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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 *** 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 *** 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 ***,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 *** intrachain interaction J of−8.4 K is *** 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

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 *** them,Luminescent Metal-Organic Frameworks(LMOFs)and Hydrogen-bonding Organic Frameworks(HOFs)show great promise for fluorescence detection to different *** 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 *** 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 *** Cd-MOF formed a six-fold interpenetrating structure,it was still able to retain a large pore *** dense stacking structure increases the quinoxaline density,which effectively expanded the sensitivity and detection range of fluorescence ***,Cd-MOF showed better detection for nitro explosives,antibiotics,and organic small molecules with ketone *** example,compared to the previous literatures,Cd-MOF has a larger Ksv value for the nitro-explosive nitrobenzene(NB),indicating the very high detection *** 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 *** related results indic

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

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 *** 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,*** 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 *** 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

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 *** highthroughput screenings and full reaction path researches,two promising electrochemical nitrogen reduction reaction catalysts Nb-sTCNQ and MosTCNQ have been *** nitrogen reduction reaction onset potential on Nb-sTCNQ is as low as−0.48 ***,the Nb-sTCNQ catalyst can quickly desorb NH3 produced with a free energy of 0.65 eV,giving Nb-sTCNQ excellent catalytic cycle *** 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 *** 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

An AIEgens and exonuclease Ⅲ aided quadratic amplification assay for detecting and cellular imaging of telomerase activity

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Science Bulletin 2017年第14期62卷 997-1003页

作者： Xuehong Min Lei Xia Yuan Zhuang Xudong Wang Jie Du Xiaojin Zhang Xiaoding Lou Fan Xia hubei key laboratory of bioinorganic chemistry & materia medica School of Chemistry and Chemical Engineering Huazhong University of Science and Technology College of materials and chemistry Engineering Hainan University Faculty of material Science and chemistry China University of Geosciences Shenzhen Institute of Huazhong University of Science & Technology

Monitoring telomerase activity with high sensitive and reliable is of great importance to cancer analysis. In this paper, we report a sensitive and facile method to detect telomerase activity using AIEgens mod- ified probe （TPE-Py-DNA） as a fluorescence reporter and exonuclease llI （Exo lIl） as a signal amplifier. With the aid of telomerase, repeat units （TrAGGG）n are extended from the end of template substrate oligonucleotides （TS primer） that form duplex DNAs with TPE-Py-DNA. Then, Exo llI catalyzes the diges- tion of duplex DNAs, liberating elongation product and releasing hydrophobic TPE-Py. The released hydrophobic TPE-Py aggregate together and produce a telomerase-activity-related fluorescence signal. The liberated product hybridizes with another TPE-Py-DNA probe, starting the second cycle. Finally, we obtain the target-to-signal amplification ratio of 1 ：N2. This strategy exhibits good performance for detecting clinical urine samples （distinguishing 15 cancer patients＇ samples from 8 healthy ones） and checking intracellular telomerase activity （differentiating cell lines including HeLa, MDA-MB-231, MCF-7, A375, HLF and MRC-5 from the cells pretreated with telomerase-related drug）, which shows its potential in clinical diagnosis as well as therapeutic monitoring of cancer.

关键词： Quadratic amplification AIEgens Telomerase Urine samples Exonuclease Ill Cell imaging

DNA hybridization chain reaction and DNA supersandwich self-assembly for ultrasensitive detection

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Science China chemistry 2017年第3期60卷 311-318页

作者： Nannan Liu Fujian Huang Xiaoding Lou Fan Xia key laboratory of Carbon materials of Zhejiang Province College of Chemistry & Materials EngineeringWenzhou UniversityWenzhou 325027China hubei key laboratory of bioinorganic chemistry & materia medica School of Chemistry and Chemical EngineeringHuazhong University of Science and Technology CAS key laboratory of Soft Matter chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of China

The fabrication of sensitive sensors with high selectivity is highly desirable for the detection of some important biomarkers,such as nucleic acids,proteins,small molecules and *** hybridization chain reaction(HCR) and DNA supersandwich self-assembly(SSA) are two prevalent enzyme-free signal amplification strategies to improve sensitivity of the *** this review,we firstly describe the characteristics about DNA HCR and DNA SSA,and then summarize the advances in the one-dimensional DNA nanostructures assisted by HCR and *** review has been divided into three parts according to the two signal amplification methods and highlights recent progress in these two strategies to improve the detection sensitivity of proteins,nucleic acids,small molecules and ions.

