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Enhancing Dye-Triplet-Sensitized Upconversion Emission Through the Heavy-Atom Effect in CsLu2F7:Yb/Er Nanoprobes

Angewandte Chemie 2021年第1期134卷

作者： Peng Zhang Dr. Jianxi Ke Prof. Datao Tu Jiayao Li Yifan Pei Le Wang Dr. Xiaoying Shang Tianyong Guan Dr. Shan Lu Prof. Zhuo Chen Prof. Xueyuan Chen 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 Fuzhou Fujian 350002 China College of Chemistry Fuzhou University Fuzhou Fujian 350116 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China

Lanthanide (Ln 3+ )-doped upconversion (UC) nanoprobes, which have drawn extensive attention for various bioapplications, usually suffer from small absorption cross-sections and weak luminescence intensity of Ln 3+ ions. Herein, we report the controlled synthesis of a new class of Ln 3+ -doped UC nanoprobes based on CsLu 2 F 7 :Yb/Er nanocrystals (NCs), which can effectively increase the intersystem crossing (ISC) efficiency from singlet excited state to triplet excited state of IR808 up to 99.3 % through the heavy atom effect. By virtue of the efficient triplet sensitization of IR808, the optimal UC luminescence (UCL) intensity of IR808-modified CsLu 2 F 7 :Yb/Er NCs is enhanced by 1309 times upon excitation at 808 nm. Benefiting from the intense dye-triplet-sensitized UCL, the nanoprobes are demonstrated for sensitive assay of extracellular and intracellular hypochlorite with an 808-nm/980-nm dual excited ratiometric strategy.

关键词： CsLu2F7 dye sensitization lanthanide ions triplet excited states upconversion luminescence

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Synergistic Lysozyme-Photodynamic Therapy Against Resistant Bacteria based on an Intelligent Upconversion Nanoplatform

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Angewandte Chemie 2021年第35期133卷

作者： Zhuo Li Dr. Shan Lu Dr. Wenzhen Liu Tao Dai Jianxi Ke Dr. Xingjun Li Renfu Li Yuxiang Zhang Prof. Zhuo Chen Prof. Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures State Key Laboratory of Structural Chemistry and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China College of Chemistry Fuzhou University Fuzhou Fujian 350116 China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China

The rapid emergence of drug-resistant bacteria has raised a great social concern together with the impetus for exploring advanced antibacterial ways. NIR-triggered antimicrobial photodynamic therapy (PDT) by lanthanide-doped upconversion nanoparticles (UCNP) as energy donor exhibits the advantages of high tissue penetration, broad antibacterial spectrum and less acquired resistance, but is still limited by its low efficacy. Now we designed a bio-inorganic nanohybrid and combined lysozyme (LYZ) with UCNP-PDT system to enhance the efficiency against resistant bacteria. Benefiting from the rapid adhesion to bacteria, intelligently bacteria-responsive LYZ release and synergistic LYZ-PDT effect, the nanoplatform achieves an exceptionally strong bactericidal capacity and conspicuous bacteriostasis on methicillin-resistant S. aureus. These findings pave the way for designing efficiently antibacterial nanomaterials and provide a new strategy for combating deep-tissue bacterial infection.

关键词： antibacterial agents enzymes mesoporous materials photodynamic therapy upconversion nanoparticles

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Fully Aromatic Self-Assembled Hole-Selective Layer toward Efficient Inverted Wide-Bandgap Perovskite Solar Cells with Ultraviolet Resistance

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Angewandte Chemie 2023年第1期136卷

作者： Chi Li Zilong Zhang Huifeng Zhang Wenlong Yan Yuheng Li Lusheng Liang Wei Yu Xuteng Yu Yao Wang Prof. Ye Yang Prof. Mohammad Khaja Nazeeruddin Prof. Peng Gao 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 Fuzhou Fujian 350002 China Laboratory for Advanced Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 China University of Chinese Academy of Sciences Beijing 100049 China Contribution: Writing - original draft (lead) Contribution: Writing - original draft (equal) State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China Contribution: Methodology (lead) Contribution: Investigation (equal) Contribution: Software (lead) Contribution: Data curation (equal) Contribution: Resources (equal) Group for Molecular Engineering of Functional Materials Institute of Chemical Sciences and Engineering École Polytechnique Fedérale de Lausanne Peshawar 1951 Sion Switzerland Contribution: Methodology (equal)

