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Smart crystalline frameworks constructed with bisquinoxaline-based component for multi-stimulus luminescent sensing materials

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Chinese Journal of Structural chemistry 2023年第2期42卷 9-22页

作者： Peng-Da Liu Ao-Gang Liu Peng-Min Wang Yuan Chen Bao Li key laboratory of material chemistry for Energy Conversion and Storage Semiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringHubei Key Laboratory of Bioinorganic Chemistry&Materia MedicaHuazhong University of Science and TechnologyWuhanHubei 430074People's Republic of China

Crystalline materials with well-defined structures and ordered molecular arrays can provide a new research platform to fabricate new smart materials with excellent stimulus response properties.Among them,Luminescent Metal-Organic Frameworks(LMOFs)and Hydrogen-bonding Organic Frameworks(HOFs)show great promise for fluorescence detection to different pollutants.In order to further extend the smart sensing frameworks and enhance the relevant sensing performance,the present work specifically selects 4,4',4",4(")-([6,6'-biquinoxaline]-2,2',3,3'-tetrayl)tetrabenzoic acid(H4L)consisting of the bisquinoxaline functional group as an optical response group,and HOF(HUST-25,HUST=Huazhong University of Science and Technology),Zn-MOF(HUST-26),and Cd-MOF(HUST-27)were successfully obtained.HOF could achieve the fluorescence recognition of Fe^(3+),MnO_(4)^(-),Cr_(2)O_(7)^(2-),p-nitrotoluene(4-NP),2,4,6-trinitrotoluene(TNP)and metronidazole(MDZ).The detection range of Zn-MOF constructed using Zn ions was similar to that of HOF,but the detection sensitivity of metal cations was significantly improved.Although Cd-MOF formed a six-fold interpenetrating structure,it was still able to retain a large pore structure.The dense stacking structure increases the quinoxaline density,which effectively expanded the sensitivity and detection range of fluorescence sensing.Therefore,Cd-MOF showed better detection for nitro explosives,antibiotics,and organic small molecules with ketone groups.For example,compared to the previous literatures,Cd-MOF has a larger Ksv value for the nitro-explosive nitrobenzene(NB),indicating the very high detection sensitivity.The series frameworks can present excellent sensing properties mainly because the func-tional primitives can be uniformly distributed in the skeleton of the crystalline materials,forming an ordered molecular array that enables the efficient energy transfer between the external stimulus signal and the response function sites.The related results indicate that the introduction of bisquinoxaline grou

关键词： Metal-organic framework Hydrogen bonding organic framework Luminescent sening Bisquinoxaline group Sensor

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Synthesis,crystal structure,and magnetic properties of a new onedimensional chain antiferromagnet Co(ox)(bib)·H_(2)O(ox=oxalate;bib=1,4-bis(imidazole-1-yl)benzene)

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Nano Research 2023年第2期16卷 3552-3557页

作者： Yan She Yanhong Wang Shuang Li Tao Wang Hongcheng Lu School of chemistry and Chemical Engineering Key Laboratory of Material Chemistry for Energy Conversion and StorageHubei Key Laboratory of Bioinorganic Chemistry&Materia MedicaHuazhong University of Science and TechnologyWuhan 430074China key laboratory of Solidification Processing School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China

A new one-dimensional(1D)chain antiferromagnet Co(ox)(bib)·H_(2)O 1(ox=oxalate;bib=1,4-bis(imidazole-1-yl)benzene)has been successfully synthesized under hydrothermal condition and characterized by single crystal X-ray crystallography,powder X-ray diffraction,thermogravimetric analysis,Fourier transform infrared(FTIR)spectroscopy,magnetic susceptibility,and heat capacity measurements.The CoII ion is connected by oxalate ions in trans-configuration to form 1D CoII–ox–CoII spin chains,which are further separated by the long organic molecule bib.The magnetic susceptibility curve shows that 1 exhibits a feature of broad maximum around 29 K,indicating strong antiferromagnetic interactions with short spin–spin correlations along the spin chains.However,no long-range order is observed due to the negligible interchain interactions through bib ligand and weak hydrogen bonds,which is further confirmed by the heat capacity data.The intrachain interaction J of−8.4 K is estimated.Both magnetic susceptibility and heat capacity results indicate that 1 exhibits a good 1D magnetism.

