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Chinese Chemical Letters 2024年第5期35卷 392-396页

作者： Guorong Li Yijing Wu Chao Zhong Yixin Yang Zian Lin Ministry of Education Key laboratory of Analytical Science for food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350108China

Targeted construction of new covalent organic frameworks(COFs)with specific purposes and rationalities to build colorimetric assay platform for environmental pollutant monitoring have attracted increasing ***,it is still challenging due to lack of available coordination sites inside COFs pores and only a slight bonding ability for anchoring *** this work,a two-dimensional(2D)COFs(termed as Tz-COF)with high crystallinity,excellent chemical stability,and abundant sulfur coordination in its skeletons was synthesized and used for the confined growth of Au *** was found that the Au NPs showed significant dispersibility for the support of *** proposed Tz-COF@Au NPs possessed outstanding Hg^(2+)-activated peroxidase-like activity benefited from physicochemical properties of gold amalgam and synergistic effect between COFs and Au NPs to oxidize chromogenic *** on highly efficient activity and distinctive color evolution,the strategy for detecting Hg^(2+)was developed and successfully applied to determine the content of Hg^(2+)in real environmental *** work manifests that a potential strategy to establish a colorimetric assay platform for environmental pollutant monitoring based on the targeted manufacturing of novel COFs with specific functions.

关键词： Covalent organic frameworks Thiazole Sulfur coordination Au nanoparticles Hg^(2+)-activated peroxidase-like activity

Geometric and defects engineering collaboration for enhanced cascade enzymatic nanoreactors

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Nano Research 2024年第4期17卷 2451-2461页

作者： Zhichao Yu Ruijin Zeng Hexiang Gong Yuan Gao Shuyun Chen Yunsen Wang Dianping Tang Key laboratory for Analytical Science of food Safety and Biology(MOE&Fujian Province) Department of ChemistryFuzhou UniversityFuzhou 350108China

Highly evolved multi-enzyme cascade catalytic reactions in organisms facilitate rapid transfer of substrates and efficient conversion of intermediates in the catalytic unit,thus rationalizing their efficient *** this study,pore-ordered mesoporous single-atom(Fe)nitrogen-doped carbon nanoreactors(Mp-Fe-CN)were designed,in which a reasonable pore size was designed as a natural enzyme trap coupled to a simulated enzyme center.A polarity-mediated strategy was developed to obtain atomically dispersed nanoporous substrates,with the finding that polarity-guided engineering of the nitrogen-ligand environment and vacancy cluster defects clearly affects nanoporous activity,accompanied by appreciable mesoporous pore size *** active center and distal N atom coordination of Fe-N_(4) affect the catalytic process of the nanozyme exposed by density functional theory(DFT),determining the contribution of hybridized orbitals to electron transfer and the decisive step.A cascade nanoreactor-based domain-limited sarcosine oxidase developed for non-invasive monitoring of sarcosine levels in urine for evaluation of potential prostate carcinogenesis as a proof of *** on the design of surface mesoporous channels of nanocatalytic units,a bridge was built for the interaction between nanozymes and natural enzymes to achieve cascade nanocatalysis of natural enzymatic products.

关键词： nanozyme single-atom catalyst bioreactor cascade catalysis non-Invasive sensing

Thiol-mediated transportation pathway:an approach for improving tumor penetration of nanomedicines in vivo

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Science China chemistry 2024年第1期67卷 383-389页

作者： Junjie Zhang Weican Sun Xing Wang Senyan Chen Jingying Li Huanghao Yang New Cornerstone Science laboratory Key Laboratory for Analytical Science of Food Safety and Biology(Ministry of Education)College of ChemistryFuzhou UniversityFuzhou 350116China Department of chemistry and College of Biological Science and Engineering Fuzhou UniversityFuzhou 350116China

