer processes between Hg^(2+)and the CDs.In addition,the CDs-N were used as a smart invisible ink for anticounterfeiting,information encryption and decryption.Furthermore,the CDs-N were immersed into a cellulose(CMC)-based hydrogel network to prepare fluorescent hydrogels capable of simultaneously detecting and adsorbing Hg^(2+).We anticipate that this research will open possibilities for a green method to synthesize fluorescent CDs for metal ion detection and fluorescent ink production.展开更多
Fluorescent probes have emerged as indispensable chemical tools to the field of chemical biology and medicine.The ability to detect intracellular species and monitor physiological processes has not only advanced our k...Fluorescent probes have emerged as indispensable chemical tools to the field of chemical biology and medicine.The ability to detect intracellular species and monitor physiological processes has not only advanced our knowledge in biology but has provided new approaches towards disease diagnosis.In this review,we detail the design criteria and strategies for some recently reported fluorescent probes that can detect a wide range of biologically important species in cells and in vivo.In doing so,we highlight the importance of each biological species and their role in biological systems and for disease progression.We then discuss the current problems and challenges of existing technologies and provide our perspective on the future directions of the research area.Overall,we hope this review will provide inspiration for researchers and prove as useful guide for the development of the next generation of fluorescent probes.展开更多
A simple dual analyte fluorescein-based probe(PF3-Glc)was synthesised containingβ-glucosidase(β-glc)and hydrogen peroxide(H2O2)trigger units.The presence ofβ-glc,resulted in fragmentation of the parent molecule rel...A simple dual analyte fluorescein-based probe(PF3-Glc)was synthesised containingβ-glucosidase(β-glc)and hydrogen peroxide(H2O2)trigger units.The presence ofβ-glc,resulted in fragmentation of the parent molecule releasing glucose and the slightly fluorescent mono-boronate fluorescein(PF3).Subsequently,in the presence of glucose oxidase(GOx),the released glucose was catalytically converted to D-glucono-δ-lactone,which produced H2O2 as a by-product.The GOx-produced H2O2,resulted in classic H2O2-mediated boronate oxidation and the release of the highly emissive fluorophore,fluorescein.This unique cascade reaction lead to an 80-fold increase in fluorescence intensity.展开更多
A boronic acid-based anthracene fluorescent probe was functionalised with an acrylamide unit to incorporate into a hydrogel system for monosaccharide detection.In solution,the fluorescent probe displayed a strong fluo...A boronic acid-based anthracene fluorescent probe was functionalised with an acrylamide unit to incorporate into a hydrogel system for monosaccharide detection.In solution,the fluorescent probe displayed a strong fluorescence turn-on response upon exposure to fructose,and an expected trend in apparent binding constants,as judged by a fluorescence response where D-fructose>D-galactose>D-mannose>D-glucose.The hydrogel incorporating the boronic acid monomer demonstrated the ability to detect monosaccharides by fluorescence with the same overall trend as the monomer in solution with the addition of D-fructose resulting in a 10-fold enhancement(≤0.25 mol/L).展开更多
A glucose-sensitive polymer,poly(N-isopropylacrylamide-co-2-acrylamidophenylboronic acid)(P(NIPAM-co-2-AAPBA)),was synthesized by reversible addition fragmentation chain transfer(RAFT)copolymerization.Addition of gluc...A glucose-sensitive polymer,poly(N-isopropylacrylamide-co-2-acrylamidophenylboronic acid)(P(NIPAM-co-2-AAPBA)),was synthesized by reversible addition fragmentation chain transfer(RAFT)copolymerization.Addition of glucose results in reduced solubility and hence increased turbidity,rather than the normal increase in solubility(decreased turbidity)observed for other PBA-based glucose-sensitive polymers.The novel glucose-sensitive behavior is explained by a new mechanism,in which glucose acts as an additive and depresses the lower critical solution temperature(LCST)of the polymer,instead of increasing solubility by increasing the degree of ionization of the PBA groups.Experimental and theoretic analysis for the influence of glucose on the thermal behavior of P(NIPAM-co-2-AAPBA)reveals that glucose depresses the LCST of P(NIPAM-co-2-AAPBA)copolymers in a two-stage manner,a fast decrease at low glucose concentrations followed by a slow decrease at high glucose concentrations.For low glucose concentrations,the binding of glucose with PBA groups on the polymer chain increases the number of glucose molecules proximal to the polymer which influences the thermal behavior of the polymer,causing a rapid decrease in LCST.Importantly,the transition occurs at a glucose concentration equal to the reciprocal of the binding constant between PBA and glucose,thus providing a novel method to determine the binding constant.Other saccharides,including mannose,galactose and fructose,also depress the LCST of P(NIPAM-co-2-AAPBA)copolymer in the same way.展开更多