Ultraviolet-induced degradation has emerged as a critical stability concern impeding the widespread adoption of perovskite solar cells (PSCs), particularly in the context of phase-unstable wide-band gap perovskite films. This study introduces a novel approach by employing a fully aromatic carbazole-based self-assembled monolayer, denoted as (4-(3,6-dimethoxy-9H-carbazol-9-yl)phenyl)phosphonic acid (MeO-PhPACz), as a hole-selective layer (HSL) in inverted wide-band gap PSCs. Incorporating a conjugated linker plays a pivotal role in promoting the formation of a dense and highly ordered HSL on substrates, facilitating subsequent perovskite interfacial interactions, and fostering the growth of uniform perovskite films. The high-quality film could effectively suppress interfacial non-radiative recombination, improving hole extraction/transport efficiency. Through these advancements, the optimized wide-band gap PSCs, featuring a band gap of 1.68 eV, attain an impressive power conversion efficiency (PCE) of 21.10 %. Remarkably, MeO-PhPACz demonstrates inherent UV resistance and heightened UV absorption capabilities, substantially improving UV resistance for the targeted PSCs. This characteristic holds significance for the feasibility of large-scale outdoor applications.

关键词： Carbazole Hole-Selective Layer Self-Assembled Monolayer UV Resistance Wide-Bandgap Perovskite

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Moisture-Resistant Mn4+-Doped Core-Shell Structured Fluoride Red Phosphor Exhibiting High Luminous Efficacy for Warm White LEDs

Moisture-Resistant Mn4+-Doped Core-Shell Structured Fluoride...

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中国化学会第十届全国无机化学学术会议

作者： Decai Huang Haomiao Zhu Zhonghua Deng Qilin Zou Hongyu Lu Xiaodong Yi Wang Guo Canzhong Lu 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 Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences University of the Chinese Academy of Sciences

KTiF:Mn is a highly efficient narrow-band emission red phosphor with promising applications in white LEDs and wide-gamut displays.[1-3] Nevertheless, the poor moisture-resistant property of this material hinders its further commercialization. Herein, we introduce a convenient reverse cation exchange strategy to construct a core-shell structured KTiF:Mn@KTiF phosphor. As a result, a high internal photoluminescence quantum yield of 93% is achieved for the sample with the Mn concentration of 7 at.%.The packaged white LED by employing this sample asred phosphor exhibits an extraordinarily high luminous efficacy of 162 lm W, a CCT of 3510 K and a color rendering index of 93（Ra）. Particularly, the aging tests performed on this device at 85 ℃ and 85% humidity for 480 h show that the luminous efficacy retains as high as 89% with respect to its initial value. These findings demonstrate a substantial advance towards the commercial application of KTiF:Mn@KTiF phosphor.

关键词： light-emitting diodes phosphors cation exchange photoluminescence Mn4+

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Scalable Synthesis of Tungsten Disulfide Nanosheets for Alkali-Acid Electrocatalytic Sulfion Recycling and H2Generation

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Angewandte Chemie 2021年第39期133卷

作者： Luocai Yi Yaxin Ji Ping Shao Dr. Junxiang Chen Junwei Li Hao Li Kai Chen Xinxin Peng Prof. Zhenhai Wen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 P. R. China College of Chemistry and Materials Science Fujian Normal University Fuzhou 350007 China University of Chinese Academy of Science Beijing 100049 China

WS 2 nanosheets hold great promise for a variety of applications yet faces a grand challenge in terms of large-scale synthesis. We report a reliable, scalable, and high-yield (>93 %) synthetic strategy to fabricate WS 2 nanosheets, which exhibit highly desirable electrocatalytic properties toward both the alkaline sulfion (S 2− ) oxidation reaction (SOR) and the acidic hydrogen evolution reaction (HER). The findings prompted us to develop a hybrid alkali-acid electrochemical cell with the WS 2 nanosheets as bifunctional electrode catalysts of alkaline anodic SOR and acidic cathodic HER. The proof-of-concept device holds promise for self-power or low-electricity electrolytic H 2 generation and environmentally friendly recycling of sulfion with enhanced electron utilization efficiency.

