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Copper(I)cluster of Aggregation-Induced Emission and X-Ray Scintillator Characteristic

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Chemical Research in Chinese Universities 2024年第5期40卷 887-893页

作者： XIONG Jiayu WU Minjian YAO Liao-Yuan moe key laboratory of cluster sciences Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing102488P.R.China Tangshan Research Institute Beijing Institute of TechnologyTangshan063000P.R.China

Due to their precise atomic structures,photoluminescent copper nanoclusters(Cu NCs)have promising applications in basic research and technical applications,such as bioimaging,cell labeling,phototherapy,and photoactivation *** this work,we report a simple strategy for synthesizing novel CuNCs co-protected by alkynyl and phosphine ligands with the molecular formula[Cu_(7)(PPh_(3))_(10)(PE)_(3)(CH_(3)O)](Cu_(4)@Cu_(3)).Single-crystal X-ray crystallography reveals that the NC core exhibits an open square structure and an overall pyramid *** Cu_(4)@Cu_(3) units are connected through weak interactions to form dimers in crystals,creating a molecular cage that looks like two tightly closed ***_(4)@Cu_(3)exhibits dual emission in the visible *** is also an aggregation-induced emission(AIE)-active luminescent substance,which exhibits strong emission in the visible light region when ***,it has the properties of radioluminescent(RL)and could be a potential scintillator *** study not only enriches the types of atomically accurate AIE clusters,but also holds significant importance for the development of a new generation of high-performance and environmentally friendly X-ray scintillators.

关键词： Copper nanocluster Aggregation-induced emission X-Ray scintillator

Eco-Friendly Encapsulation of Metal clusters in Porous Organic Cages for Engineerable Microenvironment and Enhanced Catalysis

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CCS Chemistry 2024年第9期6卷 2186-2197页

作者： Siyu Ren Liangxiao Tan Jun-Hao Zhou Jian Sun Peng Zhang Xingzhong Cao Yun-Hong Zhang Jian-Ke Sun moe key laboratory of cluster Science Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488 Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049

Developing artificial catalysts that mimic the functionality of enzymes and adapt to the surrounding microenvironment to achieve specific activity and selectivity is a fascinating research area yet remains a great *** this work,we present a meticulously designed strategy for the successful encapsulation of ultrasmall metal clusters(MCs)within an amine-type porous organic cage(POC)through electrostatic complexation,phase transfer,and alcohol reduction *** amine cage showcases an intriguing and customizable feature that allows for the regulation of the surrounding microenvironment of the confined MCs through a feasible postmodifi-cation *** functionalization of cage skeleton further facilitates precise adjustment to the surface electronic state of Pd cluster,thereby influencing the adsorption behavior of ***,this controlled regulation leads to modified activity and chemoselectivity in the catalytic hydrogenation of halogenated ***,the investigation of the correlation between the surrounding microenvironment,substrate adsorption,and catalytic performance in the POC-immobilized MCs system has not been previously *** anticipate that our research will provide valuable insights in this field.

关键词： metal cluster porous organic cage encapsulation microenvironment catalysis

Polyoxometalate-organic cage with{Ni_(4)SiW_(9)}node for photocatalytic hydrogen evolution

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Chinese Chemical Letters 2024年第3期35卷 177-181页

作者： Jing Li Yeqin Feng Fangyu Fu Xing Xin Guoyu Yang Hongjin Lv moe key laboratory of cluster Science Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

The design and syntheses of metal-organic cages(MOCs)based on polyoxometalates(POMs)building blocks have attracted increasing attention due to their intriguing molecular architectures and physicochemical *** this work,we have successfully synthesized and systematically characterized a tetrahedral polyoxometalate-based organic cage(POC),K_(3)Na_(17)H_(12)[(C_(4)H_(6)O_(6))_(6)[Ni_(4)(OH)_(3)(A-α-SiW_(9)O_(34))]_(4)]·96H_(2)O(Ni_(16)L_(6)(SiW_(9))_(4)),using tritopic Ni_(4)-substituted Keggin cluster(Ni_(4)SiW_(9))as nodes and flexible L-(+)-tartaric acid ligands as *** resulting POC tetrahedron has been firstly investigated as efficient catalyst for visible-light-driven hydrogen production,achieving a turnover number of 15,500 after 96-h *** high catalytic performance of Ni_(16)L_(6)(SiW_(9))_(4)POC catalyst could be attributed to its unique cage structure,thereby offering more efficient catalytic component *** addition,spectroscopic analyses illustrated the photocatalytic mechanism and the structural stability of the TBA-Ni_(16)L_(6)(SiW_(9))_(4)catalyst during the photocatalytic process.

