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Distinct roles of pH and organic ligands in the dissolution of goethite by cysteine

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Journal of Environmental Sciences 2022年第3期34卷 260-268页

作者： Ji Li Chenlu Shi wenbin zeng Yaru Wang Zebin Hong Yibing Ma Liping Fang Faculty of Material Sciences and Chemistry China University of GeosciencesWuhan 430074China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management Institute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangzhou 520650China Macao Environmental Research Institute Macao University of Science and TechnologyTaipa 999078MachaoChina

Electron shuttles such cysteine play an important role in Fe cycle and its availability in soils,while the roles of pH and organic ligands in this process are poorly ***,the reductive dissolution process of goethite by cysteine were explored in the presence of organic *** results showed that cysteine exhibited a strong reactivity towards goethite-a typical iron minerals in paddy soils with a rate constant ranging from 0.01 to0.1 hr^(-1).However,a large portion of Fe(Ⅱ) appeared to be "structural species" retained on the *** decline of pH was favorable to generate more Fe(Ⅱ) ions and enhancing tendency of Fe(Ⅱ) release to *** decline of generation of Fe(Ⅱ) by increasing pH was likely to be caused by a lower redox potential and the nature of cysteine pH-dependent adsorption towards ***,the co-existence of oxalate and citrate ligands also enhanced the rate constant of Fe(Ⅱ) release from 0.09 to 0.15 hr-1;nevertheless,they negligibly affected the overall generation of Fe(Ⅱ) in opposition to the pH *** spectroscopic evidence demonstrated that two molecules of cysteine could form disulfide bonds(S-S) to generate cystine through oxidative dehydration,and subsequently,inducing electron transfer from cysteine to the structural Fe(Ⅲ) on goethite;meanwhile,those organic ligands act as Fe(Ⅱ) "strippers".The findings of this work provide new insights into the understanding of the different roles of pH and organic ligands on the generation and release of Fe induced by electron shuttles in soils.

关键词： Electron transfer Reductive dissolution Iron cycling Organic ligands

Rational Design of Organelle-Targeted Fluorescent Probes:Insights from Artificial Intelligence

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Research 2023年第3期2023卷 769-779页

作者： Jie Dong Jie Qian Kunqian Yu Shuai Huang Xiang Cheng Fei Chen Hualiang Jiang wenbin zeng Xiangya School of Pharmaceutical Sciences Central South UniversityChangsha 410083P.R.China National Engineering Research Center of Rice and Byproduct Deep Processing School of Food Science and EngineeringCentral South University of Forestry and TechnologyChangsha 410004P.R.China State Key Laboratory of Drug Research Drug Discovery and Design CenterShanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203P.R.China

Monitoring the physiological changes of organelles is essential for understanding the local biological information of cells and for improving the diagnosis and therapy of ***,fluorescent probes are considered as the most powerful tools for imaging and have been widely applied in biomedical ***,the expected targeting effects of these probes are often inconsistent with the real *** design of fluorescent probes mainly depends on the empirical knowledge of researchers,which was inhibited by limited chemical space and low ***,we proposed a novel multilevel framework for the prediction of organelle-targeted fluorescent probes by employing advanced artificial intelligence *** this way,not only the targeting mechanism could be interpreted beyond intuitions but also a quick evaluation method could be established for the rational ***,the targeting and imaging powers of the optimized and synthesized probes based on this methodology were verified by quantitative calculation and experiments.

关键词： inhibited diagnosis Probe

Intelligent design and construction of novel APN-based theranostic probe driven by advanced computational methods

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Chinese Chemical Letters 2024年第2期35卷 352-357页

作者： Yingli Zhu Jie Qian Kunqian Yu Jing Hou Yeshuo Ma Fei Chen Jie Dong wenbin zeng Xiangya School of Pharmaceutical Sciences Central South UniversityChangsha 410083China National Engineering Research Center of Rice and Byproduct Deep Processing School of Food Science and EngineeringCentral South University of Forestry and TechnologyChangsha 410004China State Key Laboratory of Drug Research Drug Discovery and Design CenterShanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China Department of Geriatrics Third Xiangya HospitalCentral South UniversityChangsha 410013China

