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HDpairFinder:A data processing platform for hydrogen/deuterium isotopic labeling-based nontargeted analysis of trace-level amino-containing chemicals in environmental water

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Journal of Environmental Sciences 2024年第2期136卷 583-593页

作者： Tingting Zhao Kristin Carroll Caley B.Craven Nicholas J.p.Wawryk Shipei Xing Jian guo Xing-Fang Li Tao Huan department of chemistry Faculty of ScienceUniversity of British ColumbiaVancouver Campus2036 Main MallVancouverBritish ColumbiaV6T 1Z1Canada Division of Analytical and Environmental Toxicology Department of Laboratory Medicine and PathologyFaculty of Medicine and DentistryUniversity of AlbertaEdmontonAlberta T6G 2G3Canada

The combination of hydrogen/deuterium(H/D)formaldehyde-based isotopic methyl labeling with solid-phase extraction and high-performance liquid chromatography–high resolution mass spectrometry(HpLC-HRMS)is a powerful analytical solution for nontargeted analysis of trace-level amino-containing chemicals in water *** the huge amount of chemical information generated in HpLC-HRMS analysis,identifying all possible H/Dlabeled amino chemicals presents a significant challenge in data *** address this,we designed a streamlined data processing pipeline that can automatically extract H/D-labeled amino chemicals from the raw HpLC-HRMS data with high accuracy and ***,we developed a cross-correlation algorithm to correct the retention time shift resulting from deuterium isotopic effects,which enables reliable pairing of H-and D-labeled ***,we implemented several bioinformatic solutions to remove false chemical features generated by in-source fragmentation,salt adduction,and natural13C ***,we used a data mining strategy to construct the AMINES library that consists of over 38,000 structure-disjointed primary and secondary amines to facilitate putative compound ***,we integrated these modules into a freely available R program,*** rationale of each module was justified and its performance tested using experimental H/D-labeled chemical standards and authentic water *** further demonstrated the application of HDpairFinder to effectively extract N-containing contaminants,thus enabling the monitoring of changes of primary and secondary N-compounds in authentic water *** is a reliable bioinformatic tool for rapid processing of H/D isotopic methyl labeling-based nontargeted analysis of water samples,and will facilitate a better understanding of N-containing chemical compounds in water.

关键词： Isotope labeling Nontargeted analysis Reactive N-compounds HpLC-HRMS Source water

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Covalent triazine frameworks modified by ultrafine pt nanoparticles for efficient photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 4908-4915页

作者： Xu Han Xueying ge Wen-Wen He Wangwang Shen Tao Zhou Jian-Sen Wang Rong-Lin Zhong Abdullah MAl-Enizi Ayman Nafady Shengqian Ma School of chemistry and Life Science Advanced Institute of Materials ScienceChangchun University of TechnologyChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China department of chemistry University of North Texas1508 W.Mulberry St.DentonTX 76201USA department of chemistry College of ScienceKing Saud UniversityRiyadh 11451Saudi Arabia

pt nanoparticles(ptNps)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen *** this study,a Schottky heterojunction has been successfully constructed by evenly loading ultrafine ptNps onto a triazine-based covalent organic frameworks(COFs).This strategy maintained the high activity of these ultra-small ptNps while maximizing the utilization of the pt active *** fabricated ptNps@covalent triazine-based framework-1(CTF-1)composite accomplished a significantly high rate of hydrogen evolution(20.0 mmol·g^(−1)·h^(−1),apparent quantum efficiency(AQE)=7.6%,atλ=450 nm)with 0.40 wt.%pt loading,giving rise to a 44-fold-increase in the efficiency of the photocatalytic hydrogen production compared to the pristine *** calculations revealed that the strong electron transfer(Q(pt)=−0.726 qe,in the analysis of Bader charge,Q(pt)is the charge quantity transferred from pt cluster to CTF-1,and qe is the unit of charge transfer quantity)between ptNps and CTF-1 triggers a strong interaction,which makes ptNps being firmly attached to the structure of CTF-1,thereby enabling high stability and excellent hydrogen production ***,the hydrogen binding free energy(ΔgH*)of ptNps@CTF-1 is much lower than that of the unmodified CTF-1,leading to a much lower intermediate state and hence a significant improvement in photocatalytic *** overall findings of this work provide a new platform to incorporate metallic Nps into COFs for the design and fabrication of highly efficient photocatalysts.

