Inappropriate use of paracetamol (PA) can induce serious liver injury,and developing accurate PA detecting methods holds great importance in the fields of drug quality control and therapeutic drug monitoring.In this w...Inappropriate use of paracetamol (PA) can induce serious liver injury,and developing accurate PA detecting methods holds great importance in the fields of drug quality control and therapeutic drug monitoring.In this work,a novel electrochemical sensor for detecting PA was successfully fabricated based on iron single atoms distributed on multiwall carbon nanotubes (Fe/MWCNTs)that were prepared through the Lewis acid doping strategy.MWCNTs wrapped by polyaniline-derived N-doped carbon not only provide the anchoring sites for Fe,but also endow the catalyst with high conductivity and mass transfer ability.Theoretical calculation results reveal that atomically dispersed Fe sites hold good catalytic activity toward PA oxidation reaction,because of easier OH absorption at the first step and more facile occurrence of the key transformation from OH*+PA into H2O*+PA_H,during which electrons transferred from PA to catalysts,thereby facilitating the dissociation of N-H bond and the oxidation of PA.The Fe/MWCNTs sensor showed excellent PA detecting performance,delivering a low detection limit of 0.14μM in wide ranges of 0.5-100μM and 100-500μM.Without any pretreatments,the built sensor can directly and accurately detect PA in several complex commercial pharmaceutical formulations and spiked human urine samples with satisfactory recoveries from 96.98% to 107.59%,thereby fully demonstrating its practical application prospects.展开更多
The development and fabrication of cucurbit[7]uril(Q[7])-based host‒vip supramolecular polymers remain challenging due to the limited cavity size of Q[7].Herein,we designed and synthesized three thiophene-pyridinium...The development and fabrication of cucurbit[7]uril(Q[7])-based host‒vip supramolecular polymers remain challenging due to the limited cavity size of Q[7].Herein,we designed and synthesized three thiophene-pyridinium vips and investigated their binding interactions with Q[7].NMR,ESI-MS spectroscopy,and DFT calculations revealed that Q[7]can encapsulate one or two thiophene groups of the vips to form supramolecular complexes,including discrete inclusion complexes and supramolecular polymers.Importantly,all supramolecular complexes demonstrated reversible photochromism in the solid state,which is attributed to viologen radical generation,as confirmed by UV-vis-NIR,ESR,and DFT studies.Due to the aggregation caused quenching(ACQ)effect induced by the intermolecularπ⋯πstacking interaction of thiophene groups within the Q[7]cavity,the Q[7]-based supramolecular polymers remained fluorescence-silent,whereas the discrete inclusion complexes showed enhanced fluorescence compared to their thiophene-pyridinium vips.The dual photochromic and fluorescence properties of the Q[7]-based supramolecular complexes render them suitable for applications in erasable inkless printing,multi-level anti-counterfeiting,and advanced information encryption.This study provides a strategy for constructing dual-functional supramolecular polymers using Q[7]-based host‒vip interactions.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22375005 and 22474003)the Provincial University Research and Innovation Team(No.2022AH010023)+4 种基金the Natural Science Foundation of Anhui Province(No.2408085JX004)the Natural Science Research Project of Anhui Province Education Department(No.2022AH050323)the Postdoctoral Start-up Funding of Anhui University of Technology(No.DT2300001444)the Doctoral Start-up Funding of Anhui University of Technology(No.DT2300000981)Anhui Medical University Research Fund Project(No.2022xkj130)
文摘Inappropriate use of paracetamol (PA) can induce serious liver injury,and developing accurate PA detecting methods holds great importance in the fields of drug quality control and therapeutic drug monitoring.In this work,a novel electrochemical sensor for detecting PA was successfully fabricated based on iron single atoms distributed on multiwall carbon nanotubes (Fe/MWCNTs)that were prepared through the Lewis acid doping strategy.MWCNTs wrapped by polyaniline-derived N-doped carbon not only provide the anchoring sites for Fe,but also endow the catalyst with high conductivity and mass transfer ability.Theoretical calculation results reveal that atomically dispersed Fe sites hold good catalytic activity toward PA oxidation reaction,because of easier OH absorption at the first step and more facile occurrence of the key transformation from OH*+PA into H2O*+PA_H,during which electrons transferred from PA to catalysts,thereby facilitating the dissociation of N-H bond and the oxidation of PA.The Fe/MWCNTs sensor showed excellent PA detecting performance,delivering a low detection limit of 0.14μM in wide ranges of 0.5-100μM and 100-500μM.Without any pretreatments,the built sensor can directly and accurately detect PA in several complex commercial pharmaceutical formulations and spiked human urine samples with satisfactory recoveries from 96.98% to 107.59%,thereby fully demonstrating its practical application prospects.
基金supported by the National Natural Science Foundation of China(Grant No.21371004)the Natural Science Foundation of Anhui Province(2408055UM003,1808085MB43)the Natural Science Research Project of Anhui Province Education Department(2023AH040150).
文摘The development and fabrication of cucurbit[7]uril(Q[7])-based host‒vip supramolecular polymers remain challenging due to the limited cavity size of Q[7].Herein,we designed and synthesized three thiophene-pyridinium vips and investigated their binding interactions with Q[7].NMR,ESI-MS spectroscopy,and DFT calculations revealed that Q[7]can encapsulate one or two thiophene groups of the vips to form supramolecular complexes,including discrete inclusion complexes and supramolecular polymers.Importantly,all supramolecular complexes demonstrated reversible photochromism in the solid state,which is attributed to viologen radical generation,as confirmed by UV-vis-NIR,ESR,and DFT studies.Due to the aggregation caused quenching(ACQ)effect induced by the intermolecularπ⋯πstacking interaction of thiophene groups within the Q[7]cavity,the Q[7]-based supramolecular polymers remained fluorescence-silent,whereas the discrete inclusion complexes showed enhanced fluorescence compared to their thiophene-pyridinium vips.The dual photochromic and fluorescence properties of the Q[7]-based supramolecular complexes render them suitable for applications in erasable inkless printing,multi-level anti-counterfeiting,and advanced information encryption.This study provides a strategy for constructing dual-functional supramolecular polymers using Q[7]-based host‒vip interactions.