Currently,the development of selective fluorescent probes toward targeted enzymes is still a great challenge,due to the existence of numerous isoenzymes that share similar catalytic capacity.Herein,a double-filtering ...Currently,the development of selective fluorescent probes toward targeted enzymes is still a great challenge,due to the existence of numerous isoenzymes that share similar catalytic capacity.Herein,a double-filtering strategy was established to effectively develop isoenzyme-specific fluorescent probe(s)for cytochrome P450(CYP)which are key enzymes involving in metabolism of endogenous substances and drugs.In the first-stage of our filtering approach,near-infrared(NIR)fluorophores with alkoxyl group were prepared for the screening of CYP-activated fluorescent substrates using a CYPs-dependent incubation system.In the second stage of our filtering approach,these candidates were further screened using reverse protein-ligand docking to effectively determine CYP isoenzyme-specific probe(s).Using our double-filtering approach,probes S9 and S10 were successfully developed for the real-time and selective detection of CYP2C9 and CYP2J2,respectively,to facilitate high-throughput screening and assessment of CYP2C9-mediated clinical drug interaction risks and CYP2J2-associated disease diagnosis.These observations suggest that our strategy could be used to develop the isoform-specific probes for CYPs.展开更多
Due to their simplicity in preparation,sensitivity and selectivity,fluorescent probes have become the analytical tool of choice in a wide range of research and industrial fields,facilitating the rapid detection of che...Due to their simplicity in preparation,sensitivity and selectivity,fluorescent probes have become the analytical tool of choice in a wide range of research and industrial fields,facilitating the rapid detection of chemical substances of interest as well as the study of important physiological and pathological processes at the cellular level.In addition,many long-wavelength fluorescent probes developed have also proven applicable for in vivo biomedical applications including fluorescenceguided disease diagnosis and theranostics(e.g.,fluorogenic prodrugs).Impressive progresses have been made in the development of sensing agents and materials for the detection of ions,organic small molecules,and biomacromolecules including enzymes,DNAs/RNAs,lipids,and carbohydrates that play crucial roles in biological and disease-relevant events.Here,we highlight examples of fluorescent probes and functional materials for biological applications selected from the special issues“Fluorescent Probes”and“Molecular Sensors and Logic Gates”recently published in this journal,offering insights into the future development of powerful fluorescence-based chemical tools for basic biological studies and clinical translation.展开更多
Triazolopyridines are an important kind of fused-ring compounds.A HOCl-promoted triazolopyridine formation strategy is reported here for the first time in which hypochlorous acid(HOCl)mildly and efficiently promotes t...Triazolopyridines are an important kind of fused-ring compounds.A HOCl-promoted triazolopyridine formation strategy is reported here for the first time in which hypochlorous acid(HOCl)mildly and efficiently promotes the formation of 1,2,4-triazolo[4,3-a]pyridines NT1-NT6 from various 2-pyridylhydrazones N1-N6.N6,a rhodol-pyridylhydrazone hybrid,was developed into a fluorescent probe for the selective detection of HOCl,and successfully applied to probe endogenous HOCl in living cells and zebrafish in situ and in real time.The present intramolecular cyclization reaction is selective and atom-economical,thereby not only providing an important approach for the convenient synthesis of triazolopyridines,but also offering a general strategy for sensitive,selective and biocompatible detection of endogenous HOCl in complex biosystems.展开更多
