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Nano Research 2024年第7期17卷 5914-5921页

作者： Chun-Ying Chen Qi-Jie Mo Fu-Zhen Li Hai-Li Song Li Zhang MOE Laboratory of Bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510006China

Alkene hydrosilylation is one of the most concise and atom-economical methods to synthesize organosilicon ***,we reported the precise immobilization of metal single atoms(M-SAs;M=Ru,Rh,Ir,Pd,Pt,and Au)into a porphyrinic metalorganic framework(MOF)of PCN-222(PCN=porous coordination network),and then applied the resultant MOF composites of M-SAs@PCN-222 to alkene *** solvent-free conditions,Pt-SAs@PCN-222 displayed an especially high catalytic efficiency with the turnover frequency up to 119 s−1 and the maximum turnover number of 906,250 at room *** and theoretical studies revealed that there existed strong interactions between Pt-SAs@PCN-222 and the substrates,which helped to condense the substrates in the cavities of the porous *** density functional theory calculations and molecular dynamics simulations disclosed that PCN-222 could transfer electrons to Pt-SAs to enhance the silane oxidative addition and drive the reaction to proceed smoothly via Chalk–Harrod pathway.

关键词： alkene hydrosilylation single atom catalysts metal-organic frameworks precision chemistry synergistic catalysis

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

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 ***,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 *** importantly,the light-induced stepped thermal relaxation(LISTR)with obvious magnetic plateau for a hidden intermediate spin state is firstly *** 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 ***,five spin states can be captured in 1·coumarin and the tristability can be modulated below 102 K through the excitation-relaxation ***,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

Engineering a high-barrier d-f single-molecule magnet centered with hexagonal bipyramidal Dy(Ⅲ) unit

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Science China chemistry 2024年第10期67卷 3291-3298页

作者： Wei Deng Chan-Ying Yao Yan-Cong Chen Ying-Qian Zhou Shan-Nan Du Jun-Liang Liu 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 University

In the pursuit of high-performance single-molecule magnets（SMMs）,incorporating intramolecular magnetic coupling emerges as a pivotal *** these,d-f SMMs have garnered significant attention due to their remarkable versatility,which lies in their ability to tune coordination environments and facilely substitute metal ***,achieving performance-centric d-f SMMs through the synergistic interplay between highly anisotropic f ions and d-f magnetic interactions remains a formidable *** mononuclear hexagonal bipyramidal(D6h) DyⅢSMMs have been successfully isolated,the exploration of d-f SMMs featuring D6h-lanthanide metal centers remains uncharted *** this study,we employed planar bipodal ligands in conjunction with “staple-like” axial phenoxide ligands to synthesize the first hexagonal bipyramidal d-f ***,this compound exhibits alternating-current magnetic susceptibilities peaking up to 68 K with an energy barrier surpassing 1,200 K,thus establishing a new benchmark within the heterometallic d-f SMM landscape inclusive of complexes with diamagnetic d metals and paramagnetic f ***,the ferromagnetic interaction at the d-f sites engenders oscillating relaxation times contingent on the magnetic field—a characteristic distinct from mononuclear *** findings shed light on a deliberate design approach for d-f SMMs,emphasizing the cooperative utilization of high-barrier lanthanide modules alongside d ions through magnetic *** synergy significantly enhances and diversifies the magnetic dynamics of these intriguing molecular systems.

关键词： single-molecule magnets magnetic coupling crystal engineering hexagonal bipyramid energy barrier

Polyelectrolytes of Inorganic Polyoxometalates:Prospecting New Charged Polymers for Advanced Applications

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Chinese Journal of Polymer Science 2024年第9期42卷 1254-1269,I0005页

作者： De-Yin Wang Zhuo-Qun Lu Wei Wang College of Medical Linyi UniversityLinyi276000China center for synthetic Soft Materials Key Laboratory of Functional Polymer Materials of the Ministry of EducationInstitute of Polymer ChemistryNankai UniversityTianjin300071China

