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Synthesis,Crystal Structure and Photoluminescence of a Dinulear Copper Complex

Chinese Journal of Structural Chemistry 2018年第10期37卷 1645-1650页

作者： LI Xiao-Ning WU Xiao-Yuan ZHAO Wan-Wan YANG Ming-Xue YU Rong-Min LU Can-Zhong 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 Sciences College of Chemistry and Materials Science Fujian Normal University

A binuclear cuprous complex [Cu（μ-I）（NPPh）]2（1,NPPh = 1-（2-（diphenylphosphanyl）phenyl）-3-phenyl-4,5-dihydro-1 H-pyrazole） was synthesized and characterized by elemental analysis,NMR and X-ray single-crystal structure *** crystallizes in triclinic space group P2_1/n with a = 10.7520（3）,b = 18.1860（5）,c = 11.8487（3）？,β = 91.864（2）,V = 2315.61（11）？~3,Z = 4,Mr = 594.87,Dc = 1.706 g/cm^3,F（000） = 1176.0,μ = 12.582 mm（-1）,GOOF = 1.048,the final R = 0.0289 and wR = 0.0670 for 3787 observed reflections with I 〉 2σ（I）.The Cu atoms in the complex are four-coordinated and adopt distorted tetrahedral coordination *** the solid state,the complex exhibits greenish yellow photoluminescence with a peak maximum of 533 nm,a decay time of 34 μs,and a photoluminescence quantum yield of 63.6% at room temperature,respectively.

关键词： cuprous complex crystal structure emissive property

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Fabrication of WO3/TiO2 Heterostructures for Efficiently Photocatalytic Gaseous Hydrocarbons Degradation:Origin of Photoactivity and Revisit the Role of WO3 Decoration

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Chinese Journal of Structural Chemistry 2018年第2期37卷 230-241页

作者：王丹潘晓阳王广涛易志国 CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences College of Physics and Materials Science Henan Normal University

Efficient oxidation of gaseous small molecular hydrocarbons under mild conditions remains a significant but challenging task to date. Here we report that WO3 decoration can obviously improve the performance of TiO2 （P25） toward the photocatalytic oxidation of several small molecular hydrocarbons （C2H6, C3H8 and C2H4） under simulated solar light irradiation. Among the WO3/TiO2 heterostructures, the 10wt%WO3/TiO2 nanocomposite shows the best photoactivities, which can efficiently oxidize C2H6, C3H8 and C2H4 within 15, 9 and 8 minutes, respectively under simulated sunlight with a light intensity of 200 mW/cm2. By strong contrast, a decreased photoactivity of TiO2 by coupling with WO3 is observed when investigating the performance of photocatalysts toward the degradation of methylene blue （MB） in liquid phase. The opposing effect of WO3 decoration on the performance of TiO2 is thoroughly investigated, and it is found that the improved photoactivities for gaseous hydrocarbon degradation is ascribed to the enhanced oxygen adsorption, resulting from WO3 decoration rather than efficient charge separation within the WO3/TiO2 heterostructures.

关键词： WO3, TiO2, photocatalytic, hydrocarbons OI

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Enhanced CO2 electrolysis at redox engineered interfaces 16

Enhanced CO2 electrolysis at redox engineered interfaces

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16th International Symposium on Solid Oxide Fuel Cells, SOFC 2019

作者： Irvine, John T.S. Xie, Kui School of Chemistry University of St.Andrews KY16 9ST United Kingdom Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian350002 China

ISBN: (纸本)9781607688747

Carbon dioxide obtained from industrial waste streams can be reduced to deliver significant reductions in global CO2 emissions. This can be achieved sustainably by utilising renewable electricity to drive the electrolysis. Solid Oxide Electrolysis (SOE) is an efficient, high temperature approach that reduces polarisation losses and best utilises process heat;however, at present, the technology is relatively unrefined for CO2 electrolysis. Approaches are based upon solid oxide fuel cell (SOFC) technology. There is an important need to develop new materials optimally tuned and better suited to the very different requirements of SOE. As in most electrochemical systems, the interfaces between active components are usually of great importance in determining the performance and lifetime of any application. Here, we report a generic approach of interface engineering to achieve active interfaces at nanoscale by a synergistic control of materials function and interface architecture. We show that the redox-engineered interfaces facilitate the atomic oxygen transfer from adsorbed CO2 molecules to the cathode lattice that determines CO2 electrolysis rate at elevated temperatures. Composite cathodes with in situ grown interfaces demonstrate significantly enhanced CO2 electrolysis and improved durability. © The Electrochemical Society.