关键词： 1,4-bis(imidazole-1-yl)benzene antiferromagnetic cobalt chain structure oxalate

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Mechanism of water oxidation catalyzed by vitamin B_(12):Redox non-innocent nature of corrin ligand and crucial role of phosphate

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Chinese Chemical Letters 2022年第1期33卷 358-361页

作者： Ying-Ying Li Rong-Zhen Liao key laboratory of material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Bioinorganic Chemistry and Materia MedicaHubei Key Laboratory of Materials Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Vitamin B_(12)(macrocyclic cobalamin)has been recently reported to be capable of electrochemically catalyzing water oxidation in a neutral phosphate buffer solution.In this work,density functional calculations were employed to elucidate the water oxidation mechanism catalyzed by vitamin B_(12).The calculations showed that the catalytic cycle starts from the L·-Co^(Ⅱ)-OH_(2)complex 1.A proton-coupled electron transfer process then leads to the formation of a L^(·)-Co^(Ⅲ)-OH complex 2,followed by another proton-coupled electron transfer event to afford a corrin ligand radical cation intermediate 3(L^(·)-Co^(Ⅲ)-O^(·)).The redox non-innocent nature of the corrin ligand plays an essential role in the oxidation process.3 is capable of triggering the O-O bond formation via a water nucleophilic attack mechanism,in which a hydrophosphate dianion functions as a base to accept a proton from the water nucleophile.A dioxygen molecule is released after the oxidation of the Co^(Ⅲ)-OOH intermediate.The rate-determining step was calculated to be the O-O bond formation with a total barrier of 16.5 kcal/mol.While the use of water molecules as the proton acceptor was found to be less feasible for the O-O bond formation,with a barrier of 31.2 kcal/mol,further highlighting the crucial of phosphate in water oxidation.

关键词： Water oxidation DFT calculations Mechanism Vitamin B_(12) Cobalt

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An interlocked coordination cage based on aromatic amide ligands

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Chinese Chemical Letters 2021年第4期32卷 1397-1399页

作者： Dan Luo Bo Pan Jiajia Zhang Chunmiao Ma Yuyang Su Quan Gan hubei key laboratory of bioinorganic chemistry & materia medica School of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

An interlocked M_(4) L_(8) coordination cage was synthesized by coordination-driven self-assembly of palladium(Ⅱ)ions with aromatic amide bidentate ligands.The reaction of the ligand and the metal at 2:1 ratio led to the monomeric M_(2) L_(4) cage as the kinetic product,while the thermodynamic product M_(4) L_(8) cage was obtained by prolongating the reaction.This conve rsion and the interlocked structure was clearly revealed by using~1 H NMR,mass spectrometry and X-ray crystallography.The driving force of interlocking was mainly attributed to the interactions(hydrogen bonding,aromatic stacking and electrostatic interaction)arising from the aptitude of flexibility of the amide ligand.

关键词： Coordination cage Interlocked structure Self-assembly ingle-crystal structure Supramolecular chemistry

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Enzymes in Nanomedicine for Anti-tumor Therapy

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Chemical Research in Chinese Universities 2023年第1期39卷 72-82页

作者： ZHOU Tong YUAN Shuaiqi QIAN Pinrong WU Yuzhou 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 TechnologyWuhan430074P.R.China College of Life Science and Technology Huazhong University of Science and TechnologyWuhan430074P.R.China

Natural enzymes are biological macromolecules catalyzing reactions in living organisms and regulating biological processes.Targeted delivery of enzymes into tumor tissues for anti-tumor therapy through nanotechnology has attracted emerging interest in recent years.In this paper,we systematically summarize the latest research progress on enzymes that used for anti-tumor therapy in nanomedicine with different action mechanisms,including anti-tumor principles,delivery modes,response modes,and synergistic therapeutic design of these enzymes.Finally,we discuss the challenges and future prospects of enzymes for anti-tumor nanomedicine.

