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Journal of Rare Earths 2024年第7期42卷 1298-1303页

作者： Pei-Yu Liao Yu-Quan Qi Zhen Li Jian-Hua Jia Ming-Liang Tong key laboratory of bioinorganic and Synthetic chemistry of Ministry of Education School of ChemistrySun Yat-Sen University

On account of the complicated magnetic exchange interactions between lanthanide ions,binuclear lanthanide complexes have broad application prospect in the field of single-molecule magnets.Therefore,it is necessary to develop reasonable bridging ligands to manipulate the directional assembly of binuclear lanthanide complexes.Herein,we selected the macrocyclic ligand LN8O2to build up two new dilanthanide complexes [Ln2(LN8O2)（OpyO）2（H2O）2]（NO3）2(1-Ln,Ln=Dy,Tb;LN8O2=hexamethyl-tetraaza-dioxe-dipyrazolacycloicosaphane-2,9,12,19-tetraene;OpyOH=2-pyridinol-1-oxide).Dynamic magnetic studies show that 1-Dy exhibits slow relaxation behavior under a 1 kOe applied field.Further fitting analysis of relaxation times gives the effective energy barrier of 38.2 cm-1,and reveals that the slow magnetic relaxation behavior is dominated by the Orbach and Raman processes.High-resolution luminescence emission spectrum indicates the energy gap of 36.8 cm-1 between the ground state and the first excited state,consistent with the magnetic measurement results.1-Tb exhibits brilliant characteristic green light emission under UV light excitation.The absolute quantum yield of 1-Tb is 44.8%,and its first-order fitted decay lifetime is 779.21 μs at room temperature.This study provides the way for directional construction of high-performance molecular materials with magnetic and optical dualfunction.

关键词： Dilanthanide complexes Macrocyclic ligand Photoluminescence behavior Rare earths Single-molecule magnets

Multifunctional properties of a polar spin chain compound[N(C_(3)H_(7))_(4)][Cu(C_(8)H_(4)NO_(4))]·H_(2)O exhibiting both one-dimensional magnetism and nonlinear optical activity

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Chinese Chemical Letters 2024年第2期35卷 622-625页

作者： Ang Li Yanhong Wang Haotian Tian Alimujiang Yalikun Yves Journaux Min Luo Hongcheng Lu key laboratory of material chemistry for Energy Conversion and Storage School of Chemistry and Chemical EngineeringHubei Key Laboratory of Bioinorganic Chemistry & Materia MedicaHuazhong University of Science and TechnologyWuhan 430074China key laboratory of optoelectronic materials chemistry and Physics Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 35002China Institut Parisien de Chimie Moléculaire IPCMSorbonne UniversitéCNRSParis F-75252France

Functional materials with multiple properties are urgent to be explored to reach high requirements for applications nowadays.In this work,a new multifunctional one-dimensional(1D)chain compound[N(C_(3)H_(7))_(4)][Cu(ohpma)]·H_(2)O 1(ohpma=deprotonated N-(2-hydoxyphenyl)oxamic acid)exhibiting both 1D antiferromagnetic and nonlinear optical properties,which are both originated from the same polar[Cu(C_(8)H_(4)NO_(4))]magnetic units,has been successfully synthesized by evaporation at room temperature.Bis-polydentate nature of the(ohpma)3−ligand with constrained tridentate and bidentate coordination sites conducts Cu^(2+)ions coordinating in different geometries and forms 1D chains along the c axis,which are further separated by the[N(C_(3)H_(7))_(4)]+cations.And the 1D magnetic chains further exhibit noncentrosymmetric polar arrangement.Nonlinear optical study shows polar compound 1 exhibits a discernible second-harmonic generation(SHG)efficiency and the calculation of the partial density of states indicates that the SHG efficiency of 1 is mainly originated from the polar[Cu(C_(8)H_(4)NO_(4))]magnetic units.Moreover,magnetic susceptibility shows a broad maximum around 70 K with strong intrachain interaction of J/k B=−113.0 K but no long-range order is observed down to 2 K,suggesting that 1 shows a good 1D magnetism.Both good 1D magnetism and SHG activity suggest that 1 could be as a potential multifunctional material,particularly.

