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Metal–Organic Cages with {SiW9Ni4} Polyoxotungstate Nodes

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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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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{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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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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Facile synthesis of quantum sized Co₃O₄ nanostructures and their magnetic properties

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Nano-Structures and Nano-Objects 2018年 15卷 1-9页

作者： Anandhababu, G. Ravi, G. Department of Physics Alagappa University Karaikudi Sivaganga Tamilnadu India 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 YangQiao West Road 155# Fuzhou Fujian 350002 China

We examined the quantum sized Co3O4 formation with hexagonal morphology of diameter about 20 nm. The photoluminescence study proved the surface defect-rich Co3O4 nanostructures. The combined synergistic effect of quan... 详细信息

We examined the quantum sized Co₃O₄ formation with hexagonal morphology of diameter about 20 nm. The photoluminescence study proved the surface defect-rich Co₃O₄ nanostructures. The combined synergistic effect of quantum sized hexagonal nanoplates structures and surface defects are favorable for the enhanced magnetic properties in Co₃O₄ nanostructures. The addition of surfactants and changing of microwave powers led to the paramagnetic behavior. Room temperature magnetic measurements of Ni-doped Co₃O₄ exhibits weak ferromagnetic nature of Co₃O₄ nanostructures. With practical, environmental friendly and solvent-free microwave strategy provides a brand new promising route for large-scale preparation of metal oxide for outstanding magnetic performance. © 2018 Elsevier B.V.

关键词： Defects Magnetization Microwave nanostructures Paramagnetism Photoluminesence

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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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Dually-Passivated Perovskite Solar Cells with Reduced Voltage Loss and Increased Super Oxide Resistance

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Angewandte Chemie 2021年第15期133卷

作者： Qin Zhou Yifeng Gao Chunsheng Cai Zhuangzhuang Zhang Jianbin Xu Prof. Zhongyi Yuan Prof. Dr. Peng Gao 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 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 Institute of Polymers and Energy Chemistry (IPEC) College of Chemistry Nanchang University 999 Xuefu Avenue Nanchang 330031 China

In recent years, the power conversion efficiency (PCE) of perovskite solar cells (PSCs) has witnessed rapid progress. Nevertheless, the pervasive defects prone to non-radiative recombination and decomposition exist at the surface and the grain boundaries (GBs) of the polycrystalline perovskite films. Herein, we report a comprehensive dual-passivation (DP) strategy to effectively passivate the defects at both surface and GBs to enhance device performance and stability further. Firstly, a fluorinated perylene-tetracarboxylic diimide derivative is permeated in the perovskite metaphase during antisolvent treatment, and then a fluorinated bulky aromatic ammonium salt is introduced over the annealed perovskite. The reduction of defect density can be unambiguously proved by the superoxide species generation/quenching reaction. As a result, optimized planar PSCs demonstrate a decreased open-circuit voltages deficit from 0.47 to 0.39 V and the best efficiency of 23.80 % from photocurrent scanning with a stabilized maximum power output efficiency of 22.99 %. Without encapsulation, one typical device can maintain over 85 % of the initial efficiency after heating on a hot plate at 100 °C for 30 h under relative humidity (RH) of 70 %. When the device is aged under 30±5 % RH, over 97 % of its initial PCE is retained after 1700 h.

关键词： defects dual-passivation perovskite solar cells stability superoxide

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Rücktitelbild: Ultra-Small Air-Stable Triplet-Triplet Annihilation Upconversion Nanoparticles for Anti-Stokes Time-Resolved Imaging (Angew. Chem. 47/2023)

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Angewandte Chemie 2023年第47期135卷

作者： Dr. Bolong Zhang Dr. Kieran D. Richards Beatrice E. Jones Abigail R. Collins Rosie Sanders Dr. Sarah R. Needham Dr. Pu Qian Amoghavarsha Mahadevegowda Prof. Caterina Ducati Prof. Stanley W. Botchway Prof. Rachel C. Evans Department of Materials Science and Metallurgy University of Cambridge 27 Charles Babbage Road Cambridge CB3 0FS UK 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 Diamond Light Source Didcot Oxfordshire OX11 0QX UK Central Laser Facility Science and Technology Facilities Council Rutherford Appleton Laboratory Harwell Science and Innovation Campus Oxfordshire OX11 0QX UK Materials and Structural Analysis Thermo Fisher Scientific Achtseweg Noord 5 5651 GG Eindhoven The Netherlands The Faraday Institution Quad One Harwell Science and Innovation Campus Didcot UK

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Back Cover: Ultra-Small Air-Stable Triplet-Triplet Annihilation Upconversion Nanoparticles for Anti-Stokes Time-Resolved Imaging (Angew. Chem. Int. Ed. 47/2023)

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Angewandte Chemie International Edition 2023年第47期62卷

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