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Enhancing the deep-red/near-infrared fluorescence of higher rylene diimides via the chalcogen-annulation strategy

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Science China Chemistry 2024年第4期67卷 1324-1333页

作者： Kai Chen Xiao Chen Ke Hu Yilun Zhao Yujian Liu Guogang Liu Jinquan Chen Wei Jiang Zhigang Shuai da-hui qu Zhaohui Wang Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Key Laboratory of Organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China State Key Laboratory of Precision Spectroscopy East China Normal University500 Dongchuan RoadShanghai 200241China

Deep-red/near-infrared fluorescence is highly suitable for bioimaging owing to its ability to deeply penetrate tissues,organs,and live animals.However,developing organic fluorophores with high deep-red/near-infrared fluorescence quantum yield(Φ_(FL))and fluorescent brightness remain a significant challenge owing to the energy gap law.Herein,we developed a straightforward and effective chalcogen-annulation strategy by introducing O,S and Se into the bay region of TDI and QDI fluorophores,realizing the increase ofΦFLand fluorescent brightness up to 10 times.To our best knowledge,this study potentially stands as the pioneering instance showcasing the anti-heavy-atom effect of chalcogens,and the absoluteΦFL(93%)and fluorescent brightness(128,200 cm^(-1)mol^(-1)L)of Se-TDI is among top deep-red/near-infrared organic fluorophores currently available.The femtosecond transient absorption(fs-TA)measurements show the absence of obvious changes of the excited state lifetime after the introduction of chalcogens in TDI and QDI fluorophores,indicating that intersystem crossing(ISC)can be neglected in TDI and QDI fluorophores.Theoretical calculations further reveal the chalcogen-annulation strategy increase the radiative rates and reduce the reorganization energy of several accepting modes at the ground state in TDI fluorophores,leading to the suppression of internal conversion(IC)processes.Our chalcogen-annulation strategy,which effectively increases the Φ_(FL)and restricts the IC processes,while remaining unaffected by the heavy-atom effect,offers novel insights and theoretical support for the design and synthesis of deep-red/near-infrared organic fluorophores with high Φ_(FL)and fluorescent brightness.

关键词： π-extended rylene diimides chalcogen-annulation strategy deep-red/near-infrared fluorescence

Electrically Driven Nonresonant Single Molecular Switches

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CCS Chemistry 2024年第2期6卷 465-472页

作者： Rui Wang Ajun Tang Zhi Li Yunpeng Li dahui qu Hongxiang Li Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237

Electrical switching of a single-molecule junction provides a practical module to perform sophisticated operations in electronic devices.However,designing an all-electrically-driven molecular switch is a great challenge.Here,we experimentally and theoretically investigated the charge transport characteristics of isoindigo(ISO)-molecules at the single-molecule level using the scanning tunneling microscope break junction technique.We find that the single-molecule junctions of ISO-molecules display bias voltage-driven switching characteristics.These switches are realtime,reversible,and nondestructive under low-bias voltages.Experimental results show that the mechanism of the switch is not the transition from nonresonant charge transport to resonant charge transport,but it is the shift of the frontier orbital energy levels of ISO-molecules and the change of the interfacial electronic coupling with bias voltage.Our results will advance the design of high-performance bias voltage-driven molecular switches.

关键词： single-molecule junction isoindigo molecular switch bias voltage nonresonant charge transport molecular electronics

Digitalizing river aquatic ecosystems

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Journal of Environmental Sciences 2024年第3期137卷 677-680页

作者： Yaohui Bai hui Lin Chenchen Wang Qiaojuan Wang Jiuhui qu Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China School of Environmental and Municipal Engineering Tianjin Chengjian UniversityTianjin 300384China Center for Water and Ecology Tsinghua UniversityBeijing 100084China

Traditional river health assessment relies on limited water quality indices and representative organism activity,but does not comprehensively obtain biotic and abiotic information of the ecosystem.Here,we propose a new approach to evaluate the ecological and health risks of river aquatic ecosystems.First,detailed physicochemical and biological characterization of a river ecosystem can be obtained through pollutant determination(especially emerging pollutants)and DNA/RNA sequencing.Second,supervised machine learning can be applied to perform classification analysis of characterization data and ascertain river ecosystem ecology and health.Our proposed methodology transforms river ecosystem health assessment and can be applied in river management.