关键词： pt nanoparticles covalent triazine-based framework-1(CTF-1) photocatalysts hydrogen evolution reaction

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Combining cisplatin and a STINg agonist into one molecule for metalloimmunotherapy of cancer

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National Science Review 2024年第1期11卷 107-119页

作者： Shuren Zhang Dongfan Song Wenhao Yu Ji Li Xiaoyu Wang Yachao Li Zihan Zhao Qi Xue Jing Zhao Jie p.Li Zijian guo State Key Laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center (ChemBIC) Nanjing University department of Urology Afflliated Drum Tower HospitalMedical SchoolNanjing University Nanchuang (Jiangsu)Institute of chemistry and Health

Mounting evidence suggests that strategies combining DNA-damaging agents and stimulator of interferon genes(STINg) agonists are promising cancer therapeutic regimens because they can amplify STINg activation and remodel the immunosuppressive tumor microenvironment. However, a single molecular entity comprising both agents has not yet been developed. Herein, we designed two ptIV-MSA-2 conjugates(Ⅰand Ⅱ) containing the DNA-damaging chemotherapeutic drug cisplatin and the innate immuneactivating STINg agonist MSA-2; these conjugates showed great potential as multispecific small-molecule drugs against pancreatic cancer. Mechanistic studies revealed that conjugate Ⅰ upregulated the expression of transcripts associated with innate immunity and metabolism in cancer cells, significantly differing from cisplatin and MSA-2. An analysis of the tumor microenvironment demonstrated that conjugate I could enhance the infiltration of natural killer(NK) cells into tumors and promote the activation of T cells, NK cells and dendritic cells in tumor tissues. These findings indicated that conjugate I, which was created by incorporating a pt chemotherapeutic drug and STINg agonist into one molecule, is a promising and potent anticancer drug candidate, opening new avenues for small-molecule-based cancer metalloimmunotherapy.

关键词： platinum drug STINg agonist single-molecule multitarget metalloimmunology

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Effects of length alteration of OpE-containing mono- and dinuclear alkynylplatinum(II) terpyridine complexes on photophysical, structural and morphological properties

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Nano Research 2024年第10期17卷 8893-8903页

作者： Jason Koon-Lam poon Sammual Yu-Lut Leung Eric Ka-Ho Wong Vivian Wing-Wah Yam Institute of Molecular Functional Materials State Key Laboratory of Synthetic Chemistry and Department of ChemistryThe University of Hong KongHong Kong 999077China

A series of mononuclear complexes and unsymmetric dinuclear alkynylplatinum(II)terpyridine complexes with oligo(paraphenylene ethynylene)(OpE)-derived backbone with a variation of the lengths of alkoxy chains and OpE backbones was *** morphological properties,packing lattice and gelation behaviors of the mononuclear complexes were systematically studied,and the thermodynamic parameters and packing lattices of the dinuclear complexes were also investigated,providing further insights into the roles of the non-covalent interactions and their delicate balance in constructing sophisticated supramolecular *** and nanotube formation have been observed upon a delicate control of the intermolecular interactions by altering the lengths and structural dimensions of the complexes.

关键词： supramolecular chemistry self-assembled nanostructures platinum(II)complexes metallogel

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Enhanced charge separation by incomplete calcination modified co-doped TiO_(2)nanoparticle for isothiazolinone photocatalytic degradation

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Nano Research 2024年第6期17卷 4834-4843页