关键词： Multifunctional properties Magnetic property Nonlinear optical property Evaporation One-dimensional chain

Upgrading waste NO_(x) into amino acids via electrocatalysis on Co nanoparticles encapsulated in hollow carbon nanofibers

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Science China chemistry 2024年第6期67卷 1946-1952页

作者： Jiahui Xian Kaixing Cai Peisen Liao Shihan Wang Guangqin Li key laboratory of bioinorganic and Synthetic chemistry of Ministry of Education LIFMIGCMESchool of ChemistrySun Yat-Sen UniversityGuangzhou510275China

Electrocatalytic conversion of waste nitrogen oxide(NO_(x))into value-added nitrogenous chemicals,especially amino acid,is an emerging strategy to alleviate NO_(x)pollution.However,this process suffers from the coexistence of multiple competitive reactions leading to complex product distribution and low efficiency,and thus the rational design and modulation of efficient catalysts remains a formidable challenge.Herein,well-designed Co nanoparticles encapsulated in hollow carbon nanofiber(CoHCNF)were constructed to promote the amino acid electrosynthesis via dealing waste NO_(x)coupling with biomass-derived keto acids.Ascribed to the rapid reactant diffusion,electron transport and efficient contact with abundant accessible Co catalytic sites stemmed from the unique hollow nanotubular structure,Co-HCNF manifested impressive glycine synthesis performance in one-pot adopting NO as the nitrogen source with Faradaic efficiency(FE)of 41.7%and a corresponding yield rate of 222.3μmol h^(-1)as well as 120 h robust stability.Interestingly,it also demonstrates an excellent performance with the FE of 42.8%for NO_(3)~-solution as the nitrogen source.Specially,this strategy displays a broad universality for the synthesis of other amino acids.This work not only highlights the importance of hollow-structuring electrocatalyst towards upgrading wasted NO_(x)species into amino acids,but also promotes the further development of electrosynthetic systems for high-valued N-containing organic chemicals.

关键词： electrocatalysis NO_(x)reduction amino acid porous materials hollow structure

Traceless photodegradable polymer cocoons for universal protein delivery and light-controlled gene editing

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Science China chemistry 2024年第2期67卷 664-676页

作者： Huaibin Yu Meron Tsegay Kifle Lili Chen Feihong Xiong Yan Zhang Shangbang Gao Wei Hou Shuliang Chen Weining Zhao Yuzhou Wu hubei Engineering Research Center for Biomaterials and medical Protective materials Hubei Key Laboratory of Bioinorganic Chemistry&Materia MedicaKey Laboratory of Material Chemistry for Energy Conversion and StorageMinistry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan430074China Zhengzhou Research Institute Harbin Institute of TechnologyZhengzhou450000China College of Life Science and Technology Huazhong University of Science and Technology(HUST)Wuhan430074China Institute of medical Virology School of Basic Medical SciencesWuhan UniversityWuhan430071China College of Pharmacy Shenzhen Technology UniversityShenzhen518118China

Polymer conjugation was found highly valuable in clinic to improve the bioavailability of protein therapeutics.However,it is still a tremendous challenge to achieve a complete release of original proteins from the conjugated hybrid under external stimulus to recover active proteins in the targeted tissue.Herein,we report a general light-controlled protein delivery methodology by weaving a photodegradable polymer cocoon around proteins,which could reliably protect them from degradation in the dark while efficiently releasing them under illumination without any residual atoms.The surface charge of the polymer shell is easily tunable to facilitate efficient cell uptake.The versatility of this strategy is demonstrated by the delivery of the Cas9/sg RNA complex that realized light-controlled gene editing both in vitro and in vivo,and such repertoire is of particular value in regard to minimizing the off-target toxicity of CRISPR-Cas9-based gene therapy.