关键词： Digitalizing River ecosystem health Emerging pollutants High throughput sequencing Machine learning

Detection of Novel BEST1 Variations in Autosomal Recessive Bestrophinopathy Using Third-generation Sequencing

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Current Medical Science 2024年第2期44卷 419-425页

作者： Jia-xun LI Ling-rui MENG Bao-ke HOU Xiao-lu HAO da-jiang WANG Ling-hui qu Zhao-hui LI Lei ZHANG Xin JIN Department of Senior Ophthalmology the Third Medical Center of PLA General HospitalBeijing 100853China Department of Ophthalmology the 74th Army Group HospitalGuangzhou 510318China

Objective:Autosomal recessive bestrophinopathy(ARB),a retinal degenerative disease,is characterized by central visual loss,yellowish multifocal diffuse subretinal deposits,and a dramatic decrease in the light peak on electrooculogram.The potential pathogenic mechanism involves mutations in the BEST1 gene,which encodes Ca2+-activated Cl−channels in the retinal pigment epithelium(RPE),resulting in degeneration of RPE and photoreceptor.In this study,the complete clinical characteristics of two Chinese ARB families were summarized.Methods:Pacific Biosciences(PacBio)single-molecule real-time(SMRT)sequencing was performed on the probands to screen for disease-causing gene mutations,and Sanger sequencing was applied to validate variants in the patients and their family members.Results:Two novel mutations,c.202T>C(chr11:61722628,p.Y68H)and c.867+97G>A,in the BEST1 gene were identified in the two Chinese ARB families.The novel missense mutation BEST1 c.202T>C(p.Y68H)resulted in the substitution of tyrosine with histidine in the N-terminal region of transmembrane domain 2 of bestrophin-1.Another novel variant,BEST1 c.867+97G>A(chr11:61725867),located in intron 7,might be considered a regulatory variant that changes allele-specific binding affinity based on motifs of important transcriptional regulators.Conclusion:Our findings represent the first use of third-generation sequencing(TGS)to identify novel BEST1 mutations in patients with ARB,indicating that TGS can be a more accurate and efficient tool for identifying mutations in specific genes.The novel variants identified further broaden the mutation spectrum of BEST1 in the Chinese population.

关键词： autosomal recessive bestrophinopathy BEST1 gene third-generation sequencing mutation

Cucurbit[8]uril-mediated multi-color fluorescence system for time-dependent information encryption

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Science China Chemistry 2023年第4期66卷 1111-1119页

作者： Biyan Lin Qian Wang Zhen Qi Hanren Xu da-hui qu Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterInstitute of Fine ChemicalsFrontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

Programming microscopic assembly mode to control macroscopic property is an attractive research objective.In particular,controlling molecular assembly to control fluorescence is of considerable interest for developing smart fluorescent materials.Herein,a color-tunable supramolecular emissive system was developed based on cucurbit[8]uril mediated host-guest assembly.Chemical designing for the molecular structures with minimized change resulted in different assembly modes and hence generating distinctive fluorescence,including green,yellow and orange with the addition of cucurbit[n]uril.Taking advantage of this feature,the advanced information encryption material(4D code)with multiple encryption levels and time-dependent encryption feature was developed.Such a code was dynamic on time scale,generating a series of 3D codes with time.The encrypted information only can be recognized by integrating time-coursed codes.This work provides a new insight for designing intelligent fluorescent materials for information encryption with high level of security.

