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Handedness-inverted polymorphic helical assembly and circularly polarized luminescence of chiral platinum complexes

Science China Chemistry 2021年第5期64卷 788-799页

作者： zhong-Liang Gong yu-wu zhong Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of PhotochemistryCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China

Circularly polarized luminescence(CPL)materials have potential applications in three-dimensional(3D)displays,quantum encryption,and optical *** development of single-component CPL materials with polymorphic assembly and handedness inversion remains a significant ***,we present the access of such materials by controlling the underlying assembly pathway of well-designed chiral emitters.A pair of enantiomeric platinum complexes(R)-1 and(S)-1 decorated with a chiralα-methylbenzyl isocyanide ligand were *** using the mixed-solvent(THF/n-hexane,THF=tetrahydrofuran)or high-concentration condition,these complexes were found to assemble via a cooperative or isodesmic pathway with significantly enhanced yellow or red emission,*** aggregate samples obtained via these conditions show efficient CPL(dissymmery factor|glum|>0.02,emission quantum yieldΦ>20%).Interestingly,different assembly pathway leads to helical nanoribbons or nanofibers with opposite handedness from the complex with the same molecular *** has been unambiguously and consistently manifested by circular dichroism and CPL spectral analysis and transmission electron,scanning electron,and atomic force microscope *** work demonstrates an appealing example of constructing polymorphic helical architectures with highly efficient CPL and inverted handedness thanks to the excellent assembly and emission of platinum complexes.

关键词： self-assembly nanostructures circularly polarized luminescence chiral materials platinum complexes

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Photofunction-Directed Coordination Molecular Engineering

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Chinese Journal of Chemistry 2021年第3期39卷 543-549页

作者： yu-wu zhong Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of PhotochemistryCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBejjing 100049China

Molecular engineering has emerged as a highly interdisciplinary field of study on function-directed molecular design,material synthesis,and property optimization,accompanied by a deep understanding of the structure-property *** this review,our recent progress on the design and preparations of photofunctional metal complexes and related materials is summarized from the perspective of coordination molecular *** particular,a series of cyclometalated diruthenium complexes with near-infrared(NIR)electrochromic property have been synthesized by engineering the bridging ligand structures.A group of ruthenium-amine conjugated complexes with multistage NIR electrochromism are obtained on the basis of a multicenter *** engineering the ligand structures,a series of new ruthenium and platinum complexes are synthesized to show switchable luminescence in response to various *** addition,photoluminescent ruthenium,iridium,and platinum complexes are assembled to afford micro/nanocrystals with well-defined morphology and luminescent properties.

关键词： Photochemistry Photophysics Transitional metals Metal-metal interactions Conjugation Luminescence

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Urea-bridged diferrocene: structural, electrochemical, and spectroelectrochemical studies

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Science China Chemistry 2015年第9期58卷 1444-1450页

作者： zhong-Liang Gong yu-wu zhong Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences

Urea-bridged diferrocene derivatives N,N?-diferrocenylurea(1) and N,N?-dimethyl-N,N?-diferrocenylurea(2) were prepared and characterized. Single-crystal X-ray analysis shows that Compound 1 has a trans-trans linear conformation whereas Compound 2 has a trans-cis conformation. Both compounds display two consecutive redox couples with, respectively, E1/2 of +0.29 and +0.42 V vs. Ag/Ag Cl for 1 and +0.31 and +0.50 V for 2. Spectroelectrochemical studies show the presence of distinct intervalence charge transfer(IVCT) transitions for the one-electron-oxidized mixed-valent Compound 1+, with an estimated electronic coupling parameter of 190 cm?1. By contrast, the one-electron-oxidized Compound 2+ shows much weaker IVCT transitions.