We describe the synthesis and evaluation of an azulene-based chemodosimeter for nitrite.The probe was found to undergo two distinct color changes upon introduction of aqueous nitrite ion.A near-instant formation of a ...We describe the synthesis and evaluation of an azulene-based chemodosimeter for nitrite.The probe was found to undergo two distinct color changes upon introduction of aqueous nitrite ion.A near-instant formation of a grey color provides a qualitative indication of the presence of nitrite,followed by the formation of a deep-yellow/orange color,the endpoint from which quantitative data can be derived.The azulene probe exhibits 1:1 stoichiometry of reaction with nitrite in water,and is selective for nitrite over other anions.The azulene probe was applied to determine nitrite content in cured meat,and compared with the British Standard testing procedure(Griess test).The value obtained from the azulene-based probe agreed closely with the standard test.Our procedure only requires the preparation of one standard solution,instead of the three required for the standard Griess test.展开更多
Fluorescent probes are intelligently designed molecules that transform the act of binding/reacting with a target analyte into an optical signal[1,2].Their high sensitivity and specificity coupled with high spatial and...Fluorescent probes are intelligently designed molecules that transform the act of binding/reacting with a target analyte into an optical signal[1,2].Their high sensitivity and specificity coupled with high spatial and temporal resolution offers a non-invasive approach to observe a specific analyte within complex biological environments in real time with high precision[3].These"molecular tools"have the capability to interrogate the role of specific biomarkers that are associated with a particular disease state or can be used to improve our understanding of the role or certain species in a biological pathway[4,5].展开更多
This issue of Frontiers of Chemical Science and Engineering highlights recent progress toward fluorescent probes that was originally conceived to coincide with 7th Conference on Molecular Sensors and Molecular Logic G...This issue of Frontiers of Chemical Science and Engineering highlights recent progress toward fluorescent probes that was originally conceived to coincide with 7th Conference on Molecular Sensors and Molecular Logic Gates(MSMLG 2020)to celebrate the career of Seiji Shinkai and hosted by Anthony Czarnik at the University of Nevada in Reno.Sadly,that meeting was cancelled due to the pandemic associated with COVID-19.However,this collection of research and review papers will now serve as an introduction to MSMLG 2022 which will be in Dublin,Ireland on 7–10 June 2022,where Thorfinnur Gunnlaugsson will be the local host.The collection of papers contained in this special issue covers in vitro and in vivo applications and illustrates the potential for practical sensing and imaging of disease-related species.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52370110 and 21607044)supported by the Fundamental Research Funds for the Central Universities(No.2023MS146)the Open Research Fund of the School of Chemistry and Chemical Engineering,Henan Normal University for support(Nos.2020ZD01 and 2021YB07)。
文摘Mercury ion(Hg^(2+)),as one of the most toxic heavy metal ions,accumulates easily in the environment,which can generate potential hazards to the ecosystem and human health.To effectively detect and remove Hg^(2+),we fabricated four types of carbon dots(CDs)using carboxymethyl nanocellulose as a carbon source doped with different elements using a hydrothermal method.All the CDs exhibited a strong fluorescence emission,excitation-dependent emission and possessed good water dispersibility.Moreover,the four fluorescent CDs were used for Hg^(2+)recognition in aqueous solution,where the CDs-N exhibited better sensitivity and selectivity for Hg^(2+)detection,with a low limit of detection of 8.29×10^(-6)mol/L.It was determined that the fluorescence quenching could be ascribed to a photoinduced charge-transfer processes between Hg^(2+)and the CDs.In addition,the CDs-N were used as a smart invisible ink for anticounterfeiting,information encryption and decryption.Furthermore,the CDs-N were immersed into a cellulose(CMC)-based hydrogel network to prepare fluorescent hydrogels capable of simultaneously detecting and adsorbing Hg^(2+).We anticipate that this research will open possibilities for a green method to synthesize fluorescent CDs for metal ion detection and fluorescent ink production.