关键词： host-guest systems fluorescence multi-color emission information encryption cucurbituril

Visualizing Aβdeposits in live young AD model mice with a simple red/near-infrared-fluorescent AIEgen

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Science China Chemistry 2022年第2期65卷 339-352页

作者： Yipu Wang Dong Mei Xinyi Zhang da-hui qu Ju Mei Key Laboratory for Advanced Materials Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryJoint International Research Laboratory for Precision Chemistry and Molecular EngineeringInstitute of Fine ChemicalsSchool of Chemistry&Molecular EngineeringEast China University of Science&TechnologyShanghai 200237China Clinical Research Center Beijing Children’s HospitalCapital Medical UniversityNational Center for Children’s HealthBeijing 100045China

Precise and early detection ofβ-amyloid(Aβ)deposits in situ and in real time is pivotal to the diagnosis and early intervention of Alzheimer’s disease(AD).Optical imaging stands out to be a promising technique for such a task;however,it still remains a big challenge,due to the lack of high-performance imaging contrast agent.Restricted by poor blood-brain barrier(BBB)penetrability,short-wavelength excitation and emission,as well as the aggregation-caused quenching effect,the widely used goldstandard probes cannot be used for early in-vivo imaging of Aβdeposits.Herein,we integrate the Aβdeposits-favored geometry,amphiphilic and zwitterionic molecular structure,extended D-π-A electronic structure,and 3 D conformation into one molecule,facilely establishing a simple and economic imaging contrast agent that enjoys high specificity and affinity to Aβdeposits,good BBB penetrability,bright red/near-infrared fluorescence,low interference from autofluorescence,aggregation-induced emission(AIE)feature,high signal-to-noise ratio(SNR),and high contrast.In-vitro,ex-vivo,and in-vivo experiments with different strains of mice indicate that AIE-CNPy-AD holds the universality to Aβdeposits identification.Noteworthily,AIE-CNPy-AD is even able to precisely trace the small and sparsely-distributed Aβdeposits in AD model mice as young as 4-month-old APP/PS1 mice,the youngest having Aβdeposits.Moreover,the present probe could clearly reveal the increase and enlargement of Aβdeposits as the mice grow.Therefore,AIE-CNPy-AD might be an ideal alternative for early AD diagnosis and highly reliable monitoring of AD progression.

关键词： Aβdeposits AIE Alzheimer’s disease(AD) red/NIR fluorescence in-vivo imaging diagnosis

Machine learning-based radiomics score improves prognostic prediction accuracy of stage II/III gastric cancer: A multi-cohort study

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World Journal of Gastrointestinal Surgery 2024年第2期16卷 345-356页

作者： Ying-Hao Xiang Huan Mou Bo qu hui-Rong Sun Department of General Surgery Lichuan People's HospitalEnshi 445400Hubei ProvinceChina

BACKGROUND Although accurately evaluating the overall survival(OS)of gastric cancer patients remains difficult,radiomics is considered an important option for studying pro-gnosis.AIM To develop a robust and unbiased biomarker for predicting OS using machine learning and computed tomography(CT)image radiomics.METHODS This study included 181 stage II/III gastric cancer patients,141 from Lichuan People's Hospital,and 40 from the Cancer Imaging Archive(TCIA).Primary tumors in the preoperative unenhanced CT images were outlined as regions of interest(ROI),and approximately 1700 radiomics features were extracted from each ROI.The skeletal muscle index(SMI)and skeletal muscle density(SMD)were measured using CT images from the lower margin of the third lumbar vertebra.Using the least absolute shrinkage and selection operator regression with 5-fold cross-validation,36 radiomics features were identified as important predictors,and the OS-associated CT image radiomics score(OACRS)was cal-culated for each patient using these important predictors.RESULTS Patients with a high OACRS had a poorer prognosis than those with a low OACRS score(P<0.05)and those in the TCIA cohort.Univariate and multivariate analyses revealed that OACRS was a risk factor[RR=3.023(1.896-4.365),P<0.001]independent of SMI,SMD,and pathological features.Moreover,OACRS outperformed SMI and SMD and could improve OS prediction(P<0.05).CONCLUSION A novel biomarker based on machine learning and radiomics was developed that exhibited exceptional OS discrimination potential.

