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Flexibility of Metal-Organic Framework Tunable by Crystal Size at the Micrometer to Submillimeter Scale for Efficient Xylene Isomer Separation

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Research 2019年第1期2019卷 433-441页

作者： Xiao Yang Hao-Long Zhou Chun-Ting He Zong-Wen Mo Jia-Wen Ye Xiao-Ming Chen Jie-Peng Zhang moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Understanding,controlling,and utilizing the flexibility of adsorbents are of great importance and difficulty.Analogous with conventional solid materials,downsizing to the nanoscale is emerging as a possible strategy for controlling the flexibility of porous coordination polymers(or metal-organic frameworks).We report a unique flexibility controllable by crystal size at the micrometer to submillimeter scale.Template removal transforms[Cu_(2)(pypz)_(2)]·0.5p-xylene(MAF-36,Hpypz=4-(1H-pyrazol-4-yl)pyridine)with one-dimensional channels toα-[Cu_(2)(pypz)_(2)]with discrete small cavities,and further heating gives a nonporous isomerβ-[Cu_(2)(pypz)_(2)].Both isomers can adsorb p-xylene to give[Cu_(2)(pypz)_(2)]·0.5p-xylene,meaning the coexistence of guest-driven flexibility and shape-memory behavior.The phase transition temperature fromα-[Cu_(2)(pypz)_(2)]toβ-[Cu_(2)(pypz)_(2)]decreased from~270℃ to~150℃ by increasing the crystal size from the micrometer to the submillimeter scale,ca.2-3 orders larger than those of other size-dependent behaviors.Single-crystal X-ray diffraction showed coordination bond reconstitution and chirality inversion mechanisms for the phase transition,which provides a sufficiently high energy barrier to stabilize the metastable phase without the need of downsizing to the nanoscale.By virtue of the crystalline molecular imprinting and gate-opening effects,α-[Cu_(2)(pypz)_(2)]andβ-[Cu_(2)(pypz)_(2)]show unprecedentedly high p-xylene selectivities of 16 and 51,respectively,as well as ultrafast adsorption kinetics(<2 minutes),for xylene isomers.

关键词： isomers coordination adsorbent

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构建三元WO_(3)/CsPbBr_(3)/ZIF-67异质结用于高效光催化CO_(2)还原

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Science China Materials 2022年第6期65卷 1550-1559页

作者：董玉杰江勇廖金凤陈洪燕匡代彬苏成勇 moe key laboratory of bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510006China

近年来,卤素钙钛矿纳米材料以其优异的光电性能在光催化等领域引起了关注.然而,光生载流子严重的复合反应和较差的反应动力学也极大地限制了其光催化性能.本论文设计合成了一种三元WO_(3)/CsPbBr_(3)/ZIF-67异质光催化剂,并将其应用于... 详细信息

近年来,卤素钙钛矿纳米材料以其优异的光电性能在光催化等领域引起了关注.然而,光生载流子严重的复合反应和较差的反应动力学也极大地限制了其光催化性能.本论文设计合成了一种三元WO_(3)/CsPbBr_(3)/ZIF-67异质光催化剂,并将其应用于有效的CO_(2)光还原反应.研究表明,WO_(3)与CsPbBr_(3)之间构建的Z型电荷转移路径能够保证光生载流子的有效转移和分离.此外,在表面修饰具有活性Co中心的ZIF-67壳层作为助催化剂有利于改善复合材料的CO_(2)的吸附和活化能力.因此,电荷分离和CO_(2)吸附性能的增强大大提高了WO_(3)/CsPbBr_(3)/ZIF-67的光催化活性,还原产物中CO产率达到99.38μmol g_(−1),是单一CsPbBr_(3)的6.8倍.这项工作有望为开发高效的卤素钙钛矿基光催化剂及其在CO_(2)还原和其他复杂光催化反应中的应用提供参考.

关键词： Z-scheme heterojunction halide perovskite CO_(2)photoreduction heterostructure charge separation

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Modulating hydrothermal condition to achieve carbon dots-zeolite composites with multicolor afterglow

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Nano Research 2023年第5期16卷 7761-7769页

作者： Jiali Wen Zhifeng Zeng Bolun Wang Junyu Hong Yingyuan Chen Jianyu Zhang Jiyang Li Jiuxing Jiang moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510006China State key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Department of chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and ReconstructionThe Hong Kong University of Science and TechnologyKowloonHong Kong 999077China Guangdong Provincial key laboratory of Optical Chemicals XinHuaYue GroupMaoming 525000China