关键词： mixed-valent compounds ferrocene electrochemistry urea spectroelectrochemistry

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New insight into hydrogen bond-mediated electron transfer

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Science China Chemistry 2019年第8期62卷 927-928页

Electron transfer (ET) is one of the most fundamental processes in nature, biological systems, and optoelectronic devices. The in-depth ET investigations of synthetic materials are of great significance for the understanding of those occurring in natural systems. Mixed-valence (MV) compounds, consisting of two bridged redox motifs that are structurally identical but different in valence, provide an appealing platform for this purpose [1]. To date, a vast number of MV compounds have been synthesized and examined. However, successful or even partially successful examples of MV compounds with efficient electronic coupling and ET through a hydrogen bond are very limited [2,3]. The difficulty in building hydrogen bond-bridged MV compounds is mainly caused by the dynamic nature and elusive chargetransporting property of hydrogen bond and its decreased stability upon redox reactions.

关键词： New insight transfer stability

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Towards precise synthesis of functional polymers by iterative electropolymerization

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Science China Chemistry 2020年第9期63卷 1175-1176页

作者： Kun Tang yu-wu zhong Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of PhotochemistryCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China

The controllable synthesis of polymers and macromolecules with precise structures is one of the biggest challenges in polymer chemistry[1].Although polymers with welldefined architectures and compositions could now be prepared by various living polymerization techniques[1],it remains elusive to produce macromolecular materials with precise controls of monomer sequences and easy purification procedures.

关键词： precise polymerization synthesis

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Water reduction by an organic single-chromophore photocatalyst

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Chinese Journal of Structural Chemistry 2024年第8期43卷 12-14页

作者： Kun Tang yu-wu zhong Beijing National Laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesKey Laboratory of PhotochemistryInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of chemical Sciences University of Chinese Academy of SciencesBeijing100049China

Photocatalytic reduction of water into hydrogen(H_(2))provides a promising means for the conversion and storage of solar energy[1-3].A pioneering work in this field was reported by Fujishima and Honda in 1972,who used... 详细信息

关键词： catalyst photochemical ultraviolet

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Circularly polarized luminescence of coordination aggregates

Aggregate

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Aggregate 2022年第5期3卷 82-99页

作者： zhong-Liang Gong zhong-Qiu Li yu-wu zhong Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of PhotochemistryCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijingChina School of Chemical Sciences University of Chinese Academy of SciencesBeijingChina

The development and applications of materials with efficient circularly polarized luminescence(CPL)have become an interdisciplinary frontier research *** summarize herein the recent advance in the development and applications of CPLactive aggregates based on metal-ligand coordination materials(termed as“coordination aggregates”).The materials surveyed are classified as aggregates of smallmolecular metal complexes,which include monocomponent assemblies of Pt(II)complexes and other complexes and binary aggregates of metal complexes,and CPL-active metal-ligand coordination helicates,polymers,and *** efforts in improving the dissymmetry luminescence factors and quantum yields of these materials and the use of the aggregation strategy in enhancing the performance of isolated molecules are *** recent applications of chiral metal complexes in circularly polarized organic light-emitting diodes(OLEDs)based on solution-or evaporation-processed procedures are *** addition,the uses of lanthanide complexes in CPL-contrast imaging and as CPL probes are *** common discussion on the mechanism of aggregation-enhanced CPLs and a perspective on future works of CPL-active coordination aggregates are finally given.

关键词： chiral metal complexes circularly polarized luminescence coordination helicates and polymers liquid crystals metal-organic frameworks supramolecular assemblies

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Near-infrared electrochromism of multilayer films of a cyclometalated diruthenium complex prepared by layer-by-layer deposition on metal oxide substrates

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Science China Chemistry 2019年第12期62卷 1675-1685页

作者： Zhi-Juan Li Chang-Jiang Yao yu-wu zhong Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of PhotochemistryCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China

