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Unraveling the triplet excited-state dynamics of Bi^(3+)in vacancyordered double perovskite Cs_(2)SnCl_(6) nanocrystals

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Nano Research 2022年第7期15卷 6422-6429页

作者： Mengyao Jin Wei Zheng Zhongliang Gong Ping Huang Renfu Li Jin Xu Xingwen Cheng Wei Zhang Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry Fuzhou UniversityFuzhou 350116China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Luminescent metal halides doped with ns^(2-)metal ions such as 6s^(2-)metal Bi^(3+)have aroused reviving interest owing to their outstanding optical properties;however,the origin of the photoluminescence(PL)remains controversial and ***,we report a strategy for the controlled synthesis of Bi^(3+)-doped vacancy-ordered double perovskite Cs_(2)SnCl_(6)nanocrystals(NCs)and unravel the triplet excited-state dynamics of Bi^(3+)through temperature-dependent PL and ultrafast femtosecond transient absorption *** to the aliovalent Bi^(3+)doping in the spatially confined zero-dimensional(0D)structure of Cs2SnCl6,Bi^(3+)ions experience an enhancive Jahn-Teller distortion in the excited state,which results in intense broadband blue PL originating from the inter-configurational 3P0,1→1S0 transitions of Bi^(3+)at 450 nm,with a large Stokes shift and a quantum yield of 35.2%.Specifically,an unusual thermal-enhanced Jahn-Teller splitting of the excitation band and a remarkable transition of the PL lifetime from ms at 10 K toμs at 300 K were observed,as solid evidence for the isolated Bi^(3+)*** findings clarify the controversy about the PL origin in ns^(2-)metal ion-doped lead-free luminescent metal halides,thereby paving the way for exploring their optoelectronic applications.

关键词： bismuth luminescent nanocrystals metal halide excited-state dynamics electron-phonon coupling

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A sandwiched luminescent heterostructure based on lanthanide-doped Gd_(2)O_(2)S@NaYF_(4)core/shell nanocrystals

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Aggregate 2023年第6期4卷 163-171页

作者： Dengfeng Yang Wei Zheng Ping Huang Meiran Zhang Wei Zhang Zhiqing Shao Wen Zhang Xiaodong Yi Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouChina Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China FuzhouChina Fujian College University of Chinese Academy of SciencesFuzhouChina College of Chemistry Fuzhou UniversityFuzhouChina

Lanthanide(Ln^(3+))oxysulfide nanocrystals(NCs)have great prospect in many advanced technologies;however,they suffer from a low photoluminescence efficiency due to the volatility of sulfur and deleterious surface quenching ***,we report a novel sandwiched luminescent heterostructure based on Ln^(3+)-doped Gd_(2)O_(2)S@NaYF_(4)core/shell NCs with tunable sulfur content in the sandwich *** means of Eu^(3+)as the sensitive structural probes,we unravel the ligand-mediated structure control of the NCs from Gd_(2)O_(3):Ln^(3+)@NaYF_(4)to Gd_(2)O_(2)S:Ln^(3+)@NaYF_(4)with tailored S2–*** a sandwich-type core/shell heterostructure enables us to achieve efficient and multicolor downshifting and upconversion luminescence(UCL),with up to 208.8 folds of enhancement in UCL intensity as compared to that of their core-only *** findings provide a general approach for the controlled synthesis of lanthanide oxysulfide@fluoride heterostructure,which offers a new way for the materials design towards diverse emerging applications.

关键词： Gd_(2)O_(2)S heterostructure lanthanide NaYF_(4) upconversion luminescence

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A cobalt redox switch driving alcohol dehydrogenation by redox coupled molecular swing

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Chinese Chemical Letters 2023年第6期34卷 459-462页

作者： Guoling Li Yang Liu Wei Wang Zhu Zhuo Yougui Huang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesXiamen 361021China Xiamen Institute of Rare Earth Materials Haixi InstituteChinese Academy of SciencesXiamen 361021China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Developing redox switches that not only perform specific mechanical movements but also drive important chemical reactions is important but a great ***,we report a redox pair of cobalt species(Co^(Ⅲ)/Co^(Ⅱ))that switches through photo-dehydrogenation of alcohol and hydrogenation of *** cobalt species is equipped with a flexible azo-ligand containing two bulky planar substituents.A planar oxidated sate(Co^(Ⅲ)species)can be photo-reduced to a saddle-like reduced state(Co^(Ⅱ))with alcohol molecules as electron donors,and in turn the Co^(Ⅲ)species can be recovered with azo-ligand as oxidant under acidic *** the redox states of the pair are isolated and characterized by single crystal X-ray *** the switching cycle,alcohol is oxidized to aldehyde by azo-ligand through proton coupled electron transfer and the cobalt complex acts as a redox *** results provide important insights into alcohol dehydrogenation catalyzed by redox complexes.

