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Axial enantiomers with donor-regulated TADF feature for multicolor circularly polarized electroluminescence

Science China Chemistry 2024年第6期67卷 2039-2045页

作者： Chen-Hao Guo Wen-Long Zhao Ke-Ke Tan Wei-Chen Guo Liheng Feng Chuan-Feng Chen Meng Li School of Chemistry and Chemical engineering Shanxi UniversityTaiyuan030006China Beijing National laboratory for molecular Sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing100049China

This study optimized the TADF feature of axial chiral enantiomers through precise donor engineering,and multicolor CP-TADFwas achieved in the axial chiral *** pairs of axial enantiomers with donor-regulated TADF feature,namely(R/S)-TPCBD,(R/S)-DPCBD,and(R/S)-DPACBD,were synthesized by introducing carbazole donors with different substituents onto biphenyl cyanide *** the electron-donating ability of donors increases,the emission of these axial enantiomers ranges from 455,476 to 552 nm,their singlet-triplet energy gaps(ΔE_(ST))gradually decrease from 0.30,0.22 to 0.02 e V,accompanied by an increasement in the transition rate(k_(RISC))of RISC process,and the k_(RISC)of DPACBD could reach up to 7.16×10^(5)s^(-1).These axial enantiomers also exhibit mirror-image CD and circularly polarized luminescence(CPL)***,OLEDs based on TPCBD,DPCBD,and DPACBD as emitter were then fabricated,which displayed blue,green,and orange electroluminescence with EQE_(max)of 13.0%,16.4%,and 25.0%,*** results also exhibited a phenomenon of device efficiency increasing with the enhancement of donor ***,the CP-OLEDs using(R/S)-TPCBD,(R/S)-DPCBD and(R/S)-DPACBD as emitters displayed intense CPEL signals with g_(EL)values of 3.4×10^(-3)/-4.1×10^(-3),3.2×10^(-3)/-3.1×10^(-3)and2.3×10^(-3)/-2.1×10^(-3),*** convenient molecular engineering of donor regulation in the same molecular skeleton,CP-TADF materials with multicolor CPEL and improved device performance could be conveniently achieved.

关键词： axial chirality thermally activated delayed fluorescence circularly polarized luminescence electroluminescence organic light-emitting diodes

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Advances of graphdiyne-supported metal catalysts in thermocatalytic reactions

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Nano Research 2024年第4期17卷 2223-2233页

作者： Jia Yu Yida Yang Yuliang Li Changyan Cao Weiguo Song Beijing National laboratory for molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of Molecular Nanostructures and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Beijing National laboratory for molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of organic solidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Supported metal catalysts are widely used in the modern chemical *** electronic interaction between supports and active components is of great significance for heterogeneous ***(GDY),a new type of carbon allotrope with sp-hybridized carbon atoms,πconjugate structure,and electron transmission capability,is a promising candidate as catalyst *** years have witnessed the rapid progress of GDY-supported metal catalysts for different catalysis *** that most processes in the current chemical industry are thermocatalytic reactions,we herein give an overview about the advances and particular characteristics of GDY-supported catalysts in these *** geometric structure and electronic properties of GDY are first ***,the synthesis methods for GDY-supported metal catalysts and their applications in thermocatalytic reactions are discussed,in which the effect of electronic interaction on catalytic performance is ***,the current challenges and future directions of GDY-supported metal catalysts for thermocatalysis are *** is expected that this review will enrich our understanding of the advances of GDY as a superior support for metal catalysts in thermocatalytic reactions.

关键词： graphdiyne metal catalysts thermocatalytic reactions heterogeneous catalysis

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Knittable and washable aerogel fiber inspired by polar bear hair

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Science China Materials 2024年第2期67卷 705-706页

作者： Yue Liu Huisheng Peng State Key laboratory of molecular engineering of Polymers Department of Macromolecular Scienceand Institute of Fiber Materials and DevicesFudan UniversityShanghai 200438China

The advances in chemistry and materials have boosted the development of smart textiles,which are poised to revolutionize human lifestyles through multifunctional integration,such as heating,cooling,sensing and supplying energy^([1,2]).Among them,thermal insulation is an essential function of textiles to protect humans from complex and extreme environments and realize personal thermal management without energy con-sumption^([3]).