Responsive luminescence materials with prolonged lifetime and multicolor emission have drawn great attention due to their attractive optical property and potential applications.Herein,two responsive carbon dots(CDs)based composites:CD_(1)@MCM-22P and CD_(2)@ZSM-12 were achieved by a one-step hydrothermal method.By adjusting the hydrothermal condition,CD_(1)@MCM-22P owns temperature-dependent afterglow,while CD_(2)@ZSM-12 is equipped with excitation-dependent room-temperature phosphorescence.The photoluminescence mechanisms of CD1@MCM-22P and CD_(2)@ZSM-12 were investigated and proposed,and the composites were applied in multi-mode anti-counterfeiting.This work provides an insight as well as a feasible method for the development of multi-emissive CDs@zeolite composite.

关键词： carbon dots zeolitic matrices responsive photoluminescence room-temperature phosphorescence thermally activated delayed fluorescence

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Construction of cobalt vacancies in cobalt telluride to induce fast ionic/electronic diffusion kinetics for lithium-ion half/full batteries

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Journal of Materials Science & Technology 2022年第32期127卷 124-132页

作者： Lei Hu Lin Li Yuyang Zhang Xiaohong Tan Hao Yang Xiaoming Lin Yexiang Tong Anhui laboratory of Functional Coordinated Complexes for Materials chemistry and Application School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000China moe of the key laboratory of bioinorganic and synthetic chemistry The Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong ProvinceSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China Guangxi key laboratory of Electrochemical Energy Materials School of Chemistry&Chemical EngineeringGuangxi UniversityNanning 530004China key laboratory of Theoretical chemistry of Environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006China

Designing novel electrode materials with unique structures is of great significance for improving the performance of lithium ion batteries(LIBs).Herein,copper-doped Co_(1-x)Te@nitrogen-doped carbon hollow nanoboxes(Cu-Co_(1-x)Te@NC HNBs)have been fabricated by chemical etching of Cu Co-ZIF nanoboxes,followed by a successive high-temperature tellurization process.The as-synthesized Cu-Co_(1-x)Te@NC HNBs composite demonstrated faster ionic and electronic diffusion kinetics than the pristine Co Te@NC HNBs electrode.The existence of Co-vacancy promotes the reduction of Gibbs free energy change(ΔG_(H^(*)))and effectively improves the Li~+diffusion coefficient.XPS and theoretical calculations show that performance improvement is ascribed to the electronic interactions between Cu-Co_(1-x)Te and nitrogen-doped carbon(NC)that trigger the shift of the p-band towards facilitation of interfacial charge transfer,which in turn helps boost up the lithium storage property.Besides,the proposed Cu-doping-induced Co-vacancy strategy can also be extended to other conversion-type cobalt-based material(CoSe_(2))in addition to asobtained Cu-Co_(1-x)Se_(2)@NC HNBs anodes for long-life and high-capacity LIBs.More importantly,the fabricated LiCoO_(2)//Cu-Co_(1-x)Te@NC HNBs full cell exhibits a high energy density of 403 Wh kg^(-1)and a power density of 6000 W kg^(-1).We show that the energy/power density reported herein is higher than that of previously studied cobalt-based anodes,indicating the potential application of Cu-Co_(1-x)Te@NC HNBs as a superior electrode material for LIBs.

关键词： MOF-derived material Cobalt telluride Cobalt vacancy Diffusion kinetics Lithium storage

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Spherical lanthanide nanoclusters toward white-light emission and cell membrane imaging

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Nano Research 2023年第8期16卷 11495-11502页

作者： Hai-Ling Wang Zhiqiang Ni Ze-Yu Ruan Zhong-Hong Zhu Pei-Yu Liao Guangxue Feng Jian-Hua Jia Ming-Liang Tong key laboratory of bioinorganic and synthetic chemistry of Ministry of Education School of ChemistrySun Yat-Sen UniversityGuangzhou 510006China State key laboratory of Luminescent Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesSchool of Materials Science and EngineeringSouth China University of TechnologyGuangzhou 510640China

Lanthanide doping is an effective strategy for modulating the emission of emitters.Herein,by changing the cluster composition to control the energy transfer pathway,the application potential of high-nuclearity lanthanide cluster(HLC)as white-light emitter has been confirmed for the first time.Specifically,by precisely controlling the proportion of GdIII,TbIII,and EuIII ions in reactants,we obtained a spherical heterotrimetallic nanocluster Gd_(10)Tb_(12)Eu_(10),a white-light emitter with quantum yield(QY)of 12.58%and lifetime of 327.14μs.High-resolution electrospray ionization mass spectrometry(HRESI-MS)demonstrates that homometallic nanoclusters Ln_(32)(Ln=Gd,Tb,and Eu)are tetracationic clusters and are highly stable in solution.The peripheral dense organic ligands provide a protective layer for the cluster core,which improves the stability of Ln_(32) in aqueous solution,avoids the contact between metal centers and bioactive molecules,and greatly reduces the biological toxicity.In cell imaging experiments,cationic clusters Ln_(32) are mainly localized on the cell membrane with negative charge distribution.As far as we know,this is the first time that spherical lanthanide nanoclusters have been used for membrane imaging of living cell,opening the door for the application of HLCs in biological imaging.