关键词： Redox switch Alcohol dehydrogenation Azo-ligand hydrogenation Cobalt complex Mechanical motion

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Recent progress, challenges and prospects of electrolytes for fluoride-ion batteries

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Energy Reviews 2024年第3期3卷 102-128页

作者： Ming Zhang Xiaocao Cao Yaowei Hao Haodong Wang Jian Pu Bo Chi Zhongrong Shen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen361021China College of Chemical Engineering Fuzhou UniversityFuzhouFujian350116China School of Materials Science and Engineering State Key Laboratory of Material Processing and Die&Mould TechnologyHuazhong University of Science and TechnologyWuhan430074China

In the development of new electrochemical concepts for the fabrication of high-energy-density batteries,fluorideion batteries(FIBs)have emerged as one of the valid candidates for the next generation electrochemical energy storage technologies,showing the potential to match or even surpass the current lithium-ion batteries(LIBs)in terms of energy density,safety without dendritic grains,and elimination of dependence on scarce lithium and cobalt ***,the development of FIBs is still in its infancy and their performance is far from satisfactory,with issues such as the lower fluoride-ion conductivity of the electrolytes and the reversibility of the electrodes hindering their *** reviews have mainly focused on inorganic solid electrolytes with a brief emphasis on the development of various fluoride-ion conductors and their ion-conducting ***,this review summarizes the current developments in various electrolytes,a systematic overview of the current progress for various fluoride-ion electrolytes is presented by beginning with the history,structure and classification of FIBs,ion-transport mechanisms are briefly *** advances in different classes of fluoride-ion electrolytes are *** methods for optimizing the ionic conductivity characteristics of the fluoride-ion electrolytes are ***,an outlook on the future research direction of FIBs is given by highlighting some critical issues,challenges and prospects of fluoride-ion electrolytes.

关键词： Solid electrolyte Liquid electrolyte Composited electrolyte Fluoride-ion Conductivity

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A new class of luminescent nanoprobes based on main-group Sb^(3+) emitters

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Nano Research 2022年第1期15卷 179-185页

作者： Chunguang Zhang Meiran Zhang Wei Zheng Jiaojiao Wei Shiteng Wang Ping Huang Xingwen Cheng Tao Dai Zhuo Chen Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China Fujian Science Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Inorganic luminescent nanocrystals(NCs)doped with main-group ns^(2)-metal ions have evoked tremendous interest in many technological fields owing to their superior optical ***,we report a new class of luminescent nanoprobes based on 5s2-metal Sb3+-doped CaS NCs that are excitable by using a near ultraviolet light-emitting *** optical properties and excited-state dynamics of Sb3+in CaS NCs are comprehensively surveyed through temperature-dependent steady-state and transient photoluminescence(PL)*** to the strong electron-phonon coupling of Sb^(3+)in CaS NCs,Sb3+ions experience a dynamic Jahn-Taller distortion on the excited state,which results in bright green PL of Sb3+with a broad emission band,a large Stokes shift,and a high PL quantum yield up to 17.3%.By taking advantage of the intense PL of Sb^(3+),we show in proof-of-concept experiments the application of biotinylated CaS:Sb^(3+)NCs as sensitive luminescent nanoprobes for biotin receptor-targeted cancer cell imaging and zebrafish imaging with a high imaging *** findings provide fundamental insights into the excited-state dynamics of Sb^(3+)in CaS NCs,thus laying a foundation for future design of novel and versatile luminescent nanoprobes via main-group ns2-metal doping.