关键词： textiles insulation extreme

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“Three-in-one” strategy of trifluoromethyl regulated blood-brain barrier permeable fluorescent probe for peroxynitrite and antiepileptic evaluation of edaravone

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Chinese Chemical Letters 2024年第10期35卷 360-363页

作者： Lei Shen Hongmei Liu Ming Jin Jinchao Zhang Caixia Yin Shuxiang Wang Yutao Yang Key laboratory of Medicinal Chemistry and molecular Diagnosis of the Ministry of Education Chemical Biology Key Laboratory of Hebei ProvinceState Key Laboratory of New Pharmaceutical Preparations and ExcipientsCollege of Chemistry and Materials ScienceHebei UniversityBaoding 071002China Key laboratory of Chemical Biology and molecular engineering of Ministry of Education Institute of Molecular ScienceShanxi UniversityTaiyuan 030006China

Epilepsy,as a chronic neurological disease of the brain,is closely related to oxidative stress,and the peroxynitrite(ONOO-)significantly rise up in this ***,ONOO-is considered as a potential biomarker for early prediction of ***,some potential diagnostic reagents for epilepsy are hindered by the blood-brain barrier(BBB).Meanwhile,“drug repurposing”is attracting a growing ***(EDA),as a first-line drug in the clinical treatment of cerebral ischemia,plays antioxidant roles in scavenging free radicals,promising potential antiepileptic ***,it is imperative to develop fluorescent probes for monitoring ONOO-fluctuations in the epileptic ***,we proposed a novel fluorescent probe with the thiocarbonate as the promising recognition unit for ONOO-and dicyanoisophorone derivative as the ***,by the“three-in-one”strategy,the introduction of trifluoromethyl into DCI-ONOO-3 can extend the emission wavelength of the fluorophore,shorten the response and increase ***,DCI-ONOO-3 was used for monitoring ONOO-fluxes in brain of epileptic mice and evaluating the antiepileptic efficacy of *** opens up a new way for the design of BBB permeable fluorescent probes,and provides a convincing new method for the diagnosis and treatment of epilepsy.

关键词： Fluorescent probe Blood-brain barrier Peroxynitrite Epilepsy Drug repurposing

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Expressing a human RNA demethylase as an assister improves gene-editing efficiency in plants

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molecular Plant 2024年第3期17卷 363-366页

作者： Mengyan Bai Wenxin Lin Chunyan Peng Peizhe Song Huaqin Kuang Jieni Lin Jieping Zhang Jiyao Wang Bo Chen Huarong Li Fanjiang Kong Guifang Jia Yuefeng Guan Guangdong Provincial Key laboratory of Plant Adaptation and molecular Design Innovative Center of Molecular Genetics and EvolutionSchool of Life SciencesGuangzhou UniversityGuangzhou 510006China College of Agronomy China Agricultural UniversityBeijing 100193China College of Life Sciences Fujian Agriculture and Forestry UniversityFuzhouFujian 350002China Synthetic and Functional Biomolecules Center Bejing National Laboratory for Molecular SciencesKey Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Kingagroot Co. Ltd.QingdaoShandong 266000China Tsinghua University-Peking University Joint Center for Life Sciences Bejing 100871China

Dear Editor,Despite myriad successful applications of gene editing in plant functional genomics research and precision breeding,many challenges persist around the efficiency of gene-editing tools for many plant *** instance,soybean(Glycine max)is a major crop providing oil and protein to human diets and feedstock,but its gene-editing efficiency remains relatively low(Bai et al.,2019).

关键词： editing breeding

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engineering the Interface Between Au Nanoparticles and CoO-Ov to Enhance the Catalytic Performance of 5-Hydroxymethylfurfural(HMF)to 2,5-Dimethylfuran(DMF)

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Chemical Research in Chinese Universities 2024年第1期40卷 47-54页

作者： XIANG Shuang GUO Yong LIU Xiaohui WANG Yanqin Key laboratory for Advanced Materials and Joint International Research laboratory of Precision Chemistry and molecular engineering Feringa Nobel Prize Scientist Joint Research CenterResearch Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237P.R.China

The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis ***,we create the Au-CoO-OV interface in the 1.0%Au/Co3O4-Rod-250 catalyst,which could dissociate H2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural(HMF)to 2,5-dimethylfuran(DMF).The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-OV surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen(signals of Au-D and O-D vibration)compared with bare CoO(Co3O4-Rod-250).This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.

