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Evolution of hollow nanosphere to microtube in the self-assembly of chiral dansyl derivatives and inversed circularly polarized luminescence

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Chinese Chemical Letters 2024年第7期35卷 285-290页

作者： Sifan Du Yuan Wang Fulin Wang Tianyu Wang Li Zhang Minghua Liu Beijing Key Laboratory for Science and Application of Functional molecular and Crystalline Materials Department of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China National Laboratory for molecular Science(BNLMS) CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Here,we designed asymmetric(m DS)and symmetrical(d DS)chiral V-shaped molecules by linking one or two dansyl groups to trans-1,2-cyclohexane diamine and investigated the solvent-regulated structural transformation and inversed circularly polarized luminescence(CPL)in the *** increasing water volume fraction(fw)in the mixed solvent of water/acetonitrile,asymmetric mDS selfassembled into hollow nanospheres and microtubes,while solid nanospheres and solid microplates were corresponding to symmetric d *** this transformation process,the emission of m DS and d DS was changed from yellow-green to blue and cyan color,which was ascribed to twisted intramolecular charge transfer(TICT)and locally excited(LE)fluorescence of V-shaped DS *** conformation of N,Ndimethyl groups with respect to naphthalene ring also led to the transformation of *** tubular and platelike structures had stronger and reversed CPL signals in comparison with spheroidal *** chiral information of DS assembly could be effective transferred to achiral Nile red via co-assembly strategy,which endowed Nile red exhibiting inversed induced CPL signal regulated by water *** work provides a method for achieving a variety of self-assembled structures with adjustable chiroptical properties.

关键词： CPL inversion Hollow structure Self-assembly Dansyl Chirality transfer

Polyelectrolyte Complexes and Coacervates Formed by De novo-Designed Peptides and Oligonucleotide

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Chinese Journal of Polymer Science 2024年第9期42卷 1333-1340,I0007页

作者： Tian-Hao Ren De-Hai Liang Beijing National Laboratory for molecular Sciences Department of Polymer Science and Engineering and the Key Laboratory of Polymer Chemistry and Physics of the Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

The liquid-liquid phase separation of biopolymers in living cells contains multiple interactions and occurs in a dynamic *** the regulation mechanism is still a *** this work,we designed a series of peptides(XXLY)_(6)SSSGSS and studied their complexation and coacervation behavior with single-stranded ***“X”and“Y”are varied to combine known amounts of charged and non-charged amino acids,together with the introduction of secondary structures and pH *** show that the electrostatic interaction,which is described as charge density,controls both the strength of complexation and the degree of chain relaxation,and thus determines the growth and size of the *** hydrophobic interaction is prominent when the charges are ***,the secondary structures of peptides exhibit profound effect on the morphology of the phases,such as solid phase to liquid phase *** study gains insight into the phase separation under physiological *** is also helpful to create coacervates with desirable structures and functions.

关键词： Polyelectrolyte complex Coacervate Peptides Secondary structure Electrostatic interaction

Interparticle energy transfer between NaNdF_(4) and NaYbF_(4) in self-assembled nanostructures

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Journal of Rare Earths 2024年第6期42卷 1029-1035,I0001页

作者： Xinyu Chen Haoze Yang Yuyang Gu Chenqing Wen Yishuo Sun Jiaming Ke Wei Feng department of chemistry and State Key Laboratory of molecular Engineering of Polymers Fudan University Shanghai200433China

Forster resonance energy transfer(FRET)is a widely used spectroscopic *** development of donor-acceptor combinations is essential to advance this *** make the energy transfer efficiency independent of the external environment,we explored the potential of constructing donor—acceptor combinations with lanthanide ion-doped nanoparticles(LNPs),in which the 4f electrons of the lanthanide ions are shielded by the 5s and 6p ***-radiative energy transfer between LNPs was demonstrated in self-assembled nanostructures and core-shell structure of LNPs was used to control the distance between donor and acceptor in self-assembled *** emission intensity ratio of donor and acceptor illustrates that the energy transfer efficiency decreases significantly with increasing distance and the effective energy transfer distance is 8.5 nm,showing the potential of using LNPs as donor-acceptor pairs in the construction of distance-dependent energy transfer system.