关键词： CaS Sb^(3+) photoluminescence excited-state dynamics nanoprobe bioimaging

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Time-resolved luminescent nanoprobes based on lanthanide nucleotide self-assemblies for alkaline phosphatase detection

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Nano Research 2023年第8期16卷 11250-11258页

作者： Yunqin Zhang Yang Cao Yan Liu Yingjie Yang Mingmao Chen Hang Gao Lushan Lin Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China College of Biological Science and Engineering Fuzhou UniversityFuzhou 350108China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117China Fujian College University of Chinese Academy of SciencesFuzhou 350002China

Currently,enzyme-responsive nanomaterials have shown great promise in prognosis or diagnosis of disease ***,the great obstacle for conventional enzyme-responsive nanomaterials frequently lies in autofluorescence interference,poor monodispersity,uncontrollable size and morphology,low optical stability,and biotoxicity,which fundamentally impede their practical application in biological *** overcome these deficiencies,we proposed a novel strategy for reliable and precise detection of an enzyme disease biomarker,alkaline phosphatase(ALP),through lanthanide(Ln^(3+))nucleotide nanoparticles(LNNPs)with extremely improved monodispersity and uniformity,which were achieved by the coordination self-assembly between ATP and Ln^(3+)inside micellar ***,for ATP-Ce/Tb LNNPs,highly improved photoluminescence(PL)emission of Tb^(3+)can be achieved via efficient Ce^(3+)*** demonstrated that ALP could specifically cleave the phosphorus–oxygen(P–O)bonds of ATP and result in the collapse of ATP-Ce/Tb scaffold,finally leading to the PL quenching of Tb^(3+).By taking advantage of time-resolved(TR)PL technique,the fabricated ATP-Ce/Tb LNNPs presented superior selectivity and sensitivity for the ALP bioassay in complicated serum samples,thus revealing the great potential of ATP-Ce/Tb LNNPs in the areas of ALP-related disease prognosis and diagnosis.

关键词： alkaline phosphatase(ALP)-responsive micellar nanoreactor coordination self-assembly lanthanide sensitization time-resolved photoluminescence(TRPL)

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A General Self-Sacrifice Template Strategy to 3D Heteroatom-Doped Macroporous Carbon for High-Performance Potassium-Ion Hybrid Capacitors

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Nano-Micro Letters 2021年第9期13卷 1-15页

作者： Junwei Li Xiang Hu Guobao Zhong Yangjie Liu Yaxin Ji Junxiang Chen Zhenhai Wen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research On the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002People’s Republic of China

Potassium-ion hybrid capacitors(PIHCs)tactfully combining capacitor-type cathode with battery-type anode have recently attracted increasing attentions due to their advantages of decent energy density,high power density,and low cost;the mismatches of capacity and kinetics between capacitor-type cathode and battery-type anode in PIHCs yet hinder their overall performance ***,based on prediction of density functional theory calculations,we find Se/N co-doped porous carbon is a promising candidate for K+storage and thus develop a simple and universal self-sacrifice template method to fabricate Se and N co-doped three-dimensional(3D)macroporous carbon(Se/N-3DMpC),which features favorable properties of connective hier-archical pores,expanded interlayer structure,and rich activity site for boosting pseudocapacitive activity and kinetics toward K^(+)storage anode and enhancing capacitance performance for the reversible anion adsorption/desorption *** expected,the as-assembled PIHCs full cell with a working voltage as high as 4.0 V delivers a high energy density of 186 Wh kg^(−1) and a power output of 8100 W kg^(−1) as well as excellent long service *** proof-of-concept PIHCs with excellent performance open a new avenue for the development and application of high-performance hybrid capacitors.

关键词： Potassium-ion hybrid capacitors Self-sacrifice template Se/N co-doped 3D macroporous Long service life

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Separation of aluminum from rare earth by solvent extraction with 4-octyloxybenzoic acid

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Journal of Rare Earths 2023年第2期41卷 290-299页

作者： Gaoshan Yu Zhiyuan Zeng Yun Gao Shuainan Ni Hepeng Zhang Xiaoqi Sun CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Research Center for Rare Earth Engineering Technology Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100039China Jiangxi Province Key Laboratory of Cleaner Production of Rare Earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhou 341000China