A cyclometalated diruthenium complex 2 bridged by 1,2,4,5-tetra(pyrid-2-yl)benzene with six carboxylic acid groups at two ends was *** and multilayer films FTO/TiO2/(2)n(Zr)(n=1,2)and FTO/SnO2:Sb/(2)n(Zr)(n=1-4)have been prepared via interfacial layer-by-layer coordination assembly of 2 with zirconium(IV)*** films show two consecutive redox couples in the potential range between 0 and+1.0 V ***/*** films exhibit reversible near-infrared electrochromism upon switching of redox *** response time of the films on SnO2:Sb is around a few seconds,while that on TiO2 is around a few tens of *** film deposition cycles were found to have a great impact on the electrochromic *** six films examined,the two-layered film on SnO2:Sb displays the best balanced performance with a contrast ratio of 56%at 1,150 nm and good cyclic stability(9%loss of contrast ratio after 1,000 continuous double-potential-switching cycles),which is superior to that of the previously reported electropolymerized films of a related diruthenium complex with the same bridging *** addition,the X-ray photoelectron spectroscopy,scanning electron microscopy,and electron transfer mechanism of these films have been investigated.

关键词： electrochromism diruthenium complexes multilayer films metal oxides layer-by-layer assembly

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Circularly polarized phosphorescence and photon transport of micro/nanocrystals of ruthenium and iridium complexes with chiral anions

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Science China Chemistry 2023年第10期66卷 2892-2902页

作者： zhong-Qiu Li zhong-Liang Gong Tongling Liang Stefan Bernhard yu-wu zhong Jiannian Yao Beijing National Laboratory for Molecular Sciences(BNLMS) CAS Key Laboratory of PhotochemistryCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Department of Chemistry Carnegie Mellon UniversityPittsburghPennsylvania 15213USA

Materials with efficient circularly polarized phosphorescences(CPPs) are of potential use in advanced data encryption and anticounterfeiting, bioimaging, optoelectronic devices and so forth. Herein, a simple method is presented for the preparations of CPP-active micro/nanocrystals with large luminescence dissymmetry factors(glum), high phosphorescence quantum efficiencies(Φ_(P)) and tunable emission colors. Diastereomeric Ir^(Ⅲ) and Ru^(Ⅱ) complexes with chiral(±)-camphorsulfonate counter-anions are readily synthesized and assembled into crystalline microrods, microplates or nanofibers with ordered morphologies. The chirality information of chiral counter-anions is efficiently transferred to the metal components to afford CPPs with cyan, green,yellow, or red emission colors and Φ_(P)in the range of 5%–85%. The number of chiral anions is found to play a role in influencing the CPP magnitudes of these crystals. The dicationic Ru^(Ⅱ) and tricationic Ir^(Ⅲ) complexes show glumvalues in the 10^(-2)order, which are much larger with respect to those of monocationic Ir^(Ⅲ) complexes. Single crystal X-ray analysis is performed to obtain information on the chirality transfer of these materials. In addition, circularly polarized photonic signal waveguiding is demonstrated using the microcrystals of an Ir^(Ⅲ)complex. This work demonstrates an appealing strategy of constructing chiral micro/nano-architectures for potential applications in chiral nanophotonics.

关键词： circularly polarized luminescence transition metal complexes chirality transfer micro/nanocrystals photon transport

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A Star-Shaped Solvatofluorochromic Pyrene-Triarylamine Derivative as a Fluorescent Thermometer over a Wide Temperature Range

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Chinese Journal of Chemistry 2020年第12期38卷 1515-1520页

作者： Tian-Ge Sun zhong-Liang Gong Jiang-Yang Shao yu-wu zhong Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of PhotochemistryCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China

of main observation and conclusion A star-shaped compound 1 with a pyrene core and four triarylamine arms has been prepared and *** exhibits intense intramolecular-charge-transfer(ICT)emissions with strong *** the basis of the temperature-dependent emission color and wavelength changes,compound 1 behaves as a fluorescent thermometer between 200 and 400 Kwith a high *** comparison,model compounds with one or two triarylamine arms show distinctly lower thermosensitivity.

关键词： compound conclusion intense

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