关键词： Lanthanide nanoparticles Self-assembly Energy transfer Distance Epitaxialgrowth Rare earths

Nanomaterial Assisted Exosome Analysis Using Mass Spectrometry

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Chemical Research in Chinese Universities 2024年第2期40卷 237-254页

作者： ZHANG Yi ZHOU Bokai LI Qiuning JIN Mingshi BAI Yu Beijing National Laboratory for molecular Sciences Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871P.R.China department of chemistry Yanbian UniversityYanji133002P.R.China

Exosomes,extracellular vesicles(EVs)that play crucial roles in biological processes,have emerged as attractive targets for noninvasive disease diagnosis and *** spectrometry(MS)offers high sensitivity,high throughput,and excellent qualification and quantification capacity,which is the ideal approach for exosome ***’unique physiochemical properties,controllable morphology,and large surface area make them promising in biological sample pretreatment and *** contributed diverse functions to the exosome MS analysis,encompassing substrates for exosome isolation and cargos enrichment,matrices for laser desorption/ionization(LDI),read-out signals and supporters for signal amplification strategies,*** this review,recent progress in the applications of nanomaterial in the exosome MS analysis was summarized and a comprehensive discussion on the challenges and perspectives was proposed for the development of an advancing analysis approach of exosomes for the accurate diagnosis and monitoring of diseases.

关键词： Exosome Nanomaterial Enrichment Matrix Mass spectrometry

Fluorescent carbon dots synthesized in solid phase and air for application in LEDs

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Nano Research 2024年第9期17卷 8495-8503页

作者： Wei-Jie Zheng Zhao-Nan Sun Yi-Ming Wang Huan-Ming Xiong department of chemistry and Shanghai Key Laboratory of molecular Catalysis and Innovative Materials Fudan UniversityShanghai 200438China

Carbon dots(CDs)have been widely adopted as optical materials because of their excellent luminescent ***,most of the reported synthetic methods are conducted in solvents,especially hydrothermal/solvothermal reactions,leading to intractable problems such as toxic and flammable solvents,complex and inseparable by-products,and dangerously high pressures and ***-phase synthesis of CDs in air is an effective solution to overcome the above issues,but solid reactions always result in uncontrolled growth and agglomeration of *** this study,some inorganic salts are selected as catalysts for synthesizing CDs in solid states and air,which also play as dispersants to hinder CDs *** the meantime,some aromatic derivatives containing hydroxyl and amino groups are chosen as carbon sources,ground with the optimized catalyst,and then heated together in *** production yields are affected by the reaction time and reactant ratio,while the graphitization degrees of the CDs are determined by the reaction *** IG/ID value of their Raman spectra increases from 0.59 to 0.85,and the particle size decreases from 2.5 to 1.4 nm when the synthesis temperature is increased from 200 to 280℃.The as-prepared CDs show emission peaks ranging from 366 to 606 nm,with the photoluminescence(PL)quantum yield up to 53%.Their emission color variation mainly results from different carbon sources,which can be ascribed to the differences in the element composition,functional groups,and graphitic nitrogen content of these *** dispersing CDs of different concentrations into polyvinyl alcohol(PVA)and combining them with blue LEDs,cold,standard,and warm white light emitting devices(WLEDs)are prepared,with a color rendering index(CRI)up to *** the as-prepared CDs have antioxidant ability at high temperature,the as-prepared WLEDs have long lifespans,remaining the effective white luminescence after 72 h continuous work.