关键词： Au-CoO-OV interface Hydride species Heterolytic dissociation 5-Hydroxymethylfurfural(HMF) 2 5-Dimethylfuran(DMF)

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Size-controlled synthesis and near-infrared photothermal response of Cp^(*)Rh-based metalla[2]catenanes and rectangular metallamacrocycles

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Chinese Chemical Letters 2024年第6期35卷 337-343页

作者： Ying Zhao Yin-Hang Chai Tian Chen Jie Zheng Ting-Ting Li Francisco Aznarez Li-Long Dang Lu-Fang Ma College of Chemistry and Chemical engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal UniversityLuoyang 471934China College of Chemistry Zhengzhou UniversityZhengzhou 450001China Shanghai Key laboratory of molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of PolymersDepartment of ChemistryFudan UniversityShanghai 200438China

A variety of research reports on novel supramolecular topologies have been published over the last ***,it is still a great challenge to tap into the inner functional properties of these ***,two tetranuclear metallamacrocycles 1 and 2 and four octonuclear[2]catenanes 3-6 were constructed successfully via a coordination-driven self-assembly strategy,by conscious design and use of the tetramethyl bidentate pyridine ligand L1,and the appropriate selection of six binuclear half-sandwich rhodium building units with different longitudinal *** complexes have been fully characterized by single crystal X-ray diffraction analysis and NMR ***,near-infrared photothermal studies of the obtained[2]catenanes reveal different photothermal response in solid and solution states,which may be attributed to a strong fluorescence quenching effect of the half-sandwich organometallic fragment and different conjugated effect of Cp^(*)Rh based building blocks in the interlocking *** photothermal conversion efficiencies of[2]catenanes 4-6 fall in the range 30.5%-16.5% *** contribution aims to play a key role in the experimental development of Cp^(*)-based photothermal materials.

关键词： Catenanes Photothermal materials Supramolecular topologies Half-sandwich fragment 3,3'-N-donor analogues

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Synthesis of NaY zeolite from a submolten depolymerized perlite:Alkalinity effect and crystallization kinetics

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Chinese Journal of Chemical engineering 2024年第6期70卷 130-138页

作者： Yanli Qu Peng Dong Li Yang Yuanyuan Yue Haoliang Wang Jingcai Cheng Chao Yang CAS Key laboratory of Green Process and engineering State Key Laboratory of Petroleum Molecular&Process EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical engineering University of Chinese Academy of SciencesBeijing 100190China Qingyuan Innovation laboratory Quanzhou 362801China National engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350108China

NaY zeolites are synthesized using submolten salt depolymerized natural perlite mineral as the main silica and alumina sources in a 0.94 L stirred *** of alkalinity ranging from 0.38 to 0.55(n(Na_(2)O)/n(SiO_(2)))on the relative crystallinity,textural properties and crystallization kinetics were *** results show that alkalinity exerts a nonmonotonic influence on the relative crystallinity and textural properties,which exhibit a maximum at the alkalinity of *** nucleation kinetics are studied by fitting the experimental data of relative crystallinity with the Gualtieri *** is shown that the nucleation rate constant increases with increasing alkalinity,while the duration period of nucleation decreases with increasing *** n(Na_(2)O)/n(SiO_(2))ratios ranging from 0.38 to 0.55,the as-synthesized NaY zeolites exhibit narrower crystal size distributions with the increase in *** growth rates determined from the variations of average crystal size with time are 51.09,157.50,46.17 and 24.75 nm·h^(-1),*** is found that the larger average crystal sizes at the alkalinity of 0.38 and 0.43 are attributed to the dominant role of crystal growth over ***,the combined action of prominent crystal growth and the longer duration periods of nucleation at the alkalinity of 0.38 and 0.43 results in broader crystal size *** findings demonstrate that control of the properties of NaY zeolite and the crystallization kinetics can be achieved by conducting the crystallization process in an appropriate range of alkalinity of the reaction mixture.

关键词： NaY zeolite Submolten salt depolymerized perlite Alkalinity Crystallization kinetics

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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

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Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction

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Nano Research 2024年第6期17卷 5298-5304页

作者： Yuwei He Yueguang Chen Renjie Wu Zhihe Xiao Mengxian Li Chunfeng Shi Leyu Wang State Key laboratory of Chemical Resource engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China State Key laboratory of Petroleum molecular and Process engineering SINOPEC Research Institute of Petroleum Processing Co.Beijing 100083China

Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains ***,we report a facile synthesis of bimetallic ultrathin PtM(M=Mo,W,and Cr)nanowires(NWs)composed of group VI B transition metal atomic sites anchored on the *** NWs possess uniform sizes and well-controlled atomic *** to PtW and PtCr catalysts,the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt^(−1).Remarkably,they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR,surpassing previously reported Pt-based ***,the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm^(−2)(H_(2)-O_(2)conditions at 80℃),which is 1.09 times that of commercial Pt/*** ligand effect in the bimetallic surface not only facilitates strong coupling between Mo(4d)and Pt(5d)atomic orbitals to hinder atom leaching but also modulates the d-states of active site,significantly optimizing the adsorption of key oxygen(*O and*OH)species and accelerating the rate-determining step in ORR pathways.

关键词： ligand effect oxygen reduction reaction group VI B transition metal ultrathin nanowires multiple oxygen species

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