关键词： photodegradable polymer-protein conjugate protein delivery light control gene editing

Light-induced stepped thermal relaxation in a Hofmann-type metal-organic framework

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Science China chemistry 2024年第6期67卷 1983-1989页

作者： Wen Cui Wei-Wei Wu Ze-Yu Ruan Yan-Cong Chen Guang-Jun Zeng Guan-Xi Chen Si-Guo Wu Zhao-Ping Ni Ming-Liang Tong key laboratory of bioinorganic and Synthetic chemistry of Ministry of Education School of ChemistryInstitute of Green Chemistry and Molecular EngineeringGuangdong Basic Research Center of Excellence for Functional Molecular EngineeringSun Yat-sen UniversityGuangzhou510275China

Spin-crossover(SCO)materials with light-induced multistability have potential applications in multi-addressable opto-magnetic memory devices and multiple switches.Here,we reported a three-dimensional Hofmann-type metal-organic framework(MOF)[Fe(bpy){Pt(CN)_(4)}]·coumarin(1·coumarin,bpy=4,4′-bipyridine),which exhibits an incomplete and hysteretic SCO behavior.Most importantly,the light-induced stepped thermal relaxation(LISTR)with obvious magnetic plateau for a hidden intermediate spin state is firstly realized.This hidden spin state is also observed for the first time in the thermal relaxation after light-assisted spin state annealing(LASSA).Meanwhile,an extremely rare bi-directional light-induced excited spin-state trapping(LIESST)with the highest reverse-LIESST temperature is observed.Therefore,five spin states can be captured in 1·coumarin and the tristability can be modulated below 102 K through the excitation-relaxation mechanism.Hence,the light-and temperatureinduced multistability provides a new strategy for developing multistable materials.

关键词： light magnetic multistability iron metal-organic framework spin-crossover

Natural products inspired[3+2]cycloaddition enables efficient construction of hydroxylated tetrahydrofuran acetals and concise syntheses of lignans

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Science China chemistry 2024年第7期67卷 2306-2313页

作者： Dong-Yue Cai Weiming Shi Zhao-Hui Jin Zhi-Xiang Yu Jin-Xin Zhao Jian-Min Yue State key laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China University of Chinese Academy of Sciences Beijing 100049China Beijing National laboratory for Molecular Sciences(BNLMS) Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking UniversityBeijing 100871China

Mimicking biosynthetic pathways of hongkonoids led to the development of a new Cu(Ⅰ)-catalyzed[3+2]cycloaddition ofα-hydroxyketone andβ-keto enol ethers,affording tetrahydrofuran acetals in a highly diastereoselective manner and 100%atom economy.Computational studies on the mechanism disclosed a concerted but asynchronous Michael addition/aldol reaction.Of the same importance,this methodology provides a practical biomimetic approach for one-step construction of the dibenzylbutyrolactol lignan backbone starting from two phenyl propane derivatives,opening up a powerful new approach for lignan synthesis,which is showcased by succinct total syntheses of two biologically important aryltetralin-type lignans,β-apopicropodophyllin and cycloolivil.Given the mild and operationally simple conditions,the developed chemistry might have a promising prospect in potential industrial applications.

关键词： [3+2]cycloaddition transition-metal catalysis tetrahydrofuran lignans natural products

A comprehensive review of meal?replacement from dining table to sickbed: beyond biomedical potentials

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Food Science and Human Wellness 2024年

作者： Hao Qiang Tianshu Xu Peng Ma Siyuan Zhang Guanhua Du Guifen Qiang Tengfei Ji The School of chemistry Cardiff University State key laboratory of Bioactive Substance and Function of Natural Medicines Institute of materia medica Chinese Academy of medical Sciences and Peking Union medical College and Beijing key laboratory of Drug Target and Screening Research State key laboratory Institute of materia medica Chinese Academy of medical Sciences and Peking Union medical College