Polyelectrolytes are charged polymers comprising macromolecules in which substantial portions of the constituent units contain cationic(e.g.,pyridinium,ammonium)or anionic(e.g.,sulfonate,carboxylate)groups,which possess special functions from the features of counterions,such as dissociation to charged species,mechanical stability,phase behavior,***,functional polyelectrolytes have been widely applied in many *** this perspective,we present some progresses in the studies of poly(polyoxometalate)s,denoted as poly(POM)s,as a kind of new charged polymers/polyelectrolytes,by covalent bonding between the inorganic polyoxometalate(POM)clusters and the organic polymer *** to the distinct positions of POMs in polymer chain and functions of poly(POM)s,they are divided into the following four categories:crosslinked poly(POM);side-chain poly(POM);backbone poly(POM),including poly(POM)-conjugated polymer hybrid and block poly(POM)-polymer;and POM-based covalent organic framework(PCOF).This perspective introduces the synthesis methods of poly(POM)polyelectrolytes and their macromolecular and aggregate structural characteristics,while also focusing on their properties and *** application areas include catalysis,thermal resistance,optical functions,fuel cells and batteries,etc.

关键词： Charged polymer Polyelectrolyte Polyoxometalate Poly(polyoxometalate) Covalent organic framework

DDX21 is a new player in co-transcriptional RNA modification and functions

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Science China Life Sciences 2024年第10期67卷 2291-2293页

作者： Chengqi Yi State Key Laboratory of Protein and Plant Gene Research School of Life SciencesPeking University Peking-Tsinghua center for Life Sciences Peking University Department of Chemical Biology and synthetic and functional biomolecules center College of Chemistry and Molecular EngineeringPeking University Beijing Advanced center of RNA Biology (BEACON) Peking University

Ever since the first discovery of chemical modifications of RNA in 1951,researchers have been captivated by the diverse types of modifications,their associated enzymes and proteins（writers,erasers,or readers）,and their downstream functional implications（Song and Yi,2017）.Among the over 170 distinct types of RNA modifications identified thus far,N6-methyladenosine（m6A） stands out as the most prevalent internal modification on mammalian messenger RNA（mRNA）(Song and Yi,2017).

关键词： N-6-METHYLADENOSINE

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Dynamic Spacer Installation of Multifunctionalities into Metal-Organic Frameworks for Spontaneous One-Step Ethylene Purification from a Ternary C_(2)-Hydrocarbons Mixture

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CCS chemistry 2024年第1期6卷 241-254页

作者： Yang-Yang Xiong Cheng-Xia Chen Tony Pham Zhang-Wen Wei Katherine A.Forrest Mei Pan Cheng-Yong Su MOE Laboratory of Bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275 Department of chemistry University of South FloridaTampaFlorida 33620

Simultaneous ethane and acetylene removal from a C_(2)-gases mixture(C_(2)H_(6),C_(2)H_(4),and C_(2)H_(2))through a one-step separation process for ethylene purification is of great importance yet challenging in petrochemical industry,owing to their similar molecule sizes and physical ***,a series of multifunctionalized metal–organic frameworks(MOFs),LIFM-XYY-1∼8(LIFM stands for Lehn institute of functional Materials,and XYY are the initials of the first author),are constructed via a dynamic spacer installation(DSI)approach to optimize the pore-nanospaces for efficient C_(2)H_(4) isolation from the ternary C_(2)-gases *** of variable organic-spacers into the prototypical MOFs,LIFM-28 or PCN-700,results in dramatically improved pore volume/surface area,contracted pore size,and functionalized pore surface,which in turn bring out high C_(2)-gases uptake capacities,enhanced C_(2)H_(6) and C_(2)H_(2) adsorption selectivities over C_(2)H_(4),and fast adsorption kinetics,providing an effective strategy to achieve delicate trade-off among these indexes for adequate separation ***,optimized LIFM-XYY-7 presents four-times C_(2)H_(6) and C_(2)H_(2) adsorption capacities than *** breakthrough experiments reveal that poly-grade C_(2)H_(4)(>99.9%)can be obtained from binary or ternary C_(2)-hydrocarbon mixtures through a single separation *** with themolecular simulations,this work demonstrates a promising protocol of porenanospace engineering via multi-functional optimization by the DSI approach to screen out MOFs for a formidable task.