Multifunctional molecules with both optical signal and pharmacological activity play an important role in drug development,disease diagnosis,and basic theoretical *** N(APN),as a representative tumor biomarker with anti-tumor potential,still lacks a high-precision theranostic probe specifically targeting *** this study,a novel quaternity design strategy for APN theranostic probe was *** proposed strategy utilizes advanced machine learning and molecular dynamics simulations,and cleverly employs the strategy of conformation-induced fluorescence recovery to achieve multi-objective optimization and integration of functional *** this strategy,a unique“Off-On”theranostic probe,ABTP-DPTB,was ingeniously constructed to light up APN through fluorescence restoration,relying on conformation-induced effects and solvent *** from the common diagnostic probes,the intelligent design with non-substrated linkage makes ABTP-DPTB for long-term in-situ *** fabricated probe was used for detecting and inhibiting APN in various environments,with a better in vitro inhibitory than golden-standard drug bestatin.

关键词： Theranostic probe Artificial intelligence Conformational restriction Fluorescence restoration Design strategy

An ESIPT-based NIR-fluorescent probe for exosome labeling and in situ imaging

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Chinese Chemical Letters 2023年第11期34卷 220-224页

作者： Jipeng Ding Runsha Xiao Anyao Bi Guanyang Chen Nengwei Zhang Zihua Chen Xueping Feng wenbin zeng Xiangya School of Pharmaceutical Sciences Central South UniversityChangsha 410013China Department of Gastrointestinal Surgery Hunan Key Laboratory of Precision Diagnosis and Treatment of Gastrointestinal TumorXiangya HospitalCentral South UniversityChangsha 410013China Institute of Medical Sciences Xiangya HospitalCentral South UniversityChangsha 410013China Peking University Ninth School of Clinical Medicine(Beijing Shijitan Hospital Capital Medical University)Beijing 100038China

Exosomes play significant roles in physiological and tumorigenic processes and it is desirable to visualize and track the ***,a novel amphiphilic fluorescent probe HBT-Exo based on excited-state intramolecular proton transfer(ESIPT)mechanism is reported for *** ESIPT characteristics were confirmed by both theory calculation and experimental observation,which enable the probe to show a large Stokes shift as well as near-infrared(NIR)keto-form ***-Exo displayed excellent biocompatibility and remarkable efficiency for exosome-labeling in gastric cancer ***,the labeled exosomes were successfully applied for the real-time in situ imaging in mouse models.

关键词： Exosome Fluorescent probe Excited state intramolecular proton transfer Gastric cancer Bioimaging

Monitoring intracellular pH fluctuation with an excited-state intramolecular proton transfer-based ratiometric fluorescent sensor

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Chinese Chemical Letters 2021年第10期32卷 3057-3060页

作者： Bin Feng Yingli Zhu Jiaxin Wu Xueyan Huang Rong Song Liu Huang Xueping Feng wenbin zeng Xiangya School of Pharmaceutical Sciences Central South UniversityChangsha 410013China The Molecular Imaging Research Center Central South UniversityChangsha 410013China Hunan Key Laboratory of Diagnostic and Therapeutic Drug Research for Chronic Diseases Central South UniversityChangsha 410013China Xiangya Hospital Central South UniversityChangsha 410013China

Intracellular pH is a key parameter related to various biological and pathological *** this study,a ratiometric pH fluorescent sensor ABTT was developed harnessing the amino-type excited-state intramolecular proton transfer(ESIPT) *** on whether the ESIPT proceeds normally or not,ABTT exhibited the yellow fluorescence in acidic media,or cyan fluorescence in basic *** to the variation,ABTT behaved as a promising sensor which possessed fast and reversible response to pH change without interference from the biological substances,and exported a steady ratiometric signal(I_(478)/I_(546)).Moreover,due to the ESIPT effect,large Stokes shift and high quantum yield were also exhibited in ***,ABTT was applied for monitoring the pH changes in living cells and visualizing the pH fluctuations under oxidative stress *** results elucidated great potential of ABTT in understanding pH-dependent physiological and pathological processes.