关键词： Electrolysis

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Lanthanide-doped near-infrared Ⅱ luminescent nanoprobes for bioapplications

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Science China Materials 2019年第8期62卷 1071-1086页

作者： Shaohua Yu Datao Tu Wei Lian Jin Xu Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China University of Chinese Academy of Sciences Beijing 100049 China College of Chemistry Fuzhou University Fuzhou 350116 China

Luminescent biosensing in the second nearinfrared(NIR-II) region is featured with superior spatial resolution and high penetration depth by virtue of the suppressed scattering of long-wavelength photons. Hitherto, the reported NIR-II nanoprobes are mostly based on carbon nanotubes, organic fluorophores or semiconducting quantum dots. As an alternative, trivalent lanthanide ions(Ln3+) doped nanoparticles have been emerging as a novel class of promising nanoprobes. In this review, we highlight the recent progress in the design of highly efficient Ln3+-doped NIR-II nanoparticles towards their emerging bioapplications, with an emphasis on autofluorescence-free bioimaging, sensitive bioassay, and accurate temperature sensing. Moreover, some efforts and challenges towards this rapidly expanding field are envisioned.

关键词： lanthanide ions nanoprobe near-infrared Ⅱluminescence bioimaging bioassay temperature sensing

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Coupled Solar Battery with 6.9 % Efficiency

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Angewandte Chemie 2023年第30期135卷

作者： Lei Jiao Dr. Xiang Zhang Dr. Yangyang Feng Dr. Jing Lin Prof. Daqiang Yuan Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China

Solar-to-electrochemical energy storage in solar batteries is an important solar utilization technology comparable to solar-to-electricity (solar cells) and solar-to-fuel (photocatalytic cells) conversion. Unlike the indirect approach of integrated solar flow batteries combining photoelectrodes with redox-electrodes, coupled solar batteries enable direct solar energy storage, but are hampered by low efficiency due to rapid charge recombination of materials and misaligned energy levels between electrodes. Herein, we propose a design for a coupled solar battery that intercouples two photo-coupled ion transfer (PCIT) reactions through electron-ion transfer upon co-photo-pumping of photoelectrochemical storage cathode and anode. We used a representative covalent organic framework (COF) to achieve efficient charge separation and directional charge transfer between two band-matched photoelectrochemical storage electrodes, with a photovoltage sufficient for COF dual-redox reactions. By pumping these electrodes, the coupled solar battery stores solar energy via two synergistic PCIT reactions of electron-proton-relayed COF oxidation and reduction, and the stored solar energy is released as electrochemical energy during COF regeneration in discharge while interlocking the loops. A breakthrough in efficiency (6.9 %) was achieved, adaptive to a large-area (56 cm 2 ) tandem device. The presented photo-intercoupled electron-ion transfer (PIEIT) mechanism provides expandable paths toward practical solar-to-electrochemical energy storage.

关键词： Coupled Solar Battery Covalent Organic Framework Photo-Intercoupled Electron-Ion Transfer Photoelectrochemical-Storage Electrode Solar-to-Electrochemical Energy Storage

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The Marriage of Perovskite Quantum Dots with Rare-Earth Emitters

The Marriage of Perovskite Quantum Dots with Rare-Earth Emit...