Abnormal tumor microenvironment imposes barriers to tumor penetration of nanomedicine,which remains a major challenge for effective ***,we present disulfide-based nanoparticles that actively penetrate deep tumors in vivo through a thiol-mediated transportation *** achieve active tumor accumulation in vivo,disulfide-based nanoparticles are modified with folic acid units(FA-DBNPs).It is gratifying that FA-DBNPs still enter cells via the thiol-mediated pathway,which facilitates transcellular transportation and tumor penetration both in vitro and in ***,FA-DBNPs exhibit GSH concentration-dependent depolymerization characterization,indicating that the GSH level in tumor tissues regulates the penetration depth of *** from these advantages,FA-DBNPs showed potent anti-tumor activity in mouse models,leading to the significant regression of *** current study lays a foundation that thiol-mediated transportation is a promising approach in nanomedicine design for solid tumor therapy.

关键词： deep penetration thiol-mediated pathway transcellular transportation solid tumor

Effect of inorganic arsenic in paddy soil on the migration and transformation of selenium species in rice plants

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Journal of Environmental Sciences 2024年第9期143卷 35-46页

作者： Ganga Raj Pokhrel Kaiteng Wang Kaiyang Ying Yongchen Wu Ze Wang Xi Zhu Can Qu Hong Li Fengfu Fu Guidi Yang Fujian Provincial Key laboratory of Agroecological Processing and Safety Monitoring Key Laboratory for Medicinal Plant Chemistry and Chemical BiologyCollege of JunCao Science and EcologyFujian Agriculture and Forestry UniversityFuzhou 350002China Department of chemistry Birendra Multiple CampusTribhuvan UniversityChitwan 00977-44200BharatpurNepal Key laboratory for Analytical Science of food Safety and Biology of Ministry of Education Fujian Provincial Key Lab of Analysis and Detection for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350116China

Selenium(Se)in paddy rice is one of the significant sources of human Se ***,the effect of arsenic(As)pollution in soil on the translocation of Se species in rice plants is *** this research,a pot experiment was designed to examine the effect of the addition of 50 mg As/kg soil as arsenite or arsenate on the migration of Se species from soil to indica Minghui 63 and *** results showed that the antagonism between inorganic As and Se was closely related to the rice cultivar and Se oxidation state in *** to the standalone selenate treatment,arsenite significantly(p<0.05)decreased the accumulation of selenocystine,selenomethionine and selenate in the roots,stems,sheaths,leaves,brans and kernels of both cultivars by 21.4%-100.0%,40.0%-100.0%,41.0%-100%,5.4%-96.3%,11.3%-100.0% and 26.2%-39.7% respectively,except for selenocystine in the kernels of indica Minghui 63 and selenomethionine in the leaves of indica Minghui 63 and the stems of indica *** also decreased(p<0.05)the accumulation of selenocystine,selenomethionine and selenate in the roots,stems,brans and kernels of both cultivars by 34.9%-100.0%,30.2%-100.0%,11.3%-100.0% and 5.6%-39.6%respectively,except for selenate in the stems of indica Minghui ***,relative to the standalone selenite treatment,arsenite and arsenate decreased(p<0.05)the accumulation of selenocystine,selenomethionine and selenite only in the roots of indica Minghui 63 by 45.5%-100.0%.Our results suggested that arsenite and arsenate had better antagonism toward Se species in selenate-added soil than that in selenite-added soil;moreover,arsenite had a higher inhibiting effect on the accumulation of Se species than arsenate.

关键词： Rice(Oryza sativa L.) Inorganic arsenic Selenium species Translocation Antagonistic effect

Utilization of hydralazine as a reactive matrix for enhanced detection and on-MALDI-target derivatization of saccharides

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Chinese Chemical Letters 2024年第5期35卷 386-391页

作者： Dan Ouyang Huan Huang Yanting He Jiajing Chen Jiali Lin Zhuling Chen Zongwei Cai Zian Lin Ministry of Education Key laboratory of Analytical Science for food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350108China School of Pharmacy Bengbu Medical UniversityBengbu 233000China Partner State Key laboratory of Environmental and Biological Analysis Department of ChemistryHong Kong Baptist UniversityHong KongChina