关键词： carbon dot solid-phase synthesis white LED photoluminescence inorganic salt catalysis

Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li department of chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State Key Laboratory of Surface Physics and department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable ***,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as *** key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon *** mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion *** method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

Understanding of the structural evolution of catalysts and identification of active species during CO_(2) conversion

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Chinese Chemical Letters 2024年第4期35卷 17-30页

作者： Li Li Fanpeng Chen Bohang Zhao Yifu Yu department of chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China

Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and ameliorate the ever-fragile environment status. However, the complexity of the CO_(2) conversion reaction and the strong reduction conditions lead to the inevitable structural evolution, making it difficult for the prior design of suitable catalytic materials. Herein, to guide the rational design of efficient catalysts,we will be centered on the thermal, electro, and photo-induced structural evolution and active species identification during the CO_(2) conversion, including the in situ/operando characterization techniques monitoring the activation, steady, and deactivation stage of the catalysts as well as the inherent restructuring mechanism towards active species. Besides, the future challenges and opportunities on the merits of combining the structural evolution with the adsorbed intermediates recognized by ultra-fast spectroscopic techniques, simultaneously, the combination of theoretical simulation and the results of in situ experiments will also be addressed. This review can not only guide the identification of real active species, but also provide an approach to design the specific active species towards CO_(2) conversion, rather than only focusing on activity, for the purpose of practical industrial application.

关键词： CO_(2) Structural evolution Active species In situ Operando

Ni-catalyzed highly regio- and stereo-selective diborylative cyclization of 1,6-enynes with diboron reagent

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Science China chemistry 2024年第3期67卷 981-989页

作者： Qitao Guan Zhen Shen Yiqiang Tian Genping Huang Chun Zhang Institute of molecular Plus Tianjin Key Laboratory of Molecular Optoelectronic ScienceDepartment of ChemistrySchool of SciencesTianjin UniversityTianjin 300072China State Key Laboratory of Elemento-Organic chemistry Nankai UniversityTianjin 300071China

The Ni-catalyzed highly selective diborylative cyclization of 1,6-enynes with diboron reagent has been developed. When pinB-Bdan was used, multiple types of boron-containing functional groups could be installed into organic molecule with great chemoselectivity and regioselectivity though this reaction. Meanwhile, if B_2pai_2 was employed, the asymmetric diborylative cyclization could be well induced by using strategy of dynamic kinetic resolution. Importantly, the above reactions could afford desired product with 100% atomic economy, and could be compatible with different series of substituents. The studies of further transformation well illustrated that different type products could serve diverse synthetic strategy. Notably, the reaction mechanism was intensively studied by density functional theory(DFT) calculations, which could reveal the mechanism of regio- and enantio-selective control.

关键词： nickel-catalyzed organoboron cyclization regioselectivity enantioselectivity

Competitive intermetallics formation in Pd-Zn-Cd system via seeded growth from ultra-thin Pd nanosheets for electrocatalytic ethanol oxidation reaction

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Nano Research 2024年第9期17卷 8552-8559页

作者： Donghao Zhang Lianxi Si Qianqian Ren Xintong Yan Shi Hu department of chemistry School of ScienceTianjin Key Laboratory of Molecular Optoelectronic ScienceTianjin UniversityTianjin 300072China

Pd-based catalysts exhibit higher catalytic activity and durability in many electrochemical ***,the electrochemical performance can be further enhanced by fine-tune of the alloy *** binary alloys have been fully studied,the multicomponent alloys are far beyond understanding,which leaves cocktail effect a compromised explanation for the high-entropy *** Pd nanosheet-seeded growth was used to synthesize a Pd-Zn-Cd ternary alloy by accurately controlling the Pd-Zn-Cd molar ratio through adjusting the amount of introduced Cd *** analysis of the crystal phase structure of PdCdZnx and PdZn_(x)Cd_(1-x),the competitive relationship of Zn and Cd in the alloying process with Pd was unveiled:Pd1Cd1 intermetallics(IMC)is thermodynamically favored over Pd_(1)Zn_(1)IMC in the ternary ***,the increased structure stability of PdCd over PdZn does not bring about increased durability in the catalytic ethanol oxidation *** morphology selection of Pd seeds is also crucial for the study,as Pd cubes,Pd tetrahedrons,and Pd octahedrons do not form PdZn in the same *** successful alloying through the seeded growth depends on the maximum diffusion depth of foreign atoms into the seed.

关键词： PdZn alloy seed growth method ethanol oxidation reaction composition control ternary alloying