作者： Zhiren guo Xiao Zhang Xinyuan Li Chang Cui Zilei Zhang Hansheng Li Dongxiang Zhang Jinying Li Xiyan Xu Jiatao Zhang School of chemistry and Chemical Engineering Beijing Institute of TechnologyBeijing 102488China department of chemistry MSU-BIT UniversityShenzhen 517182Chin

photocatalytic oxidation techniques are promising for degradation of the highly ecotoxic and refractory isothiazolinone bactericides in relevant industrial ***,low charge separation and directional transport efficiency under solar light radiation restrain their practical ***,we report a nanostructured photocatalyst doped with gd and B in TiO_(2)with carbon incorporation and defect formation through incomplete *** specific surface area,grain size,and hydrophilicity of TiO_(2)are improved,which is beneficial for the interfacial reaction between the photocatalyst and *** reduction of the bandgap,the broadening of the photo-absorption range,and the retarded electron-hole recombination promote the photocatalytic performance due to the improved oxygen vacancies based on the electron distribution *** difference in partial density of states(ΔpDOS)between the current catalyst and raw TiO_(2)indicates that the co-doping of gd and B with incomplete calcination changes the electronic hybridization of conduction band and valence band near the Fermi level,and affects the band gap *** improved charge separation and directional transport efficiency and benefited the formation of main active species,including•OH and O_(2)•−,for the pollutant *** rate of photocatalytic removal of benzisothiazolinone(BIT)by the current photocatalyst reaches 1.25 h^(−1),being 4.31 times that of TiO_(2).The current work offers a constructive approach to the design and synthesis of nanostructured photocatalysts for the photocatalytic degradation of refractory organic pollutants.

关键词： TiO_(2)nanoparticle charge separation oxygen vacancies electron distribution modification photocatalytic degradation

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Emerging two-dimensional Mo-based materials for rechargeable metal-ion batteries:Advances and perspectives

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Journal of Energy chemistry 2024年第2期89卷 487-518,I0012页

作者： Qingqing Ruan Yuehua Qian Mengda Xue Lingyun Chen Qichun Zhang department of Applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China department of Materials Science and Engineering City University of Hong Kong999077Hong KongChina

With the rapid development of rechargeable metal-ion batteries(MIBs)with safety,stability and high energy density,significant efforts have been devoted to exploring high-performance electrode *** recent years,two-dimensional(2D)molybdenum-based(Mo-based)materials have drawn considerable attention due to their exceptional characteristics,including low cost,unique crystal structure,high theoretical capacity and controllable chemical ***,like other transition metal compounds,Mo-based materials are facing thorny challenges to overcome,such as slow electron/ion transfer kinetics and substantial volume changes during the charge and discharge *** this review,we summarize the recent progress in developing emerging 2D Mo-based electrode materials for MIBs,encompassing oxides,sulfides,selenides,*** introducing the crystal structure and common synthesis methods,this review sheds light on the charge storage mechanism of several 2D Mo-based materials by various advanced characterization *** latest achievements in utilizing 2D Mo-based materials as electrode materials for various MIBs(including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)and zinc-ion batteries(ZIBs))are discussed in ***,the modulation strategies for enhancing the electrochemical performance of 2D Mo-based materials are highlighted,focusing on heteroatom doping,vacancies creation,composite coupling engineering and nanostructure ***,we present the existing challenges and future research directions for 2D Mo-based materials to realize high-performance energy storage systems.

关键词： Molybdenum-based materials Two-dimensional materials Lithium-ion batteries Sodium-ion batteries Zinc-ion batteries

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Two Indium(III)-based Fluorescent Metal-Organic Frameworks for Highly Sensing Fe^(3+),2,4-DNp,and TNp

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Chemical Research in Chinese Universities 2024年第1期40卷 119-126页

作者： WANg Dan LI Wen LI guanghua HUA Jia LIU Yunling State Key Laboratory of Inorganic Synthesis&preparative chemistry Jilin UniversityChangchun130012P.R.China