关键词： Polyoxometalate Polyoxometalate-organic cages Photocatalytic hydrogen production Visible light illumination

Structural Regulations of Layered Borates:From Centric Layers to Chiral Porous Layers

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Precision Chemistry 2024年第6期2卷 256-262页

作者： Chong-An Chen Guo-Yu Yang moe key laboratory of cluster Science School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

Three pentaborates were made by precise structural regulations under hydrothermal conditions,namely,K_(2)Cs-[B_(5)O_(8)(OH)]·0.5CO_(3)(1),KNa_(4)Cs[B_(5)O_(8)(OH)]_(2)·2OH(2),and NaBa[B_(5)O_(8.5)(OH)](3).Compound 1 features the typical 2D layers constructed from the four-connected B_(5)O_(10)(OH)*** adjustment of the reactants and pH values of the systems to remove interlayered CO_(3)^(2−)groups,the centric layers in 1 were transformed to the chiral layers of *** further adjusting cationic templates based on host−guest charge matching,the B_(5)O_(10)(OH)cluster unit was transformed to B_(5)O_(11)(OH),which built the chiral porous layers of *** chiral compounds 2 and 3 exhibit moderate second harmonic generation(SHG)responses of 1.1 and 1.7 times that of KDP(KH_(2)PO_(4)).The structural regulations actualize the evolutions on both structural symmetries and dimensions.

关键词： oxoboron cluster hydrothermal syntheses layers structural regulation nonlinear optical property

EMT transcription factors activated circuits:A novel tool to study EMT dynamics and its therapeutic implications

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Synthetic and Systems Biotechnology 2024年第1期9卷 1-10页

作者： Tianying Chen Wangyue Jia Bo Zhang Hanqi Xie Qiong Wu moe key laboratory of Bioinformatics Center for Synthetic and System BiologySchool of Life SciencesTsinghua UniversityBeijing100084China

The epithelial mesenchymal transition(EMT)plays significant roles in the progression of cancer and fibrotic ***,this process is reversible,resulting in mesenchymal epithelial transition(MET),which plays an important role in cancer *** is a lack of methods to trace and target EMT cells using synthetic biology circuits,which makes it difficult to study the cell fate or develop targeted *** this study,we introduced responsive EMT sensing circuits,which sense the EMT using specific promoters that respond to transcription factors typical of EMT activation(EMT-TFs).The transcriptional strength of EMT-sensing promoters decreased more than 13-fold in response to the overexpression of the ***,the NOT gate circuits were built by placing the tetR transcription repressor under the control of EMT sensing promoters and expressed an output signal using the constitutive CMV promoter modified with tetO sites This circuit is named EMT sensing and responding *** the EMT transcription factors was present,we observed a 5.8-fold signal increase in the ***,we successfully distinguished mesenchymal breast cancer cells from epithelial cancer cells and repressed the proliferation of EMT tumor cells using our *** EMT sensing and responding circuits are promising tools for the identification of EMT cells,which is crucial for EMT-related disease therapy and investigating the mechanisms underlying the reversible EMT process.

关键词： Epithelial mesenchymal transition Synthetic biology Tumor killing

Electronic structure engineering of single atomic sites by plasmoninduced hot electrons for highly efficient and selective photocatalysis

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Nano Research 2024年第8期17卷 6960-6967页

作者： Xiaoya Huang Xinyuan Li Akang Chen Hongfei Gu Shouyuan Li Tailei Hou Shuwen Zhu Shuang Yu Yin Song Jiatao Zhang Beijing key laboratory of Construction Tailorable Advanced Functional Materials and Green Applications MIIT Key Laboratory of Medical Molecule Science and Pharmaceutical EngineeringMOE Key Laboratory of Cluster ScienceSchool of Chemistry and Chemical EngineeringSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China MIIT key laboratory of Complex-field Intelligent Exploration School of Optics and PhotonicsBeijing Institute of TechnologyBeijing 100081China

Single atom(SA)catalysts have achieved great success on highly selective heterogeneous catalysis due to their abundant and homogeneous active *** electronic structures of these active sites,restrained by their localized coordination environments,significantly determine their catalytic performances,which are difficult to ***,we investigated the effect of localized surface plasmon resonance(LSPR)on engineering the electronic structures of single atomic ***,core–shell structures consisted of Au core and transition metal SAs loaded N-doped carbon(CN)shell were constructed,namely Au@M-SA/CN(M=Ni,Fe,and Co).It was demonstrated that plasmon-induced hot electrons originated from Au were directionally injected to the M-SAs under visible light irradiation,which significantly changed their electronic structures and meanwhile facilitated improved overall charge separation *** as-prepared Au@Ni-SA/CN exhibited highly efficient and selective photocatalytic CO_(2) reduction to CO performance,which is 20.8,17.5,and 6.9 times those of Au nanoparticles,Au@CN,and Ni-SA/CN,*** spectroscopy analysis and theoretical calculations confirmed that the plasmon enhanced Ni-SA/CN sites featured increased charge density for efficient intermediate activation,contributing to the superb photocatalytic *** work provides a new insight on plasmon and atomic site engineering for efficient and selective catalysis.