关键词： Excited-state intramolecular proton transfer Intracellular pH Sulfonamide Ratiometric sensor Fluorescent imaging

Au nanoparticles based ultra-fast “Turn-On” fluorescent sensor for detection of biothiols and its application in living cell imaging

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Chinese Chemical Letters 2020年第5期31卷 1083-1086页

作者： Hailiang Zhang Pengfei Xu Xintong Zhang Xiaozheng Cao Wenxiu Han Meihui Liu Xiaohui Liu wenbin zeng Xiangya School of Pharmaceutical Sciences Central South UniversityChangsha 410006China Institute of Clinical Pharmacy and Pharmacology Jining First People's HospitalJining Medical UniversityJining 272000China Yidu Central Hospital of Weifang Weifang 261000China

Au or other metal nanostructures have the ability to strongly quench the fluorescence of *** feature has made AuNP-conjugates attractive for the construction of platforms for various bioanalytes to overcome the limitations of small molecule fluorophores(poor solubility,long reaction time).In this paper,an ultrafast"Turn-On"fluo rescent sensor for biothiols was *** sensor is based on the fluorescent resonance energy transfer(FRET)effect between the fluorophore(PN)and AuNPs,which effectively quenches the fluorescence of the *** the presence of thiols,PN is displaced and released from AuNP surfaces,and thus,the fluorescence is rapidly *** sensor features appreciable water solubility and ultrafast response time(a few seconds for Cys).In addition,it exhibits high selectivity and a detection limit as low as 12 nmol/L for ***,the sensor presents good biocompatibility and has been successfully applied for imaging biothiols in living cells.

关键词： Gold nanoparticle FRET Biothiols Sensor Fluorescent imaging

Tactfully revealing the working mechanisms on a tetraarylimidazole derivative:AIE characteristic,ESIPT process and ICT effect integrating in one molecule

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Chinese Chemical Letters 2023年第8期34卷 392-397页

作者： Min Liu Shibo Zhong Bin Feng Yueming Ren Xiaohui Liu Shuaige Bai Fei Chen Shao Liu wenbin zeng Xiangya School of Pharmaceutical Sciences Central South UniversityChangsha 410013China Department of Pharmacy Xiangya HospitalCentral South UniversityChangsha 410008China National Clinical Research Center for Geriatric Disorders Xiangya HospitalCentral South UniversityChangsha 410008China

Recently,a novel tetraarylimidazole derivative 2-(benzo[d]thiazol-2-yl)-4-(4,5-bis(4-methoxyphenyl)-1-phenyl-1H-imidazol-2-yl)-phenol(be called MHBT herein)was architectured by our research group showing the fascinating synergy of aggregation-induced emission(AIE)characteristic,excited-state intramolecular proton transfer(ESIPT)mechanism and intramolecular charge transfer(ICT)***,a detailed and reasonable interpretation of its mechanisms both in theory is urgently ***,to unveil the working mechanism meticulously,herein,we tactfully applied density functional theory(DFT)and time-dependent density functional theory(TD-DFT)methods to illuminate the underlying mechanisms in different solvent *** optimizing the structures,the geometric parameters of hydrogen bonds(HBs),the infrared(IR)vibrational spectrum,the reduced density gradient(RDG)isosurfaces were calculated in detail,vividly explaining how the enhancement of HBs behaved as the driving force to proceed ESIPT ***,the frontier molecular orbitals(FMOs)combined with the potential energy curves(PECs)were conducted to interpretate the role and character of ICT and ESIPT in molecule ***,the PECs of MHBT for dihedral angles in different organic solvents were calculated to compare the dominant torsion degree,rationalizing the AIE phenomenon from the view of the restriction of intramolecular rotation *** work may well underpin the understanding of the interaction between different mechanisms in fluorescent dyes and thereby provide meaningful guideline for the design and construction of ideal molecules.