基金the National Natural Science Foundation of China(21788102,91853201)the Shanghai Municipal Science and Technology Major Project(2018SHZDZX03)+9 种基金the International Cooperation Program of Shanghai Science and Technology Committee(17520750100)the Projects from the Shanghai Science and Techonology Commission(19441905000)the Fundamental Research Funds for the Central Universities(222201717003)the Programme of Introducing Talents of Discipline to Universities(B16017)for financial supportthe National Natural Science Foundation of China(22107028)National Postdoctoral Program for Innovative Talents(BX20190115)Shanghai Post-doctoral Excellence Program(2019044)China Postdoctoral Science Foundation(2020M681206)for financial supportthe Project funded by China Postdoctoral Science Foundation(2020M681196)the Royal Society for a Wolfson Research Merit Award and the Open Research Fund of the School of Chemistry and Chemical Engineering,Henan Normal University for support(2020ZD01)。
文摘Fluorescent probes have emerged as indispensable chemical tools to the field of chemical biology and medicine.The ability to detect intracellular species and monitor physiological processes has not only advanced our knowledge in biology but has provided new approaches towards disease diagnosis.In this review,we detail the design criteria and strategies for some recently reported fluorescent probes that can detect a wide range of biologically important species in cells and in vivo.In doing so,we highlight the importance of each biological species and their role in biological systems and for disease progression.We then discuss the current problems and challenges of existing technologies and provide our perspective on the future directions of the research area.Overall,we hope this review will provide inspiration for researchers and prove as useful guide for the development of the next generation of fluorescent probes.
基金the EPSRC and the University of Bath for funding.
文摘A simple dual analyte fluorescein-based probe(PF3-Glc)was synthesised containingβ-glucosidase(β-glc)and hydrogen peroxide(H2O2)trigger units.The presence ofβ-glc,resulted in fragmentation of the parent molecule releasing glucose and the slightly fluorescent mono-boronate fluorescein(PF3).Subsequently,in the presence of glucose oxidase(GOx),the released glucose was catalytically converted to D-glucono-δ-lactone,which produced H2O2 as a by-product.The GOx-produced H2O2,resulted in classic H2O2-mediated boronate oxidation and the release of the highly emissive fluorophore,fluorescein.This unique cascade reaction lead to an 80-fold increase in fluorescence intensity.
基金grateful for the support of the EPSRC and DTI(DT/F00267X/1)the Leverhulme Trust for support(F00094BC)the JDRF(2-SRA-2016-267-A-N)for support.
文摘A boronic acid-based anthracene fluorescent probe was functionalised with an acrylamide unit to incorporate into a hydrogel system for monosaccharide detection.In solution,the fluorescent probe displayed a strong fluorescence turn-on response upon exposure to fructose,and an expected trend in apparent binding constants,as judged by a fluorescence response where D-fructose>D-galactose>D-mannose>D-glucose.The hydrogel incorporating the boronic acid monomer demonstrated the ability to detect monosaccharides by fluorescence with the same overall trend as the monomer in solution with the addition of D-fructose resulting in a 10-fold enhancement(≤0.25 mol/L).
基金supported by the National Natural Science Foundation of China(51625302,51873091)the National Key Research and Development Program of China(2017YFC1103501).