关键词： single atom catalysts plasmon enhancement coupling effect photocatalysis CO_(2) reduction

Winter-spring minimum temperature variations inferred from tree-ring δ^(13)C in southeastern China

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Journal of Forestry Research 2024年第5期35卷 182-190页

作者： Wenli Li Feifei Zhou Heng Zhang keyan Fang key laboratory of Humid Subtropical Eco-Geographical Process(moe) College of Geographic SciencesFujian Normal UniversityFuzhou 350007People’s Republic of China

Long-term temperature variations inferred from high-resolution proxies provide an important context to evaluate the intensity of current ***,tem-perature reconstructions in humid southeastern China are scarce and particularly lack long-term data,limiting us to obtain a complete picture of regional temperature *** this study,we present a well-verified reconstruction of winter-spring(January–April)minimum temperatures over southeastern China based on stable carbon isotopic(δ^(13)C)records of tree rings from Taxus wallichiana *** from 1860 to *** reconstruction accounted for 56.4%of the total observed *** periods occurred during the 1860s–1910s and 1960s–*** temperatures have had an upward trend since the 1920s,most of the cold extremes were in recent *** El Niño-Southern Oscillation(ENSO)variance acted as a key modulator of regional winter-spring minimum temperature ***,teleconnections between them were a nonlinear process,i.e.,a reduced or enhanced ENSO variance may result in a weakened or intensified temperature-ENSO relationship.

关键词： Tree rings Carbon isotope Southeastern China Extreme coldness El nino-southern oscillation

Synthesis and Modulation of Low-Dimensional Transition Metal Chalcogenide Materials via Atomic Substitution

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Nano-Micro Letters 2024年第9期16卷 49-94页

作者： Xuan Wang Akang Chen XinLei Wu Jiatao Zhang Jichen Dong Leining Zhang key laboratory of cluster Science Ministry of Education of ChinaBeijing Key Laboratory of Photoelectronic and Electrophonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China Beijing National laboratory for Molecular sciences Key Laboratory of Organic SolidsInstitute of Chemistry Chinese Academy of SciencesBeijing 100190People’s Republic of China

In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk *** controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various *** this context,the atomic substitution method has emerged as a favorable *** involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely,crystal structures,and inherent properties of the resulting *** this review,we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional,one-dimensional and two-dimensional TMC *** effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are *** enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these ***,challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.

关键词： Transition metal chalcogenides Atomic substitution Ion exchange Low-dimensional materials Controllable synthesis

Auxiliary ligand-induced assembly of atomically precise silver clusters

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Science China Chemistry 2024年

作者： Yeqin Feng Xuemeng Jing Fangyu Fu Mengyun Zhao Manzhou Chi Hongjin Lü Guoyu Yang moe key laboratory of cluster Science Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical Engineering Beijing Institute of Technology

Establishing the correlation between inter-cluster assembly and auxiliary ligands at the atomic level is crucial for the development of metal cluster *** this work,we report the successful preparation and characterization of three Ag clusters,discrete 0-D Ag51S6Cl3（iPrS）21（TsO）15CH3CN(0-D Ag51,iPrS-=isopropanethiolate,TsO-=toluenesulfonate),1-D {Ag38S4（iPrS）18（PhCOO）12}_n(1-D Ag38,PHCOO-=benzoate),and 2-D {Ag20（SO4）Cl2（iPrS）10（NO3）6}_n(2-D Ag20),using a delicate auxiliary-ligand-induced *** analyses reveal that the types of auxiliary ligands can readily affect the structure and dimensionality of resulting Ag *** addition of different surface auxiliary ligands from TsO-to PhCOO-and then to NO3-leads to the formation of 0-D Ag51to 1-D Ag38and then to 2-D Ag20clusters under otherwise identical reaction conditions,*** resulting Ag clusters exhibited structure-related optical/luminescence properties and distinct bathochromic shifts as revealed by the temperature-dependent luminescence and single-crystal X-ray diffraction studies.

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