The emergence of meal replacement (MR) originates from physical exercise or fitness as a substitute for one or all meals and later expands to the field of weight loss. Indeed， the main application of current meal replacement is to lose body weight， whether patients with obesity， diabetes， fatty liver， infertile or pregnant women can benefit from weight loss. In addition， MRs still exhibit more biomedical potential in preventing and treating diseases， like anti-diabetes， improving fatty liver and kidney disease， preventing cancer， conceiving and reducing pregnancy complications， and improving life quality. Indeed， there are also disadvantages to meal replacement， including causing adverse effects， although most are acceptable and tolerated. To date， various commercially-developed MRs are walking from dining table to sickbed. Therefore， a scientific understanding of the advantages and disadvantages of meal replacements is crucial for their extensive application beyond biomedical potentials.

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Upgrading waste NOinto amino acids via electrocatalysis on Co nanoparticles encapsulated in hollow carbon nanofibers

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Science China chemistry 2024年

作者： Jiahui Xian Kaixing Cai Peisen Liao Shihan Wang Guangqin Li IGCME key laboratory of bioinorganic and Synthetic chemistry of Ministry of Education LIFM Sun Yat-Sen University School of chemistry

Electrocatalytic conversion of waste nitrogen oxide (NOx) into value-added nitrogenous chemicals, especially amino acid, is an emerging strategy to alleviate NOxpollution. However, this process suffers from the coexistence of multiple competitive reactions leading to complex product distribution and low efficiency, and thus the rational design and modulation of efficient catalysts remains a formidable challenge. Herein, well-designed Co nanoparticles encapsulated in hollow carbon nanofiber (CoHCNF) were constructed to promote the amino acid electrosynthesis via dealing waste NOxcoupling with biomass-derived keto acids. Ascribed to the rapid reactant diffusion, electron transport and efficient contact with abundant accessible Co catalytic sites stemmed from the unique hollow nanotubular structure, Co-HCNF manifested impressive glycine synthesis performance in one-pot adopting NO as the nitrogen source with Faradaic efficiency (FE) of 41.7%and a corresponding yield rate of 222.3μmol h-1as well as 120 h robust stability. Interestingly, it also demonstrates an excellent performance with the FE of 42.8%for NO3~– solution as the nitrogen source. Specially, this strategy displays a broad universality for the synthesis of other amino acids. This work not only highlights the importance of hollow-structuring electrocatalyst towards upgrading wasted NOxspecies into amino acids, but also promotes the further development of electrosynthetic systems for high-valued N-containing organic chemicals.

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Concise Synthesis of Lactococcus garvieae Lipoteichoic Acids Through an Additive-Modulated Preactivation Protocol and the Immunological Studies

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CCS chemistry 2024年第2期6卷 403-414页

作者： Tianlu Li Tong Li Yue Yang Haoru Zhuang Jianwu Lv Ning Zhou Miaomiao Zhang Fengshan Wang Yiqun Geng Richard R.Schmidt Peng Peng National Glycoengineering Research Center Shandong Key Laboratory of Carbohydrate Chemistry and GlycobiologyNMPA Key Laboratory for Quality Research and Evaluation of Carbohydrate Based MedicineShandong UniversityQingdao 266237 State key laboratory of Bioactive Substance and Function of Natural Medicines Institute of Materia MedicaChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100050 Department of chemistry University of KonstanzD-78457 Konstanz