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中国化学会第十届全国无机化学学术会议

作者： Wei Zheng Zhongliang Gong Datao Tu Ping Huang Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Perovskite quantum dots(PeQDs) are emerging as a new generation of optoelectronic and photovoltaic materials owing to their outstanding optoelectronic properties such as long carrier diffusion distance, large absorption coefficient, high photoluminescence(PL) quantum yield(QY), narrow emission band, and tunable band gap and PL emission by varying the halide composition.[1,2] The combination of PeQDs with rare-earth(RE) emitters may bring about new optical, electric, thermal, and magnetic properties.[3] In this talk, we shall focus on our recent efforts on the development of PeQDs and RE hybridized materials based on RE-doped PeQDs and PeQDs/RE hetero-structures. Specifically, through sensitization by RE-doped nanoparticles, we have realized full-spectrum photon upconversion tuning in all-inorganic CsPbX3(X = Cl, Br, and I) PeQDs under low power density excitation, with a color gamut of 140% NTSC, upconversion QYs approaching 0.5%, and significantly lengthened exciton lifetimes from μs to ms scale.[4] We have also developed a novel strategy for fine-tuning the persistent luminescence with a color gamut of 130% NTSC and highly synchronized afterglow decay over 8 h by using CsPbX3 PeQDs as efficient afterglow light conversion materials.[5] These findings provide a general approach for tailoring the upconversion and persistent luminescence by the marriage of PeQDs with RE emitters, thereby opening up new opportunities for PeQDs and RE emitters towards many emerging applications such as solar spectrum conversion, white-emitting persistent light source, complex data storage, and multilevel anti-counterfeiting.

关键词： perovskite quantum dots rare earths energy transfer upconversion luminescence persistent luminescence

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The Marriage of Perovskite Quantum Dots with Rare-Earth Emitters

The Marriage of Perovskite Quantum Dots with Rare-Earth Emit...

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第九届国际稀土开发与应用研讨会暨2019中国稀土学会学术年会

作者： Wei ZHENG Zhongliang GONG Datao TU Ping HUANG Xueyuan CHEN CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences

Perovskite quantum dots（PeQDs） are emerging as a new generation of optoelectronic and photovoltaic materials owing to their outstanding optoelectronic properties such as long carrier diffusion distance, large absorption coefficient, high photoluminescence（PL） quantum yield（QY）, narrow emission band, and tunable band gap and PL emission by varying the halide composition. [1,2] The combination of PeQDs with rare-earth（RE） emitters may bring about new optical, electric, thermal, and magnetic properties. [3] In this talk, we shall focus on our recent efforts on the development of PeQDs and RE hybridized materials based on RE-doped PeQDs and PeQDs/RE hetero-structures. Specifically, through sensitization by RE-doped nanoparticles, we have realized full-spectrum photon upconversion tuning in all-inorganic CsPbX（X = Cl, Br, and I） PeQDs under low power density excitation, with a color gamut of 140% NTSC, upconversion QYs approaching 0.5%,and significantly lengthened exciton lifetimes from μs to ms scale. [4] We have also developed a novel strategy for fine-tuning the persistent luminescence with a color gamut of 130% NTSC and highly synchronized afterglow decay over 8 h by using CsPbX3 PeQDs as efficient afterglow light conversion materials. [5] These findings provide a general approach for tailoring the upconversion and persistent luminescence by the marriage of PeQDs with RE emitters, thereby opening up new opportunities for PeQDs and RE emitters towards many emerging applications such as solar spectrum conversion, white-emitting persistent light source,complex data storage, and multilevel anti-counterfeiting.

关键词： perovskite quantum dots rare earths energy transfer upconversion luminescence persistent luminescence

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Tumor-Microenvironment-Responsive Biodegradable Nanoagents Based on Lanthanide Nucleotide Self-Assemblies toward Precise Cancer Therapy

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Angewandte Chemie 2022年第14期134卷

作者： Yingjie Yang Dr. Yan Liu Prof. Dr. Datao Tu Dr. Mingmao Chen Yunqin Zhang Hang Gao Prof. Dr. Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials and State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China University of Chinese Academy of Sciences Beijing 100049 China College of Biological Science and Engineering Fuzhou University Fuzhou Fujian 350108 China

Stimuli-responsive nanoagents, which simultaneously satisfy normal tissue clearance and tumor-specific responsive treatment, are highly attractive for precise cancer theranostics. Herein, we develop a unique template-induced self-assembly strategy for the exquisitely controlled synthesis of self-assembled lanthanide (Ln 3+ ) nucleotide nanoparticles (LNNPs) with amorphous structure and tunable size from sub-5 nm to 105 nm. By virtue of the low-temperature (10 K) and high-resolution spectroscopy, the local site symmetry of Ln 3+ in LNNPs is unraveled for the first time. The proposed LNNPs are further demonstrated to possess the ability for highly efficient loading and tumor-microenvironment-responsive release of doxorubicin. Particularly, sub-5 nm LNNPs not only exhibit excellent biocompatibility and predominant renal-clearance performance, but also enable efficient tumor retention. These findings reveal the great potential of LNNPs as a new generation of therapeutic platform to overcome the dilemma between efficient therapy and long-term toxicity of nanoagents for future clinical applications.