关键词： hydrogen evolution reaction molten salt synthesis sulfide oxidation reaction WS2 nanosheets

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Metal–Organic Cages with {SiW9Ni4} Polyoxotungstate Nodes

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Angewandte Chemie 2022年第19期134卷

作者： Qing Chang Xiangyu Meng Wenjun Ruan Yeqin Feng Rui Li Jiayu Zhu Prof. Yong Ding Prof. Hongjin Lv Prof. Wei Wang Prof. Guanying Chen Prof. Xikui Fang MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 China State Key Laboratory of Applied Organic Chemistry Key Laboratory of Advanced Catalysis of Gansu Province College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 China MOE Key Laboratory of Cluster Science School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing 102488 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Xiamen Institute of Rare Earth Materials Haixi Institutes Chinese Academy of Sciences Xiamen Fujian 361021 China

A tritopic, Ni-substituted Keggin cluster, {SiW 9 Ni 4 }, assembles with rigid dicarboxylate linkers to give rise to a set of discrete, POM 2 n L 3 n -type structures (POM={SiW 9 Ni 4 }) with defined interior voids. The outcome of coordination-driven self-assemblies of these polyhedral cages—from fused dimers to trigonal prisms—was found to be sensitive to bend angles of the ditopic ligands, which vary from 122° to 180°. These polyoxotungstate-based metal–organic polyhedra, when coupled with [Ru(bpy) 3 ]Cl 2 as a photosensitizer and triethanolamine as the electron donor, serve as highly effective catalysts for CO 2 reduction, with turnover numbers up to 328 and CO selectivity as high as 96.2 %. The inner cavities of such cage structures, if functionalized or of sufficient size to encapsulate targeted guest molecules, could present a new strategy towards functional materials for potential applications.

关键词： CO2 Photoreduction Metal–Organic Polyhedra Nickel Polyoxometalates Self-assembly

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{Mo126W30}: Polyoxometalate Cages Shaped by π–π Interactions

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Angewandte Chemie 2022年第50期134卷

作者： Dr. Minghui Zhu Shicheng Han Junrui Liu Mengjin Tan Prof. Dr. Wei Wang Prof. Dr. Kosuke Suzuki Prof. Dr. Panchao Yin Prof. Dr. Debin Xia Prof. Dr. Xikui Fang MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 China 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 Fuzhou 350002 China Department of Applied Chemistry School of Engineering The University of Tokyo 7-3-1 Hongo Bunkyo-ku Tokyo 113-8656 Japan South China Advanced Institute for Soft Matter Science and Technology State Key Laboratory of Luminescent Materials and Devices South China University of Technology Guangzhou 510640 China

Here we report the formation of giant {Mo 126 W 30 } polyoxometalate cages templated by π-conjugated planar ligands. Their inorganic shells incorporate arrays of 18 stacked aromatic carboxylates, such as 1,3,5-benzenetricarboxylate or 5-nitroisophthalate, and the assembly is stabilized by multiple π–π interactions. NMR data confirmed that the cages are stable in solution and the inner aromatic templates can be postsynthetically replaced by selected aliphatic dicarboxylates, paving the way for endo-functionalization and exploration of the reactivities within the cage cavities.

关键词： π Interactions Cage Compounds Ligand Exchange NMR Spectroscopy Polyoxometalates

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Selective Oxidative Coupling of Methane to Ethylene in a Solid Oxide Electrolyser Based on Porous Single-Crystalline CeO2Monoliths

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Angewandte Chemie 2022年第32期134卷

作者： Lingting Ye Zhibo Shang Prof. Dr. Kui Xie Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Key Laboratory of Design & Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North Road Huizhou Guangdong 116023 China

Catalytic conversion of CH 4 to C 2 H 4 plays an important role in the light olefin industry. Here, we report the electrochemical conversion of CH 4 to C 2 H 4 /C 2 H 6 at the anode with the electrolysis of CO 2 to CO at the cathode in a solid oxide electrolyser. We constructed well-defined interfaces that function as three-phase boundaries by exsolving single-crystalline Ni nanoparticles in porous single-crystalline CeO 2 monoliths. We engineered the chemical states and flux of active oxygen species for the oxidation of CH 4 at the anode by controlling voltage and temperature. We show the unprecedented C 2 selectivity (C 2 H 4 and C 2 H 6 ) of ≥99.5 % at a CH 4 conversion of ≈7 %. The electrolyser exhibits excellent durability without performance degradation being observed in a continuous operation of 100 hours. Our work enables a novel path for the selective conversion of CH 4 /CO 2 into useful chemicals, and the technique of building well-defined interfaces may find potential applications in other fields.