Leaching method is usually used to extract rare earth(RE)elements from ion adsorbed RE *** the leaching process,some impurities such as aluminum(Al)enter the leaching *** separation of Al from RE by carboxylic acid extractant 4-octyloxybenzoic acid(POOA)was studied in this *** changing the pH value,temperature,solvent,saponification degree and other parameters,the extraction and separation performance of POOA in chloride system was systematically *** specific extraction experiments and slope analysis,it can be seen that the stoichiometric ratio of POOA to Al is 3:1during the extraction *** separation factor of Al^(3+)and Pr^(3+)can reach about *** with easily emulsified naphthenic acid,POOA achieves better phase *** above results show that saponified POOA(S-POOA)has a good separation effect on Al and *** the condition of low concentration stripping acid of 0.60 mol/L HCl,the developed extraction system can be almost completely stripped,and the stripping rate reaches 97.52%.The regenerated POOA can be directly used for the recycling extraction.

关键词： Rare earths Aluminium 4-octyoxybenzoic acid Solvent extraction Separation

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A chiral SrSi_(2)(srs)superstructure constructed by a dual interaction system showing isotropic electrical conductivity

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Chinese Chemical Letters 2023年第9期34卷 317-320页

作者： Jin Liu Zi-Xiu Lu Fa-Fa Wu Guo-Ling Li Bin Wang Xue-Li Cao Wei Wang Zhu Zhuo Qiao-Hong Li You-Gui Huang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China State Key Laboratory of Structure Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Most porous conductive frameworks are highly anisotropic in their structures thus leading to anisotropic charge *** we report a supramolecular self-assembly which is constructed by intermolecular hydrogen bonding andπ···π*** material features a chiral,porous,cubic framework structure withπ-stacked helical columns along all of the three Cartesian *** a result,isotropic charge transport with an electrical conductivity(σ)of 2.1×10^(–7)S/cm is *** achieving isotropic charge transport in aπ-stacked supramolecular assembly,these results provide a new type of isotropic conductive framework materials alternative to conductive metal-organic frameworks(MOFs).

关键词： Electrical conductivity Self-assembly Isotropic π···πInteractions Chiral

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Low Trap Density Para-F Substituted 2D PEA_(2)PbI_(4)(X=Cl,Br,I)Single Crystals with Tunable Optoelectrical Properties and High Sensitive X-Ray Detector Performance

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Research 2023年第1期2022卷 273-283页

作者： Jiayu Di Haojin Li Li Chen Siyu Zhang Yinhui Hu Kai Sun Bo Peng Jie Su Xue Zhao Yuqi Fan Zhenhua Lin Yue Hao Peng Gao Kui Zhao Jingjing Chang State Key Discipline Laboratory of Wide Band Gap Semiconductor Technology School of MicroelectronicsXidian University710071 XianChina Advanced Interdisciplinary Research Center for Flexible Electronics Academy of Advanced Interdisciplinary ResearchXidian University710071 Xi'anChina Key Laboratory of Applied Surface and Collid Chemistry National Ministry of EducationSchool of Materials Science and EngineeringShaanxi Normal University710119 Xi'anChina CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Exploring halogen engineering is of great significance for reducing the density of defect states in crystals of organic-inorganic hybrid perovskites and hence improving the crystal ***,high-quality single crystals of PEA_(2)PbI_(4)(X=CI,Br,I)and their para-F(p-F)substitution analogs are prepared using the facile solution method to study the effects of both p-F substitution and halogen anion *** p-F substitution,the triclinic PEA_(2)PbX_(4)(X=Cl,Br)and cubic PEA_(2)PbX_(4)(X=I)crystals unifies to monoclinic crystal structure for p-F-PEA_(2)PbX_(4)(X=Cl,Br,I)*** p-F substitution and halogen engineering,together with crystal structure variation,enable the tunability of optoelectrical ***,after the p-F substitution,the energy levels are lowered with increased Fermi levels,and the bandgaps of p-F-PEA_(2)PbX_(4)(X=Cl,Br,I)are slightly *** from the enhancement of the charge transfer and the reduced trap density by p-F substitution and halogen anion engineering,the average carrier lifetime of the p-F-PEA_(2)PbI_(4)is obviously *** with PEA_(2)PbI_(4)the X-ray detector based on p-F-PEA_(2)PbI_(4)single crystals exhibits higher radiation stability under high-dose X-ray irradiation,implying long-term operando stability.

关键词： properties stability substitution

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