关键词： spherical lanthanide clusters white-light emission high stability low toxicity cell membrane imaging

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Te^(4+)掺杂Cs_(2)InCl_(5)·H_(2)O单晶的光学测温应用

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Science China Materials 2022年第3期65卷 764-772页

作者：魏俊华罗健彬廖金凤区维韬匡代彬 moe key laboratory of bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China

本文设计合成了一种Te^(4+)离子掺杂的Cs_(2)InCl_(5)·H_(2)O单晶,该单晶在紫外光激发下发射明亮橙光.未掺杂的Cs_(2)InCl_(5)·H_(2)O单晶几乎没有发光现象,但Te^(4+)掺杂的Cs_(2)InCl_(5)·H_(2)O单晶,发射峰位于660 nm,并伴随着大的Stokes位移和宽的发光半峰宽(180 nm).结合变温荧光光谱以及飞秒瞬态吸收光谱等表征,揭示了其发光机理为自陷激子发光.零维结构中的强电声耦合以及软晶格有利于形成并稳定自陷激子.特别地,由于Te^(4+)离子的最外层电子结构为5s^(2),对温度变化较为灵敏,Te^(4+)离子掺杂的Cs_(2)InCl_(5)·H_(2)O单晶的发光寿命表现出了非常强的温度依赖性,发光寿命从80 K下的6μs缩短至380 K下的19 ns,320 K处的相对灵敏度达到0.062 K^(-1),可以与传统稀土基光学测温材料相媲美.据我们所知,这是首次将铟基金属卤化物钙钛矿单晶应用于光学测温,将为设计合成新型多功能响应的金属卤化物钙钛矿发光材料提供借鉴意义.

关键词：金属卤化物温度依赖性相对灵敏度发光现象发光材料紫外光激发设计合成离子掺杂

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一例具有高低温双铁弹性的新型杂化晶体:(Me_(3)NCH_(2)CH_(2)OH)_(4)[Ni(NCS)_(6)]

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Science China Materials 2022年第1期65卷 263-267页

作者：刘德轩陈晓娴叶子铭张伟雄陈小明 moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

本文报道了一例具有反XeF4结构的新型杂化晶体(Me_(3)NCH_(2)-CH_(2)OH)_(4)[Ni(NCS)_(6)],其分子组分的较复杂有序-无序转变使得该化合物在269和360 K发生两步可逆相变.这两步相变伴随着P2_(1)/n-P4/mnc-Bmab的空间群变化,即分别属于... 详细信息

本文报道了一例具有反XeF4结构的新型杂化晶体(Me_(3)NCH_(2)-CH_(2)OH)_(4)[Ni(NCS)_(6)],其分子组分的较复杂有序-无序转变使得该化合物在269和360 K发生两步可逆相变.这两步相变伴随着P2_(1)/n-P4/mnc-Bmab的空间群变化,即分别属于正常的降温对称性破缺和反常的升温对称性破缺现象,因此使得该化合物可在低温和高温均展现出铁弹性(自发极化强度分别为0.0603和0.0073).这种不同寻常的高低温双铁弹性的发现和研究,有助于加深对反常对称性破缺相变的理解,并为今后在分子杂化晶体中探索高温铁性材料提供重要线索.

关键词：对称性破缺可逆相变铁弹性高低温杂化 NCS

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Partial Order-Disorder Transformation of Interpenetrated Porous Coordination Polymers

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CCS chemistry 2022年第5期4卷 1587-1596页

作者： Yun Li Xin-Yi Cao Kai Zheng Xue-Wen Zhang Dong-Dong Zhou Wei-Xiong Zhang Xiao-Ming Chen Jie-Peng Zhang moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510275 key laboratory of Coal to Ethylene Glycol and Its Related Technology Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002