关键词： metal-organic frameworks dynamic spacer installation C_(2)H_(6)/C_(2)H_(2)/C_(2)H_(4)gases separation pore nanospace engineering multi-functional optimization

Anion-induced differential assembly and structural transformation of supramolecular coordination cages

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Chinese Chemical Letters 2024年第3期35卷 268-272页

作者： Shao-Ping Zheng Yao-Wei Xu Pei-Yang Su Chen-Hui Liu Yin-Hui Huang Yu-Lin Lu Zhang-Wen Wei Zhiwei Jiao Hai-Sen Xu Cheng-Yong Su MOE Laboratory of Bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510006China institute of Environmental Research at Greater Bay Area Guangzhou UniversityGuangzhou 510006China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

The intimate host-anion interactions will regulate thermodynamics and kinetics in the self-assembly of cationic cages mimicking biological ***,we report construction and transformation of three Pd(Ⅱ)-based metal-organic cages(MOCs)depending on different *** conversions of the lantern-shaped MOC-34 into either octahedral MOC-35 or tricapped trigonal prism MOC-36 are induced by BF_(4)^(–)or NO_(3)^(–),***-36 is kinetically favored and can undergo quantitative conversion to the thermodynamically preferred MOC-35 upon heating,accelerated by excess BF_(4)^(–)to motivate dissociative dynamics of Pd-vertices and lower activation barrier of cage *** guest encapsulation behaviors of MOC-35 and MOC-36 have also been *** results manifest a significance of host-anion dynamics beyond complementary anion template,shedding light on the understanding of intricate anion recognition in nature.

关键词： Supramolecular coordination cage Dynamic host-anion interactions Structural transformation Anion receptor Guest inclusion

Twisted Phosphors that Violate Kasha's Exciton Model in Organic Systems

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Chinese Journal of chemistry 2024年第11期42卷 1237-1246页

作者： Boyi Fu Guangming Wang Jiuyang Li Junbo Li Xun Li Xiaoya Zhao Shuhui Ding Guoping Yan Qianqian Yan Kaka Zhang School of Materials Science and Engineering Wuhan Institute of TechnologyWuhanHubei430205 China Key Laboratory of synthetic and Self-Assembly chemistry for Organic functional Molecules Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling RoadShanghai200032 China

Kasha's exciton model proposes that T1 energy levels of organic compounds are insensitive to molecular aggregation and microenvironment change because of negligible small transition dipole moments of T1 *** model holds true in most organic systems till *** we report the fabrication of twisted organic phosphors with intramolecular charge transfer characters and flexible molecular *** doped into different organic matrices,the twisted phosphor adopts different conformation,exhibits distinct phosphorescence colors and T1 energy levels,which violates Kasha's exciton model in organic *** that the change of phosphorescence colors and maxima can be readily distinguished by human eyes and conventional instrument,the twisted phosphors would be exploited as a new type of molecular probe,which would exhibit potential application in optical sensing and stimuli-responsive systems.

关键词： Afterglow Twisted phosphor Triplet excited state Room-temperature phosphorescence Luminescence Spin-orbit coupling

Asymmetric side-chain engineering of organic semiconductor for ultrasensitive gas sensing

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Chinese Chemical Letters 2024年第3期35卷 428-433页

作者： Xiaoying Ma Xiaojuan Dai Lanyi Xiang Jiajun Chang Danfeng Zhi Haozhen Zhao Zhenjie Ni Ye Zou Xike Gao Fengjiao Zhang School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Laboratory of Organic Solids Institute of ChemistryChinese Academy of SciencesBeijing 100190China Key Laboratory of synthetic and Self-Assembly chemistry for Organic functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Binzhou institute of Technology Binzhou 256606China

Molecular structure of organic semiconductor plays a critical role in determining the performance and functionality of organic electronic devices,by optimizing the electrical,optical and physicochemical *** alkyl chains are fundamental units in tailering the solubility and assemblability,among which the asymmetric properties have been reported as key element for controlling the packing motifs and intrinsic charge ***,we expanded the scope of molecular asymmetry dependent sensing features based on a new series of naphthalene diimides(NDI)-based derivatives substituted with a same branching alkyl chain but various linear-shaped alkyl chains(Cn-).A clear molecular stacking change,from head-to-head bilayer to head-to-tail monolayer packing model,is observed based on the features of anisotropic molecular interactions with the change in the chain *** importantly,a unique LUMO level shift of 0.17 eV is validated for NDI-PhC4,providing a record sensitivity up to 150%to 0.01 ppb ammonia,due to the desired molecular reactivity and device amplification *** results indicate that asymmetric side-chain engineering opens a route for breath healthcare.

关键词： Organic thin film transistor Asymmetric side chain Gas sensing Molecular stacking Energy level manipulating