关键词： Chemotherapy Self-assembly Renal Clearance Site Symmetry Tumor-Microenvironment-Responsive

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Coupling Electron Transfer and Redox Site in Boranil Covalent Organic Framework Toward Boosting Photocatalytic Water Oxidation

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Angewandte Chemie 2024年第13期136卷

作者： Rahul Anil Borse Yan-Xi Tan Jing Lin Enbo Zhou Yangdan Hui Prof. Daqiang Yuan Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences 350002 Fuzhou Fujian P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China 350108 Fuzhou Fujian P. R. China University of Chinese Academy of Sciences 100049 Beijing P. R. China Institute of Molecular Engineering Plus Fuzhou University 350108 Fuzhou Fujian P. R. China

The efficient polymeric semiconducting photocatalyst for solar-driven sluggish kinetics with multielectron transfer oxygen evolution has spurred scientific interest. However, existing photocatalysts limited by π-conjugations, visible-light harvest, and charge transfer often compromise the O 2 production rate. Herein, we introduced an alternative strategy involving a boranil functionalized-based fully π-conjugated ordered donor and acceptor (D–A) covalent organic frameworks ( Ni-TAPP-COF-BF 2 ) photocatalyst. The co-catalyst-free Ni-TAPP-COF-BF 2 exhibits an excellent ~11-fold photocatalytic water oxidation rate, reaching 1404 μmol g −1 h −1 under visible light irradiation compared to pristine Ni-TAPP-COF (123 μmol g −1 h −1 ) alone and surpasses to reported organic frameworks counterpart. Both experimental and theoretical results demonstrate that the push/pull mechanism (metalloporphyrin/BF 2 ) is responsible for the appropriate light-harvesting properties and extending π-conjugation through chelating BF 2 moieties. This strategy benefits in narrowing band structure, improving photo-induced charge separation, and prolonged charge recombination. Further, the lower spin magnetic moment of M-TAPP-COF-BF 2 and the closer d-band center of metal sites toward the Fermi level lead to a lower energy barrier for *O intermediate. Reveal the potential of the functionalization strategy and opens up an alternative approach for engineering future photocatalysts in energy conversion applications.

关键词： covalent organic frameworks boranil-metalloporphyrin oxygen evolution reaction donor-acceptor-photocatalysts density functional theory

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Molecular Engineering of Methylated Sulfone-Based Covalent Organic Frameworks for Back-Reaction Inhibited Photocatalytic Overall Water Splitting

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Angewandte Chemie 2024年第37期136卷

作者： Xiang Zhang Zhiwei Xiao Lei Jiao Huyue Wu Yan-Xi Tan Jing Lin Daqiang Yuan Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China College of Chemistry and Materials Science Fujian Normal University Fuzhou 350007 P. R. China

Solar-to-hydrogen (H 2 ) and oxygen (O 2 ) conversion via photocatalytic overall water splitting (OWS) holds great promise for a sustainable fuel economy, but has been challenged by the backward O 2 reduction reaction (ORR) with favored proton-coupled electron transfer (PCET) dynamics. Here, we report that molecular engineering by methylation inhibits the backward ORR of molecular photocatalysts and enables efficient OWS process. As demonstrated by a benchmark sulfone-based covalent organic framework (COF) photocatalyst, the precise methylation of its O 2 adsorption sites effectively blocks electron transfer and increases the barrier for hydrogen intermediate desorption that cooperatively obstructs the PCET process of ORR. Methylation also repels electrons to the neighboring photocatalytic sulfone group that promotes the forward H 2 evolution. The resultant DS-COF achieves an impressive inhibition of about 70 % of the backward reaction and a three-fold enhancement of the OWS performance with a H 2 evolution rate of 124.7 μmol h −1 g −1 , ranking among the highest reported for organic-based photocatalysts. This work provides insights for engineering photocatalysts at the molecular level for efficient solar-to-fuel conversion.

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