Saccharides are a sort of ubiquitous and vital molecules within the whole ***,the application of saccharides analysis with matrix-assisted laser desorption/ionization mass spectrometry(MALDI-MS)is restricted by their low ionization efficiency and the instability of the sialic acid *** strategy based on nonreductive amination provides a good solution,however,this is often time consuming and may result in sample loss due to removal of excessive derivatization ***,hydralazine(HZN)was utilized as a reactive matrix for labeling reducing saccharides directly on MALDI target which eliminated tedious sample preparation and avoided sample *** optimization,effective and reproducible on-MALDI-target derivatization of neutral and acidic saccharides was achieved in both positive and negative *** with 2,5-dihydroxybenzoic acid(DHB)and 9-aminoacridine(9-AA),HZN improved the detection sensitivity of reducing saccharides and provided more abundant fragment ions in MS/MS ***,26 kinds of neutral glycans and 5 kinds of sialic glycans were identified from ovalbumin(OVA)and bovine fetuin,*** with the statistical models,this strategy could be used to distinguish and predict samples of 6 brands of beer,and discriminate 2 kinds of beer fermentation *** addition,HZN was applied for quantitative analysis of glucose in urine samples,and the obtained urine glucose concentrations of diabetic patients were consistent with the clinical test results,showing the potential of qualitative and quantitative analysis of reducing saccharides in complex samples.

关键词： Hydralazine Reactive matrix On-MALDI-target derivatization Saccharides

Decoding the genetic program of micronucleus formation: linking chromosomal instability to human disease

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Signal Transduction and Targeted Therapy 2024年第7期9卷 2840-2842页

作者： Jörg Fahrer Division of food chemistry and Toxicology Department of ChemistryRPTU Kaiserslautern-Landau67663 KaiserslauternGermany

A recent study by Adams and colleagues published in Nature unveiled more than one hundred genes that are involved in micronucleus formation,1 which is a biomarker for genomic instability and associated with aging,cancer,and other disorders.2 As an outstanding achievement,the authors identified DSCC1(DNA Replication And Sister Chromatid Cohesion 1)as a critical gene protecting against early developmental defects,genomic instability,reduced proliferative capacity,cohesinopathy-related phenotypes,and tumor development in vivo.

关键词： chromosomal linking Replication

MALDI coupled with laser-postionization and trapped ion mobility spectrometry contribute to the enhanced detection of lipids in cancer cell spheroids

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Chinese Chemical Letters 2024年第4期35卷 464-468页

作者： Jing Chen Peisi Xie Pengfei Wu Yu He Zian Lin Zongwei Cai Ministry of Education Key laboratory of Analytical Science for food Safety and Biology Fujian Provincial Key Laboratory of Analysis and Detection Technology for Food SafetyCollege of ChemistryFuzhou UniversityFuzhou 350116China Department of chemistry State Key Laboratory of Environmental and Biological AnalysisHong Kong Baptist UniversityHong KongChina College of Forestry Nanjing Forestry UniversityNanjing 210018China

Cancer cell spheroids(CCS) are a valuable three-dimensional cell model in cancer studies because they could replicate numerous characteristics of solid tumors. Increasing researches have used matrix-assisted laser desorption/ionization mass spectrometry imaging(MALDI-MSI) to investigate the spatial distribution of endogenous compounds(e.g., lipids) in CCS. However, only limited lipid species can be detected owing to a low ion yield by using MALDI. Besides, it is still challenging to fully characterize the structural diversity of lipids due to the existence of isomeric/isobaric species. Here, we carried out the initial application of MALDI coupled with laser-postionization(MALDI-2) and trapped ion mobility spectrometry(TIMS) imaging in HCT116 colon CCS to address these challenges. We demonstrated that MALDI-2 is capable of detecting more number and classes of lipids in HCT116 colon CCS with higher signal intensities than MALDI. TIMS could successfully separate numerous isobaric/isomeric species of lipids in CCS. Interestingly, we found that some isomeric/isobaric species have totally different spatial distributions in colon CCS. Further MS/MS imaging analysis was employed to determine the compositions of fatty acid chains for isomeric species by examining disparities in signal intensities and spatial distributions of product ions. This work stresses the robust ability of TIMS and MALDI-2 imaging in analyzing endogenous lipids in CCS, which could potentially become powerful tools for future cancer studies.