Controlling interpenetration and flexibility behaviors is intriguing and fundamental for porous coordination polymers.We report exceptional interpenetration behaviors involving controllable partial order–disorder structural transformations.A new bis-benzotriazolate ligand(NaH2sbbta)with a twisted and anionic backbone was designed and synthesized.The solvothermal reaction of ZnCl_(2) and NaH_(2)sbbta yielded(Et_(2)NH_(2))_(3)[Zn_(5)Cl_(4)(sbbta)_(3)]·6DEF(2)possessing two-fold interpenetrated anionic pcu networks with symmetry,shape,and charge different from the known analogues.More interestingly,powder and single-crystal X-ray diffractions showed that 2 can undergo solvent-induced structural transformation to form a noninterpenetrated anionic pcu network with larger pores(1).Consequently,1/2 can selectively adsorb/exchange cationic dyes fromneutral and anionic dyes with tunable size selectivity.However,since the transformations are reversible without obvious change of crystal sizes,the network that disappeared in X-ray crystallography should be mainly disordered rather than decomposed.Further,the structural transformations can be suppressed by thermal decomposition/removal of Et_(2)NH_(2)^(+)/Et_(2)NH.Computational simulations indicate that the ordered and disordered structures are stabilized by relatively large and small solvent molecules,respectively.

关键词： order disorder interpenetration crystalto-crystal structural transformation dye adsorption and separation

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Genomic and transcriptional changes in response to pinene tolerance and overproduction in evolved Escherichia coli

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synthetic and Systems Biotechnology 2019年第3期4卷 113-119页

作者： Fu-Xing Niu Yuan-Bin Huang Liang-Nian Ji Jian-Zhong Liu Institute of synthetic Biology MOE Key Laboratory of Bioinorganic and Synthetic ChemistrySchool of Life SciencesSun Yat-Sen UniversityGuangzhou 510275China

α-Pinene is an important monoterpene,which is widely used as a flavoring agent and in fragrances,pharmaceuticals and biofuels.Although an evolved strain Escherichia coli YZFP,which had higher tolerance to pinene and titer,has been successfully used to produce high levels of pinene,the pinene titer is much lower than that of hemiterpene(isoprene)and sesquiterpenes(farnesene)to date.Moreover,the overall cellular physiological and metabolic changes caused by higher tolerance to pinene and overproduction of pinene remains unclear.To reveal the mechanism of Escherichia coli YZFP with the higher tolerance to pinene and titer,a comparative genomics and transcriptional level analyses combining with CRISPR activation(CRISPRa)and interference(CRISPRi)were carried out.The results show that the tolerance to pinene and the overproduction of pinene in E.coli may be associated with:1)the mutations of the DXP pathway genes,the rpoA and some membrane protein genes,and their upregulations of transcription levels;and 2)the mutations of some genes and their downregulation of transcriptional levels.These comparative omics analyses provided some genetic modification strategies to further improve pinene production.Overexpression of the mutated cbpA,tabA,pitA,rpoA,sufBCDS,mutS,ispH,oppF,dusB,dnaK,dxs,dxr and flgFGH genes further improved pinene production.This study also demonstrated that combining comparative omics analysis with CRISPRa and CRISPRi is an efficient technology to quickly find a new metabolic engineering strategy.

关键词： Comparative omics analysis CRISPRa CRISPRi Pinene Escherichia coli Biosynthesis

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Mild metal-organic-gel route for synthesis of stable sub-5-nm metal-organic framework nanocrystals

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Nano Research 2017年第11期10卷 3621-3628页

作者： Yue Qi Chun-Ting He Juntao Lin Shuping Lin Jin Liu Jinghong Huang Wei Xue Guicheng Yu Hsiu-Yi Chao Yexiang Tong Zhengping Qiao moe key laboratory of bioinorganic and synthetic chemistry School of Chemistry Sun Yat-Sen University Guangzhou 510275 China

Nanoscale metal-organic frameworks （NMOFs） have attracted increased attention in recent years for miniaturized and/or biological applications.However,the synthesis of ultrasmall NMOFs with good stability is a great challenge.In this study,sub-5-nm nano-HKUST-1 was prepared for the first time via a mild metalorganic gel route without surfactants or capping agents.Controlling the gelation process via anion-ligand self-assembly is the key to the formation of NMOFs.The Tyndall effect,zeta potential,and liquid adsorption indicated strong stability of the obtained nano-HKUST-1,even in water.Adsorption experiments were performed using different dyes （crystal violet and methylene blue） to demonstrate the size-dependent adsorption thermodynamics and kinetics of this famous MOF.The results of this study provide new insights regarding the synthesis of NMOFs and their efficient applications.

关键词： metal-orgamc gel metal-organic frameworks nanoparticles,liquid adsorption

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