关键词： Radiomics Machine learning Gastric cancer Skeletal muscle density Skeletal muscle index

Robust and dynamic underwater adhesives enabled by catechol-functionalized poly(disulfides) network

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National Science Review 2023年第2期10卷 174-182页

作者： Chen-Yu Shi dan-dan He Qi Zhang Fei Tong Zhao-Tao Shi He Tian da-hui qu Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Chemistry and Molecular Engineering East China University of Science and Technology

Developing molecular approaches to the creation of robust and water-resistant adhesive materials promotes a fundamental understanding of interfacial adhesion mechanisms as well as future applications of biomedical adhesive materials.Here,we present a simple and robust strategy that combines natural thioctic acid and mussel-inspired iron-catechol complexes to enable ultra-strong adhesive materials that can be used underwater and simultaneously exhibit unprecedentedly high adhesion strength on diverse surfaces.Our experimental results show that the robust crosslinking interaction of the iron-catechol complexes,as well as high-density hydrogen bonding,are responsible for the ultra-high interfacial adhesion strength.The embedding effect of the hydrophobic solvent-free network of poly(disulfides) further enhances the water-resistance.The dynamic covalent poly(disulfides) network also makes the resulting materials re configurable,thus enabling reusability via repeated heating and cooling.This molecule-engineering strategy offers a general and versatile solution to the design and construction of dynamic supramolecular adhesive materials.

关键词： adhesives supramolecular materials dynamic polymers non-covalent crosslink iron-catechol complexes

Evaluating serum CXCL12,sCD22,Lp-PLA2 levels and ratios as biomarkers for diagnosis of Alzheimer's disease

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World Journal of Psychiatry 2024年第3期14卷 380-387页

作者： Zeng-Ling Liu Fei-Fei Hua Lei qu Na Yan hui-Fang Zhang Department of Neurology Dongying People's HospitalDongying 257000Shandong ProvinceChina

BACKGROUND Grasping the underlying mechanisms of Alzheimer's disease(AD)is still a work in progress,and existing diagnostic techniques encounter various obstacles.Therefore,the discovery of dependable biomarkers is essential for early detection,tracking the disease's advancement,and steering treatment strategies.AIM To explore the diagnostic potential of serum CXCL12,sCD22,Lp-PLA2,and their ratios in AD,aiming to enhance early detection and inform targeted treatment strategies.METHODS The study was conducted in Dongying people's Hospital from January 2021 to December 2022.Participants included 60 AD patients(AD group)and 60 healthy people(control group).Using a prospective case-control design,the levels of CXCL12,sCD22 and Lp-PLA2 and their ratios were detected by enzyme-linked immunosorbent assay kit in the diagnosis of AD.The differences between the two groups were analyzed by statistical methods,and the corresponding ratio was constructed to improve the specificity and sensitivity of diagnosis.RESULTS Serum CXCL12 levels were higher in the AD group(47.2±8.5 ng/mL)than the control group(32.8±5.7 ng/mL,P<0.001),while sCD22 levels were lower(14.3±2.1 ng/mL vs 18.9±3.4 ng/mL,P<0.01).Lp-PLA2 levels were also higher in the AD group(112.5±20.6 ng/mL vs 89.7±15.2 ng/mL,P<0.05).Significant differences were noted in CXCL12/sCD22(3.3 vs 1.7,P<0.001)and Lp-PLA-2/sCD22 ratios(8.0 vs 5.2,P<0.05)between the groups.Receiver operating characteristic analysis confirmed high sensitivity and specificity of these markers and their ratios in distinguishing AD,with area under the curves ranging from CONCLUSION Serum CXCL12 and Lp-PLA2 levels were significantly increased,while sCD22 were significantly decreased,as well as increases in the ratios of CXCL12/sCD22 and Lp-PLA2/sCD22,are closely related to the onset of AD.These biomarkers and their ratios can be used as potential diagnostic indicators for AD,providing an important clinical reference for early intervention and treatment.

关键词： Alzheimer's disease Biomarkers CXCL12 sCD22 Lp-PLA2