关键词： Matrix-assisted laser desorption/ionization(MALDI) Mass spectrometry imaging MALDI coupled with laser-postionization Trapped ion mobility spectrometry Cancer cell spheroids

Constructing porous ZnFC-PA/PSF composite spheres for highly efficient Cs^(+) removal

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Journal of Environmental Sciences 2024年第9期143卷 126-137页

作者： Senjian Han Chao Gao Wenfeng Yan Yafei Guo Shiqiang Wang Tianlong Deng College of Marine and Environmental Sciences Tianjin University of Science and TechnologyTianjin 300457China Key laboratory of Marine Resource chemistry and food Technology Ministry of EducationTianjin 300457China

Radioisotope leaking from nuclear waste has become an intractable problem due to its gamma radiation and strong water *** this work,a novel porous ZnFC-PA/PSF composite sphere was fabricated by immobilization of ferrocyanides modified zinc phytate into polysulfone(PSF)substrate for the treatment of Cs-contaminated *** maximum adsorption capacity of ZnFC-PA/PSF was 305.38 mg/g,and the removal efficiency of Cs+was reached 94.27%within 2 *** ZnFC-PA/PSF presented favorable stability with negligible dissolution loss of Zn^(2+)and Fe^(2+)(<2%).The ZnFC-PA/PSF achieved high-selectivity towards Cs+(K_(d)=2.24×10^(4)mL/g)even in actual geothermal *** adsorption mechanism was inferred to be the ion-exchange between Cs^(+)and K^(+).What’s more,ZnFC-PA/PSF worked well in the fixed-bed adsorption(E=91.92%),indicating the application potential for the hazardous Cs^(+)removal from wastewater.

关键词： Adsorption Cesium Metal ferrocyanide Composite adsorbent

Single-atom catalysts for neutral zinc-air batteries

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Science China Materials 2024年第5期67卷 1674-1675页

作者： Jiaxu Zhang Minghao Yu Faculty of chemistry and food chemistry&Center for Advancing Electronics Dresden(CfAED) Technische Universität DresdenDresden01062Germany

The escalating global energy demand underscores the urgency of developing sustainable battery ***-air batteries(ZABs)have emerged as promising candidates due to their costeffectiveness,safety,and high energy density[1-4].Conventional ZABs typically rely on a four-electron(4e-)oxygen reduction reaction(ORR)in strongly alkaline electrolytes.

关键词： battery neutral typically

Diatomic Fe-Co catalysts synergistically catalyze oxygen evolution reaction

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Nano Research 2024年第5期17卷 3794-3800页

作者： Tianmi Tang Jingyi Han Zhenlu Wang Xiaodi Niu Jingqi Guan Institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China College of food Science and Engineering Jilin UniversityChangchun 130062China

The design of diatomic catalysts with uniformly dispersed metal atoms is expected to improve catalytic performance,which is conducive to the intensive comprehending of the synergistic mechanism between dual-metal sites for the oxygen evolution reaction(OER)at the atomic ***,we design a strategy to immobilize bimetallic Fe-Co atoms onto nitrogen-doped graphene to obtain a diatomic catalyst(DA-FC-NG)with FeN_(3)-CoN_(3) *** DA-FC-NG shows excellent OER activity with a low overpotential(η_(10)=268 mV),which is superior to commercial iridium dioxide *** calculations uncover that the excellent activity of DA-FC-NG is due to the interaction between Fe and Co diatoms,which causes charge rearrangement and induces the adsorption of intermediates on the Fe-O-Co bridge structure,thus improving the catalytic OER *** work is of great significance for the design of highly active diatomic catalysts to replace noble metal catalysts for energy-related applications.

关键词： oxygen evolution reaction diatomic catalyst FeN_(3)-CoN_(3) X-ray absorption spectroscopy(XAS)spectrum theoretical calculation