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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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{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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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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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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Perovskite Sr_(0.9)Fe_(0.9)Zr_(0.1)O_(3-delta)：Redox-stable Structure, Oxygen Vacancy, Electrical Properties and Steam Electrolysis Performance

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结构化学 2018年第1期 65-74页

作者： Li Zhe Ye Lingting Xie Kui 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 MatterChinese Academy of Sciences

Many researchers have studied on perovskite oxide for its unique *** oxides,ABO3-δ,with different A and B metals have shown wide applications in many fields,in particular solid oxide ***3-δ,typical perovskite oxides,in which iron is the mixed-valence cation with the capacity to change the chemical valence,have a wide range of oxygen *** this study,Sr0.9Fe0.9Zr0.1O3-δ（SFZO） is synthesized and then treated in 5%H2/Ar and air at high temperature,exhibiting excellent redox ***-stable structure,oxygen vacancy and electrical properties of SFZO are *** electrolysis is then performed with SFZO cathode under 5%H2O/5%H2/Ar and 5%H2O/Ar atmospheres,*** present results indicate that the SFZO is a novel promising cathode material for solid oxide steam electrolyser.

关键词： phase structure solid oxide electrolyser Sr0.9Fe0.9Zr0.1O3-δ cathode steam electrolysis

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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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Ultra-Small Air-Stable Triplet-Triplet Annihilation Upconversion Nanoparticles for Anti-Stokes Time-Resolved Imaging

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Angewandte Chemie 2023年第47期135卷

Image contrast is often limited by background autofluorescence in steady-state bioimaging microscopy. Upconversion bioimaging can overcome this by shifting the emission lifetime and wavelength beyond the autofluorescence window. Here we demonstrate the first example of triplet-triplet annihilation upconversion (TTA-UC) based lifetime imaging microscopy. A new class of ultra-small nanoparticle (NP) probes based on TTA-UC chromophores encapsulated in an organic–inorganic host has been synthesised. The NPs exhibit bright UC emission (400–500 nm) in aerated aqueous media with a UC lifetime of ≈1 μs, excellent colloidal stability and little cytotoxicity. Proof-of-concept demonstration of TTA-UC lifetime imaging using these NPs shows that the long-lived anti-Stokes emission is easily discriminable from typical autofluorescence. Moreover, fluctuations in the UC lifetime can be used to map local oxygen diffusion across the subcellular structure. Our TTA-UC NPs are highly promising stains for lifetime imaging microscopy, affording excellent image contrast and potential for oxygen mapping that is ripe for further exploitation.

关键词： Fluorescence Lifetime Imaging Microscopy Nanoparticles Triplet-Triplet Annihilation Upconversion

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Facile preparation of Ce enhanced vinyl-functionalized silica aerogel-like monoliths for selective separation of radioactive thorium from monazite

Facile preparation of Ce enhanced vinyl-functionalized silic...

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稀土元素镧铈钇应用研究研讨会暨广东省稀土产业技术联盟成立大会

作者： Hao Zhang Fan Yang Ruixi Bai Zhigang Zhao Chunqing Cai Jianguo Li Ying Ma 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 Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences University of Chinese Academy of Sciences Baotou Research Institute of Rare Earths

Thorium(Th) is an associated ore of rare earth metals that is radioactive and harmful to the environment, but it is also a potential nuclear fuel replacement for uranium. The separation of Th from rare earth elements(REEs) is of great importance in environmental governance and clean-energy development. In this work, a monolithic cerium(Ce) doped silica aerogel-like with flexibility was synthesized using a low consumption and rapid technique, and it was used in a continuous solid-phase extraction as an adsorbent for the selective separation of Th/REEs. The batch adsorption experiments showed that the adsorption efficiency of Th(IV) can be up to 96% when abnormally high levels of metal ions(20 ppm) exist. Under the same conditions, the adsorption efficiency of REEs is at a near-zero level, which demonstrates the great selective separation of Th/REEs for the aerogel-like. The results also indicated that Th(IV) could desorb from the adsorbent in weak acidic media, which is friendly to the environment. Therefore, the material has application prospects for the separation of Th/REEs and removal of radioactive contamination from the environment.

关键词： silica aerogel-like monoliths selective adsorption rare earth thorium monazite

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