关键词： Enzyme Nanomedicine Protein delivery Cancer therapy

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Unveiling the Underlying Mechanism of Transition Metal Atoms Anchored Square Tetracyanoquinodimethane Monolayers as Electrocatalysts for N_(2) Fixation

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Energy & Environmental materials 2022年第2期5卷 533-542页

作者： Shengyao Lv Chunxiang Huang Guoliang Li Liming Yang hubei key laboratory of bioinorganic chemistry and materia medica Key Laboratory of Material Chemistry for Energy Conversion and StorageMinistry of EducationHubei Key Laboratory of Materials Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China key laboratory of Theoretical chemistry of Environment Ministry of EducationCenter for Computational Quantum ChemistrySchool of ChemistrySouth China Normal UniversityGuangzhou 510006China

We for the first time systematically studied the structures and electrochemical nitrogen reduction reaction properties of two-dimensional single transition-metal anchored square tetracyanoquinodimethane monolayers(labeled as:TM-sTCNQ,TM=3d,4d,5d series transition metals)by employing density functional theory method.Through highthroughput screenings and full reaction path researches,two promising electrochemical nitrogen reduction reaction catalysts Nb-sTCNQ and MosTCNQ have been obtained.The nitrogen reduction reaction onset potential on Nb-sTCNQ is as low as−0.48 V.Furthermore,the Nb-sTCNQ catalyst can quickly desorb NH3 produced with a free energy of 0.65 eV,giving Nb-sTCNQ excellent catalytic cycle performance.The high catalytic activity of the two materials might be attributed to the effective charge transfer between the active center and adsorbed N_(2),which enables the active center to adsorb and activate inert N_(2) molecules well,and the reduction processes require small energy input(i.e.,the maximum free energy changes are small).This work provides insights for finding highly efficient,stable,and low-cost nitrogen reduction reaction electrocatalysts.We hope our results can promote further experimental and theoretical research of this field.

关键词： 2D TM-sTCNQ monolayers density functional theory method electrochemical nitrogen reduction reaction high-throughput screening single-atom catalysts

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Single-atom catalysts based on two-dimensional metalloporphyrin monolayers for ammonia synthesis under ambient conditions

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Nano Research 2022年第5期15卷 4039-4047页

作者： Chun-Xiang Huang Sheng-Yao Lv Cong Li Bin Peng Guoliang Li Li-Ming Yang hubei key laboratory of bioinorganic chemistry and materia medica Key Laboratory of Material Chemistry for Energy Conversion and StorageMinistry of EducationHubei Key Laboratory of Materials Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China key laboratory of Theoretical chemistry of Environment Ministry of EducationCenter for Computational Quantum ChemistrySchool of ChemistrySouth China Normal UniversityGuangzhou 510006China

We systematically investigated the catalytic performance of 3d,4d,and 5d transition metals anchored onto two-dimensional extended porphyrin(PP)substrates as nitrogen reduction reaction(NRR)electrocatalysts,employing density functional theory(DFT)calculations and four-step high-throughput screening.Four novel metalloporphyrin(MPP,M=Zr,Nb,Hf,and Re)single-atom catalyst candidates have been identified due to their excellent catalytic performance(low onset potential,high stability,and selectivity).Through comprehensive reaction path search,the maximum Gibbs free energy changes for NRR on the ZrPP(enzymatic-consecutive hybrid path),NbPP(consecutive path),HfPP(enzymatic-consecutive hybrid path),and RePP(distal path)catalysts are 0.38,0.41,0.53,and 0.53 eV,respectively.Band structures,projected density of states,and charge/spin distributions show that the high catalytic activity is due to significant orbital hybridizations and charge transfer between N_(2) and MPP catalysts.We hope our work will promote experimental synthesis of these NRR electrocatalysts and provide new opportunities to the electrochemical conversion of N_(2) to NH_(3) under ambient conditions.