Lipoteichoic acids(LTAs)are macroamphiphiles composed of alditol,lipid,phosphate,and carbohydrate units.Due to their inherent complexity,it is a severe challenge to access LTAs with structural integrity from natural sources for biological or immunological evaluation.Here,we describe the first total synthesis of Lactococcus garvieae LTA(type II LTA),containing five distinct 1,2-cis gluco/galactopyranosidic linkages,via a novel additive-modulated O-glycosyl trichloroacetimidate preactivation glycosidation strategy.This strategy features(1)high glycosidation yields and excellent 1,2-cis stereoselectivities independent of the donor anomeric configuration,(2)common and inexpensive reagents as promoters and additives,(3)application to standard glycosyl imidate donors without resorting to participating protection,and(4)general application to reactive and less reactive glycosyl acceptors.Thus,via the precise stereocontrolled construction of three galactopyranosidic and two glucopyranosidic bonds on a multigram scale,a series of structurally well-defined LTA molecules were successfully assembled.Immunological evaluation of these type II synthetic LTAs showed a structure–activity relationship in the stimulation of a proinflammatory response.

关键词： 1,2-cis glycosidation stereoselectivity lipoteichoic acid total synthesis additive-modulated trichloroacetimidate glycosidation immune response

Reynosin protects neuronal cells from microglial neuroinflammation by suppressing NLRP3 inflammasome activation mediated by NADPH oxidase

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Chinese Journal of Natural Medicines 2024年第6期22卷 486-500页

作者： YANG Yanqiu CHE Yue FANG Mingxia YAO Xiaohu ZHOU Di WANG Feng CHEN Gang LIANG Dong LI Ning HOU Yue key laboratory of Bioresource Research and Development of Liaoning Province College of Life and Health SciencesNorth-eastern UniversityShenyang 110000China National Frontiers Science Center for Industrial Intelligence and Systems Optimization Key Laboratory of Data Analytics and Optimization for Smart IndustryMinistry of EducationNortheastern UniversityShenyang 110000China School of Traditional Chinese materia medica Key Laboratory of Innovative Traditional Chinese Medicine for Major Chronic Diseases of Liaoning provinceKey Laboratory for TCM Material Basis Study and Innovative Drug Development of Shenyang CityShenyang Pharmaceutical UniversityShenyang 110000China State key laboratory for chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541000China

Neuroinflammation,mediated by the nucleotide-binding oligomerization domain-like receptor family pyrin domain-containing-3(NLRP3)inflammasome,is a significant contributor to the pathogenesis of neurodegenerative diseases(NDDs).Reynos-in,a natural sesquiterpene lactone(SL),exhibits a broad spectrum of pharmacological effects,suggesting its potential therapeutic value.However,the effects and mechanism of reynosin on neuroinflammation remain elusive.The current study explores the effects and mechanisms of reynosin on neuroinflammation using mice and BV-2 microglial cells treated with lipopolysaccharide(LPS).Our findings reveal that reynosin effectively reduces microglial inflammation in vitro,as demonstrated by decreased CD11b expression and lowered interleukin-1 beta(IL-1β)and interleukin-18(IL-18)mRNA and protein levels.Correspondingly,in vivo,results showed a re-duction in the number of Iba-1 positive cells and alleviation of morphological alterations,alongside decreased expressions of IL-1βand IL-18.Further analysis indicates that reynosin inhibits NLRP3 inflammasome activation,evidenced by reduced transcription of NLRP3 and caspase-1,diminished NLRP3 protein expression,inhibited apoptosis-associated speck-like protein containing a CARD(ASC)oli-gomerization,and decreased caspase-1 self-cleavage.Additionally,reynosin curtailed the activation of nicotinamide adenine dinuc-leotide phosphate(NADPH)oxidase,demonstrated by reduced NADP^(+)and NADPH levels,downregulation of gp91^(phox) mRNA,pro-tein expression,suppression of p47^(phox) expression and translocation to the membrane.Moreover,reynosin exhibited a neuroprotective effect against microglial inflammation in vivo and in vitro.These collective findings underscore reynosin’s capacity to mitigate mi-croglial inflammation by inhibiting the NLRP3 inflammasome,thus highlighting its potential as a therapeutic agent for managing neuroinflammation.

关键词： Microglia NLRP3 inflammasome Reactive oxygen species NADPH oxidase Neuron Reynosin