关键词： Tetraarylimidazole derivative Aggregation-induced emission Excited-state intramolecular proton transfer Intramolecular charge transfer Density functional theory Time-dependent density functional theory

Harnessing antimicrobial peptide-coupled photosensitizer to combat drug-resistant biofilm infections through enhanced photodynamic therapy

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Acta Pharmaceutica Sinica B 2024年第4期14卷 1759-1771页

作者： Duoyang Fan Xiaohui Liu Yueming Ren Ziheng Luo Yanbing Li Jie Dong Seraphine VWegner Fei Chen wenbin zeng Xiangya School of Pharmaceutical Sciences Central South UniversityChangsha 410013China Hunan Key Laboratory of Diagnostic and Therapeutic Drug Research for Chronic Diseases Central South UniversityChangsha 410013China Sir William Dunn School of Pathology University of OxfordOxford OX13REUK Xiangya Hospital of Central South University Changsha 410013China Institute of Physiological Chemistry and Pathobiochemistry University of MünsterMünster 48149Germany

Bacterial biofilm-associated infection was one of the most serious threats to human health. However, effective drugs for drug-resistance bacteria or biofilms remain rarely reported. Here, we propose an innovative strategy to develop a multifunctional antimicrobial agent with broad-spectrum antibacterial activity by coupling photosensitizers (PSs) with antimicrobial peptides (AMPs). This strategy capitalizes on the ability of PSs to generate reactive oxygen species (ROS) and the membrane-targeting property of AMPs (KRWWKWIRW, a peptide screened by an artificial neural network), synergistically enhancing the antimicrobial activity. In addition, unlike conventional aggregation-caused quenching (ACQ) photosensitizers, aggregation-induced emission (AIE) PSs show stronger fluorescence emission in the aggregated state to help visualize the antibacterial mechanism. In vitro antibacterial experiments demonstrated the excellent killing effects of the developed agent against both Gram-positive (G^(+)) and Gram-negative (G^(–)) bacteria. The bacterial-aggregations induced ability enhanced the photoactivatable antibacterial activity against G^(–) bacteria. Notably, it exhibited a significant effect on destroying MRSA biofilms. Moreover, it also showed remarkable efficacy in treating wound infections in mice in vivo. This multifunctional antimicrobial agent holds significant potential in addressing the challenges posed by bacterial biofilm-associated infections and drug-resistant bacteria.

关键词： Photodynamic therapy Antimicrobial peptides Multidrug-resistant bacteria Aggregation-induced emission Anti-biofilm

The exquisite integration of ESIPT, PET and AIE for constructing fluorescent probe for Hg(II) detection and poisoning

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Chinese Chemical Letters 2022年第4期33卷 1861-1864页

作者： Xiang Cheng Shuai Huang Qian Lei Fei Chen Fan Zheng Shibo Zhong Xueyan Huang Bin Feng Xueping Feng wenbin zeng Xiangya School of Pharmaceutical Sciences Central South UniversityChangsha 410013China The Molecular Imaging Research Center Central South UniversityChangsha 410013China Hunan Key Laboratory of Diagnostic and Therapeutic Drug Research for Chronic Diseases Central South UniversityChangsha 410013China Xiangya Hospital Central South UniversityChangsha 410013China

Excessive mercury ions(Hg^(2+)) in the environment can accumulate in human body along with the food chain to cause serious physiological *** fluorescence probes were considered as convenient tool with great potential for Hg^(2+) *** existing probes suffer from aggregation-induced quenching(ACQ) effects and insufficient ***,a novel type of fluorophore was developed by combining the aggregation-induced emission(AIE) and excited state intramolecular proton transfer(ESIPT) ***,a phenyl thioformate group with photoinduced electron transfer(PET)effect was connected to give an efficient "turn-on" probe(HTM),which exhibited good selectivity toward Hg^(2+),short response time(30 min),coupled with extremely low detection limit(LOD=1.68 nmol/L).In addition,HTM was used successfully in real samples,cells and drug evaluation,underlying the superiority of HTM to detect Hg^(2+) in practical applications.

关键词： Aggregation-induced emission Excited state intramolecular proton transfer Photoinduced electron transfer Mercury ions Fluorescent imaging