关键词： signal amplification method hybridization chain reaction supersandwich self-assembly ultrasensitive detection

Recent advances in optical-based and force-based single nucleic acid imaging

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Science China chemistry 2017年第10期60卷 1267-1276页

作者： Shenshan Zhan Xiaoding Lou Fan Xia hubei key laboratory of bioinorganic chemistry & materia medica School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 China Faculty of material Science and chemistry China University of Geosciences Wuhan 430074 China Shenzhen Institute of Huazhong University of Science and Technology Shenzhen 518000 China

The capability to image, as well as control and manipulate single molecules such as nucleic acids(DNA or RNA) can greatly enrich our knowledge of the roles of individual biomolecules in cellular processes and their behavior in native environments. Here we summarize the recent advances of single nucleic acid imaging based on optical observation and force manipulation. We start by discussing the superiority of single molecule image, the central roles nucleic acids play in biosystems, and the significance of single molecule image towards nucleic acids. We then list a series of representative examples in brief to illustrate how nucleic acid of various morphologies has been imaged from different aspects, and what can be learned from such characterizations. Finally,concluding remarks on parts of which should be improved and outlook are outlined.

关键词： single nucleic acid imaging optical-based observation force-based manipulation fluorescent imaging atomic force microscopy

Composition Engineering Opens an Avenue Toward Efficient and Sustainable Nitrogen Fixation

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Energy & Environmental materials 2024年第1期7卷 313-325页

作者： Xiaolin Wang Liming Yang key laboratory of material chemistry for Energy Conversion and Storage Ministry of EducationWuhan 430074China hubei key laboratory of materials chemistry and Service Failure Wuhan 430074China hubei key laboratory of bioinorganic chemistry and materia medica Wuhan 430074China hubei Engineering Research Center for Biomaterials and medical Protective materials Wuhan 430074China School of chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074China

In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active sites as exemplified by diatomic metals anchored graphdiyne via the combination of hierarchical high-throughput screening,first-principles calculations,and molecular dynamics *** 43 highly efficient catalysts feature ultralow onset potentials(|U_(onset)|≤0.40 V)with Rh-Hf and Rh-Ta showing negligible onset potentials of 0 and-0.04 V,*** high catalytic activities of Rh-Hf and Rh-Ta can be ascribed to the synergistic *** forming heteronuclears,the combinations of relatively weak(such as Rh)and relatively strong(such as Hf or Ta)components usually lead to the optimal strengths of adsorption Gibbs free energies of reaction *** origin can be ascribed to the mediate d-band centers of Rh-Hf and Rh-Ta,which lead to the optimal adsorption strengths of intermediates,thereby bringing the high catalytic *** work provides a new and general strategy toward the architecture of highly efficient catalysts not only for electrocatalytic nitrogen reduction reaction(eNRR)but also for other important *** expect that our work will boost both experimental and theoretical efforts in this direction.

关键词： composition engineering strategy diatomic catalysts electrocatalytic nitrogen reduction reaction first-principles calculations graphdiyne hierarchical high-throughput screening synergistic effects

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 ***,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 *** 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

Decarboxylative cyanation and thiocyanation via catalytic electron donor-acceptor complex with copper catalysis

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Science China chemistry 2024年第9期67卷 3019-3028页

作者： Hongping Zhao Xiaoxiang Xi Tianbao Wu Zimin Chen Minyan Wang Weiming Yuan key laboratory of material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Bioinorganic Chemistry and Materia MedicaSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074China State key laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China Shenzhen Huazhong University of Science and Technology Research Institute Shenzhen 518000China

A new catalytic decarboxylative cyanation and thiocyanation via a synergistic Na I/Cu catalysis is *** photoexcited electron donor-acceptor complex by assembly of Na I,R3P,and N-acyloxy-phthalimide ester(NHPI ester)triggers the generation of alkyl radical species,which then engages in Cu-catalyzed radical coupling *** to success of this dual catalytic transformation is the reliable charge transfer between I·and Cu(I).This dual catalytic platform can eliminate the use of expensive iridium-based photocatalyst or synthetically elaborate organic dyes.A series of primary,secondary,and tertiary alkyl nitriles and thiocyanates are easily ***,an asymmetric decarboxylative cyanation by applying a chiral Cu catalyst is also developed to afford chiral nitriles in high *** mechanistic details and the origin of the high enantioselectivity are further investigated by the mechanistic experiments and the density functional theory calculations.

关键词： electron donor-acceptor catalysis copper catalysis cyanation thiocyanation asymmetric synthesis