文摘A glucose-sensitive polymer,poly(N-isopropylacrylamide-co-2-acrylamidophenylboronic acid)(P(NIPAM-co-2-AAPBA)),was synthesized by reversible addition fragmentation chain transfer(RAFT)copolymerization.Addition of glucose results in reduced solubility and hence increased turbidity,rather than the normal increase in solubility(decreased turbidity)observed for other PBA-based glucose-sensitive polymers.The novel glucose-sensitive behavior is explained by a new mechanism,in which glucose acts as an additive and depresses the lower critical solution temperature(LCST)of the polymer,instead of increasing solubility by increasing the degree of ionization of the PBA groups.Experimental and theoretic analysis for the influence of glucose on the thermal behavior of P(NIPAM-co-2-AAPBA)reveals that glucose depresses the LCST of P(NIPAM-co-2-AAPBA)copolymers in a two-stage manner,a fast decrease at low glucose concentrations followed by a slow decrease at high glucose concentrations.For low glucose concentrations,the binding of glucose with PBA groups on the polymer chain increases the number of glucose molecules proximal to the polymer which influences the thermal behavior of the polymer,causing a rapid decrease in LCST.Importantly,the transition occurs at a glucose concentration equal to the reciprocal of the binding constant between PBA and glucose,thus providing a novel method to determine the binding constant.Other saccharides,including mannose,galactose and fructose,also depress the LCST of P(NIPAM-co-2-AAPBA)copolymer in the same way.
基金The authors thank the National Natural Science Foundation of China(81930112,82174228 and 82004211)National Key R&D program of China(2018YFC1705900)+3 种基金Distinguished Professor of Liaoning Province(XLYC2002008,China)“1+X”program for Clinical Competency enhancement-Interdisciplinary Innovation Project of Second Hospital of Dalian Medical University,Dalian Science and Technology Leading Talents Project(2019RD15,China)High-level Talents of Dalian(2020RQ066 and 2020RQ076,China)the Open Research Fund of the School of Chemistry and Chemical Engineering,and Henan Normal University for support(2020ZD01 and 2021YB07,China)for financial support.T.D.J.wishes to thank the Royal Society for a Wolfson Research Merit Award.
文摘Currently,the development of selective fluorescent probes toward targeted enzymes is still a great challenge,due to the existence of numerous isoenzymes that share similar catalytic capacity.Herein,a double-filtering strategy was established to effectively develop isoenzyme-specific fluorescent probe(s)for cytochrome P450(CYP)which are key enzymes involving in metabolism of endogenous substances and drugs.In the first-stage of our filtering approach,near-infrared(NIR)fluorophores with alkoxyl group were prepared for the screening of CYP-activated fluorescent substrates using a CYPs-dependent incubation system.In the second stage of our filtering approach,these candidates were further screened using reverse protein-ligand docking to effectively determine CYP isoenzyme-specific probe(s).Using our double-filtering approach,probes S9 and S10 were successfully developed for the real-time and selective detection of CYP2C9 and CYP2J2,respectively,to facilitate high-throughput screening and assessment of CYP2C9-mediated clinical drug interaction risks and CYP2J2-associated disease diagnosis.These observations suggest that our strategy could be used to develop the isoform-specific probes for CYPs.
基金the National Natural Science Foundation of China(Grant Nos.21907030 and 22108077)the International Cooperation Program of Shanghai Science and Technology Committee(Grant No.19410712600)+4 种基金De-Tai Shi would like to thank the Natural Science Foundation of Jiangxi(Grant No.20161BAB213067)the Scientific Research Fund of Jiangxi Provincial Education Department(Grant No.GJJ170807)Tony D.James wishes to thank the Royal Society for a Wolfson Research Merit Awardthe Open Research Fund of the School of ChemistryChemical Engineering,Henan Normal University for support(Grant No.2020ZD01).
文摘Due to their simplicity in preparation,sensitivity and selectivity,fluorescent probes have become the analytical tool of choice in a wide range of research and industrial fields,facilitating the rapid detection of chemical substances of interest as well as the study of important physiological and pathological processes at the cellular level.In addition,many long-wavelength fluorescent probes developed have also proven applicable for in vivo biomedical applications including fluorescenceguided disease diagnosis and theranostics(e.g.,fluorogenic prodrugs).Impressive progresses have been made in the development of sensing agents and materials for the detection of ions,organic small molecules,and biomacromolecules including enzymes,DNAs/RNAs,lipids,and carbohydrates that play crucial roles in biological and disease-relevant events.Here,we highlight examples of fluorescent probes and functional materials for biological applications selected from the special issues“Fluorescent Probes”and“Molecular Sensors and Logic Gates”recently published in this journal,offering insights into the future development of powerful fluorescence-based chemical tools for basic biological studies and clinical translation.