Two novel metal-organic frameworks(MOFs),JLU-MOF130([In(NH2−BDC)(Imi)(1H−Imi)]·DMF·H2O,NH2−H2BDC=2-aminobenzene-1,4-dicarboxylic acid,1H−Imi=1H-imidazole,DMF=N,N-dimethylformamide)and JLU-MOF131([In(1,4-NDC)(Imi)(1H−Imi)]·DMF0.5,1,4-H_(2)NDC=1,4-naphthalene-dicarboxylic acid),were ***-MOF130 features a three-dimensional(3D)architecture with a neb ***-MOF131 is characterized by a two-dimensional(2D)structure with an sql ***-MOF130 has excellent fluorescence detection performance towards Fe^(3+),2,4-dinitrophenol(2,4-DNp),and 2,4,6-trinitrophenol(TNp),but the fluorescence detection performance of JLU-MOF131 is further improved by converting NH2−H2BDC to more conjugated 1,4-H_(2)*** Stern-Volmer(SV)quenching constant(KSV)values of JLU-MOF130 sensing 2,4-DNp,TNp,and Fe^(3+)are 5.24×10^(4),4.44×10^(4),and 4.73×10^(3) L/mol,*** corresponding limit of detection(LOD)values are 1.17,1.36,and 14.59µmol/*** KSV values for JLU-MOF131 are 1.26×10^(5),9.02×10^(4),and 8.48×103 L/mol,and the corresponding LOD values are 0.35,0.42,and 3.60µmol/L,***,the emission wavelengths of the two MOFs obviously shift as the fluorescence emission intensities decrease upon the addition of 2,4-DNp and TNp,which can be applied in selective detection.

关键词： Metal-organic framework Fluorescence quenching Fe^(3+) 2 4-Dinitrophenol(2 4-DNp) 2 4 6-Trinitrophenol(TNp)

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Reaction Kinetics and Secondary Organic Aerosol Composition Analysis of 2-Cyclohexen-1-one with NO_(3) Radicals

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Chemical Research in Chinese Universities 2024年第4期40卷 730-736页

作者： HU Lin TONg Shengrui XU Yanyong ZHANg Hailiang YU Shanshan CHEN Meifang gE Maofa Structural chemistry of Unstable and Stable Species Chinese Academy of Sciences Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing100190P.R.China College of Ecology and Environment Xinjiang UniversityUrumqi830017P.R.China University of Chinese Academy of Sciences Beijing100049P.R.China

Unsaturated ketones are typical oxygenated volatile organic compounds(OVOCs)with high reactivity,and are important precursors in air *** sources of OVOCs are complex and include direct emissions and secondary oxidation formation of VOCs in the atmosphere.2-Cyclohexen-1-one is a widespread substance,and is derived from the industrial catalytic oxidation of *** this paper,we investigated the rate constants of the chemical reactions of 2-cyclohexen-1-one with NO_(3) radicals,which is(7.25±0.29)×10^(-15) cm^(3)·molecule^(-1)·s^(-1) at 298 K and under 1 atm(1 atm=101325pa).It supplemented the kinetics of NO_(3) radicals database,and revealed its effects in the nighttime *** addition,the reaction products of 2-cyclohexen-1-one with NO_(3) radicals were detected by Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS),which revealed a series of nitrate esters in the composition of the secondary organic aerosol(SOA),which may reduce atmospheric ***,the possible pathways for the generation of the products were developed.

关键词： Kinetics Unsaturated ketone Nitrate radical Secondary organic aerosol

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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu Nps@MOFs catalyst under mild conditions

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Science China chemistry 2024年第5期67卷 1561-1568页

作者： peng-Fei guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao Key Laboratory of Advanced Energy Material chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(Nps)to form Cu Nps@1-x(x=1,2,3,and 4)with varying loading amounts of Cu Nps at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** Nps@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu Nps@1-3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu Nps@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu Nps and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu Nps@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

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proteins as nanomagnets and magnetoreceptors

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Zoological Research 2024年第4期45卷 831-832页

作者： p.J.Hore department of chemistry University of OxfordUK

It is an appealing notion that a protein molecule could act as a nanomagnet.A genetically encodable biomolecule with a permanent magnetic moment at room temperature could have a range of applications:a magnetogenetic actuator,a magnetic tag for purifying and immobilizing enzymes,a contrast agent for magnetic resonance imaging,and a basis for a biomimetic magnetic sensing device,to name just a few.A magnetic protein could perhaps also function as the sensor in the magnetic compass that enables small songbirds to navigate the huge distances between their breeding and wintering *** though such possibilities may be,how realistic are they?

关键词： magnetic magnets enable

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