关键词： Carbon Dioxide Ceria Interfaces Methane Porosity

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Resolving the Origins of Superior Cycling Performance of Antimony Anode in Sodium-ion Batteries: A Comparison with Lithium-ion Batteries

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Angewandte Chemie 2024年第11期136卷

作者： Ruiwen Shao Zhefei Sun Lei Wang Jianhai Pan Luocai Yi Yinggan Zhang Jiajia Han Zhenpeng Yao Jie Li Zhenhai Wen Shuangqiang Chen Shu-Lei Chou Dong-Liang Peng Qiaobao Zhang Beijing Advanced Innovation Center for Intelligent Robots and Systems School of Medical Technology Beijing Institute of Technology Beijing China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen Fujian 361005 China Institute for Carbon Neutralization College of Chemistry and Materials Engineering Wenzhou University Wenzhou 325035 China Department of Chemical Engineering School of Environmental and Chemical Engineering Shanghai University Shangda Road 99 Shanghai 200444 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Center of Hydrogen Science Shanghai Jiao Tong University Shanghai China State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai China Department of Energy Politecnico di Milano Via Lambruschini 4 20156 Milano Italy

Alloying-type antimony (Sb) with high theoretical capacity is a promising anode candidate for both lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs). Given the larger radius of Na + (1.02 Å) than Li + (0.76 Å), it was generally believed that the Sb anode would experience even worse capacity degradation in SIBs due to more substantial volumetric variations during cycling when compared to LIBs. However, the Sb anode in SIBs unexpectedly exhibited both better electrochemical and structural stability than in LIBs, and the mechanistic reasons that underlie this performance discrepancy remain undiscovered. Here, using substantial in situ transmission electron microscopy, X-ray diffraction, and Raman techniques complemented by theoretical simulations, we explicitly reveal that compared to the lithiation/delithiation process, sodiation/desodiation process of Sb anode displays a previously unexplored two-stage alloying/dealloying mechanism with polycrystalline and amorphous phases as the intermediates featuring improved resilience to mechanical damage, contributing to superior cycling stability in SIBs. Additionally, the better mechanical properties and weaker atomic interaction of Na−Sb alloys than Li−Sb alloys favor enabling mitigated mechanical stress, accounting for enhanced structural stability as unveiled by theoretical simulations. Our finding delineates the mechanistic origins of enhanced cycling stability of Sb anode in SIBs with potential implications for other large-volume-change electrode materials.

关键词： Antimony anode Lithium-ion batteries Sodium-ion batteries In situ transmission electron microscopy Electrochemical performance

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Wide-field decodable orthogonal fingerprints of single nanoparticles unlock multiplexed digital assays

arXiv

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arXiv 2020年

作者： Liao, Jiayan Zhou, Jiajia Song, Yiliao Liu, Baolei Chen, Yinghui Wang, Fan Chen, Chaohao Lin, Jun Chen, Xueyuan Lu, Jie Jin, Dayong Faculty of Science University of Technology Sydney NSW2007 Australia Centre for Artificial Intelligence Faculty of Engineering and IT University of Technology Sydney NSW2007 Australia State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun130022 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences FuzhouFujian350002 China UTS-SUStech Joint Research Centre for Biomedical Materials & Devices Department of Biomedical Engineering Southern University of Science and Technology Shenzhen China

The control in optical uniformity of single nanoparticles and tuning their diversity in orthogonal dimensions, dot to dot, holds the key to unlock nanoscience and applications. Here we report that the time-domain emissive profile from single upconversion nanoparticle, including the rising, decay and peak moment of the excited state population (2 profile), can be arbitrarily tuned by upconversion schemes, including interfacial energy migration, concentration dependency, energy transfer, and isolation of surface quenchers. This allows us to significantly increase the coding capacity at the nanoscale. We exemplify that at least three orthogonal dimensions, including the excitation wavelength, emission colour and 2 profiles, can be built into the nanoscale derivative 2-Dots. We further implement both time-resolved wide-field imaging and deep-learning techniques to decode these fingerprints, showing high accuracies at high throughput. This work reveals a vast library of individually preselectable nano-tags, and our ability for controlling the uniformity and diversity "at the bottom". These high-dimensional optical fingerprints provide a new horizon for applications spanning from sub-diffraction-limit data storage, security inks, to high-throughput single-molecule digital assays and super-resolution imaging. © 2020, CC-BY.

关键词： Excited states

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