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Cyanide-based Covalent Organic Frameworks for Enhanced Overall Photocatalytic Hydrogen Peroxide Production

Angewandte Chemie 2024年第19期136卷

作者： Enbo Zhou Futong Wang Xiang Zhang Yangdan Hui Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures 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 Fuzhou University Fuzhou 350108 Fujian P. R. China

Photocatalytic oxygen reduction to produce hydrogen peroxide (H 2 O 2 ) is a promising route to providing oxidants for various industrial applications. However, the lack of well-designed photocatalysts for efficient overall H 2 O 2 production in pure water has impeded ongoing research and practical thrusts. Here we present a cyanide-based covalent organic framework (TBTN-COFs) combining 2,4,6-trimethylbenzene-1,3,5-tricarbonitrile (TBTN) and benzotrithiophene-2,5,8-tricarbaldehyde (BTT) building blocks with water-affinity and charge-separation. The ultrafast intramolecular electron transfer (<500 fs) and prolonged excited state lifetime (748 ps) can be realized by TBTN-COF, resulting in a hole accumulated BTT and electron-rich TBTN building block. Under one sun, the 11013 μmol h −1 g −1 yield rate of H 2 O 2 can be achieved without any sacrificial agent, outperforming most previous reports. Furthermore, the DFT calculation and in situ DRIFTS spectrums suggesting a Yeager-type absorption of *O 2 ⋅ − intermediate in the cyanide active site, which prohibits the formation of superoxide radical and revealing a favored H 2 O 2 production pathway.

关键词： Covalent organic framework Photocatalytic H2O2 production Oxygen reduction reaction Charge-separation Intramolecular electron transfer

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Pseudo-2D Layered Organic-Inorganic Manganese Bromide with a Near-Unity Photoluminescence Quantum Yield for White Light-Emitting Diode and X-Ray Scintillator

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Angewandte Chemie 2023年第45期135卷

作者： Wei Zhang Ping Sui Prof. Wei Zheng Prof. Lingyun Li Prof. Shuaihua Wang Prof. Ping Huang Wen Zhang Qi Zhang Prof. Yan Yu Prof. Xueyuan Chen Key Laboratory of Advanced Materials Technologies and International (Hongkong Macao and Taiwan) Joint Laboratory on Advanced Materials Technologies College of Materials Science and Engineering Fuzhou University 350108 Fuzhou Fujian China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian 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 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China 350108 Fuzhou Fujian China

Eco-friendly lead-free organic–inorganic manganese halides (OIMHs) have attracted considerable attention in various optoelectronic applications because of their superior optical properties and flexible solution processibility. Herein, we report a novel pseudo-2D layered OIMH (MTP) 2 MnBr 4 (MTP: methyltriphenylphosphonium), which exhibits intense green emission under UV/blue or X-ray excitation, with a near-unity photoluminescence quantum yield, high resistance to thermal quenching (I 150 °C =84.1 %) and good photochemical stability. These features enable (MTP) 2 MnBr 4 as an efficient green phosphor for blue-converted white light-emitting diodes, demonstrating a commercial-level luminous efficiency of 101 lm W −1 and a wide color gamut of 116 % NTSC. Moreover, these (MTP) 2 MnBr 4 crystals showcase outstanding X-ray scintillation properties, delivering a light yield of 67000 photon MeV −1 , a detection limit of 82.4 nGy s −1 , and a competitive spatial resolution of 6.2 lp mm −1 for X-ray imaging. This work presents a new avenue for the exploration of eco-friendly luminescent OIMHs towards multifunctional light-emitting applications.

关键词： Manganese Halide Photoluminescence Scintillator WLED X-Ray Imaging

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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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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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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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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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Investigation of sustainable rare earth recovery on carbon electrodes by electrosorption and precipitation coupling strategy

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Journal of Environmental Chemical Engineering 2025年第4期13卷

作者： Yanxin Wang Peilin Lei Yujun Chai Xiaoqi Sun College of Chemistry and Materials Science Hebei Normal University Shijiazhuang Hebei 050024 PR China Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 PR China Hebei Key Laboratory of Inorganic Nano-materials Hebei Normal University Shijiazhuang Hebei 050024 PR China 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 Fujian 350002 PR China University of Chinese Academy of Sciences Beijing 100049 PR China

This study investigates the recovery of rare earth (RE) using a coupling electrosorption and precipitation strategy. The electrochemical behavior and recovery properties of various materials, i.e., activated carbon, carbon nanofibers, carbon nanotubes, graphene, and porous carbon, were evaluated. They show the good crystalline, amorphous or the coexistence of two states. The reaction occurred on grapheme and carbon nanofiber within the scan range, but it shows the capacitive behavior for other three. The electrosorption-precipitation coupling capacity and removal efficiency varied due to the cooperation of applied voltage and inner voltage, in addition to the effect of functional groups, defects and conductivity. During the process, rare earth ions were first adsorbed onto the electrode surface and then reacted with OH - ions to form precipitates. Meanwhile, oxygen was generated at the Pt electrode, while only trace amounts of hydrogen were observed on the working electrode due to the involvement of NO 3 - ions. Additionally, La(Ⅲ), Ce(Ⅲ), Pr(Ⅲ) and Nd(Ⅲ) ions were effectively recovered and enriched using carbon-based electrodes, with capacities of 2064.5, 2305.8, 2198.7, and 2288.9 mg·g −1 , respectively, in a 0.01 mol·L −1 RE solution. These findings suggest that the selection of materials with larger specific surface areas, high electrical conductivity, more defects, effective functional groups and low potential can reduce internal voltage, enhance reaction driving forces, and improve recovery efficiency. The recovery process has sustainable RE separation characteristics, with no volatile organic solvent (VOC), acid and alkali consumption, or wastewater.

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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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