基金the National Natural Science Foundation of China(Nos.21977082,21472148 and 21807088)Open Funding Project of the State Key Laboratory of Bioreactor Engineering(No.2018OPEN12)+2 种基金Special Foundation of the Education Committee of Shaanxi Province(No.18JK0702)Technology Plan Project of Xi’an(Nos.201805040YD18CG24 and GXYD18.1)Academic Backbone of Northwest University Outstanding Youth Support Program。
文摘Triazolopyridines are an important kind of fused-ring compounds.A HOCl-promoted triazolopyridine formation strategy is reported here for the first time in which hypochlorous acid(HOCl)mildly and efficiently promotes the formation of 1,2,4-triazolo[4,3-a]pyridines NT1-NT6 from various 2-pyridylhydrazones N1-N6.N6,a rhodol-pyridylhydrazone hybrid,was developed into a fluorescent probe for the selective detection of HOCl,and successfully applied to probe endogenous HOCl in living cells and zebrafish in situ and in real time.The present intramolecular cyclization reaction is selective and atom-economical,thereby not only providing an important approach for the convenient synthesis of triazolopyridines,but also offering a general strategy for sensitive,selective and biocompatible detection of endogenous HOCl in complex biosystems.
基金grateful Ph.D.funding to C.M.L.-A.from the EU Horizon 2020 research and innovation programme under grant agreement H2020-MSCA-CO-FUND,#665992The Centre for Sustainable Chemical Technologies is supported by EPSRC under grant EP/L016354/1EPSRC for DTP Ph.D. funding to L.C.M.
文摘We describe the synthesis and evaluation of an azulene-based chemodosimeter for nitrite.The probe was found to undergo two distinct color changes upon introduction of aqueous nitrite ion.A near-instant formation of a grey color provides a qualitative indication of the presence of nitrite,followed by the formation of a deep-yellow/orange color,the endpoint from which quantitative data can be derived.The azulene probe exhibits 1:1 stoichiometry of reaction with nitrite in water,and is selective for nitrite over other anions.The azulene probe was applied to determine nitrite content in cured meat,and compared with the British Standard testing procedure(Griess test).The value obtained from the azulene-based probe agreed closely with the standard test.Our procedure only requires the preparation of one standard solution,instead of the three required for the standard Griess test.
文摘Fluorescent probes are intelligently designed molecules that transform the act of binding/reacting with a target analyte into an optical signal[1,2].Their high sensitivity and specificity coupled with high spatial and temporal resolution offers a non-invasive approach to observe a specific analyte within complex biological environments in real time with high precision[3].These"molecular tools"have the capability to interrogate the role of specific biomarkers that are associated with a particular disease state or can be used to improve our understanding of the role or certain species in a biological pathway[4,5].
文摘This issue of Frontiers of Chemical Science and Engineering highlights recent progress toward fluorescent probes that was originally conceived to coincide with 7th Conference on Molecular Sensors and Molecular Logic Gates(MSMLG 2020)to celebrate the career of Seiji Shinkai and hosted by Anthony Czarnik at the University of Nevada in Reno.Sadly,that meeting was cancelled due to the pandemic associated with COVID-19.However,this collection of research and review papers will now serve as an introduction to MSMLG 2022 which will be in Dublin,Ireland on 7–10 June 2022,where Thorfinnur Gunnlaugsson will be the local host.The collection of papers contained in this special issue covers in vitro and in vivo applications and illustrates the potential for practical sensing and imaging of disease-related species.