关键词： electrocatalytic nitrogen reduction reaction two-dimensional(2D)extended metalloporphyrin(MPP)monolayer singleatom catalyst two-dimensional materials high-throughput screening first-principles calculations

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Neutral Five-Coordinate Arylated Copper(Ⅲ) Complex: key Intermediate in Copper-Mediated Arene Trifluoromethylation

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Chinese Journal of chemistry 2022年第16期40卷 1924-1930页

作者： Guangyu Wang Man Li Xuebing Leng Xiaosong Xue Qilong Shen key laboratory of Organofluorine chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling LuShanghai200032 China key laboratory of material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Bioinorganic Chemistry and Materia MedicaHubei Key Laboratory of Materials Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong Universityof Scienceand TechnologyWuhanHubei 430074China

Five-coordinate neutral Cu(Ⅲ)complexes have long been considered as the key intermediates in copper-mediated/catalyzed arene trifluoromethylative reactions,but the identity of these complexes remains elusive.Herein,we reported,for the first time,the preparation and characterization of these putative complexes[(bpy)Cu(CF_(3))_(2)(C_(6)F_(4)R)]and investigation of their C(sp^(2))-CF_(3) bond-forming reductive elimination.Our mechanistic studies including kinetic studies,the effect of temperature and solvents,the effect of the para-substitution of the ligand as well as DFT calculations suggest that C(sp^(2))-CF_(3) reductive elimination process proceeds via synchronous bond-breaking/bond-forming process.

关键词： Cu(Ⅲ) Reductive elimination Trifluoromethyl Mechanism Concerted pathway

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A smart photodynamic therapy strategy: depletion of glutathione in cancer cells

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Science Bulletin 2017年第5期62卷 312-313页

作者： Fujian Huang Fan Xia Faculty of material Science and chemistry China University of Geosciences hubei key laboratory of bioinorganic chemistry & materia medica School of Chemistry and Chemical EngineeringHuazhong University of Science and Technology

Photodynamic therapy(PDT)is a promising cancer treatment method with fewer side effects,minimal invasion and low toxicity compared with other traditional cancer therapy methods,such as radiotherapy,chemotherapy and su... 详细信息

关键词： PDT depletion of glutathione in cancer cells A smart photodynamic therapy strategy

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一种新型准一维反铁磁体CoF2（H2O）2（pyrazine）的制备与表征（英文）

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Science China materials 2019年第12期62卷 1815-1820页

作者：王艳红刘航符鹏卢红成 key laboratory of material chemistry for Energy Conversion and Storage School of Chemistry and Chemical Engineering Hubei Key Laboratory of Bioinorganic Chemistry & Materia Medica Hubei Key Laboratory of Material Chemistry and Service Failure Huazhong University of Science and Technology

本文通过水热法成功合成出了一种新型一维反铁磁性的过渡金属杂化氟化物CoF2(H2O)2(pyz)(pyz=吡嗪)及其两种新同构体MF2(H2O)2(pyz)(M=Ni^2+, Zn^2+).通过单晶X射线衍射方法解析出它们的晶体结构都属于相同的空间群C2/m.并且对化合物1Co... 详细信息

本文通过水热法成功合成出了一种新型一维反铁磁性的过渡金属杂化氟化物CoF2(H2O)2(pyz)(pyz=吡嗪)及其两种新同构体MF2(H2O)2(pyz)(M=Ni^2+, Zn^2+).通过单晶X射线衍射方法解析出它们的晶体结构都属于相同的空间群C2/m.并且对化合物1CoF2(H2O)2(pyz)的磁性进行了测试和讨论. Weiss常数为-20.6 K,表明化合物1中主要存在显著的反铁磁性交换作用.同时,大约为5.66μB的有效磁矩说明化合物1中有较大未遏制的轨道磁矩贡献和各向异性.由于强量子涨落的阻止作用,当温度低于2.9 K时,准一维反铁磁体1才呈现出长程磁有序,这表明其具有良好的一维磁性.

关键词：单晶X射线衍射反铁磁性过渡金属反铁磁体有效磁矩轨道磁矩量子涨落准一维

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