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Soluble porous organic cages as homogenizers and electron-acceptors for homogenization of heterogeneous alloy nanoparticle catalysts with enhanced catalytic activity

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science Bulletin 2022年第23期67卷 2428-2437,M0004页

作者： Hele Guo Yali Liu Hongliang Dong Wei Zong Kaibin Chu Weiwei Li Zhongli Fan Guanjie He Yue-E Miao Ivan P.Parkin Feili Lai Tianxi Liu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringInternational Joint Research Laboratory for Nano Energy CompositesJiangnan UniversityWuxi 214122China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China Department of Chemistry KU LeuvenLeuven 3001Belgium Center for High Pressure Science and Technology Advanced Research Shanghai 201203China Christopher Ingold Laboratory Department of ChemistryUniversity College LondonLondon WCiH OAJUK Department of Chemical Engineering University College LondonLondon WCiE 7JEUK Department of Molecular Spectroscopy Max Planck Institute for Polymer ResearchMainz 55128Germany

The creation of ultrafine alloy nanoparticles(<5 nm) that can maintain surface activity and avoid aggregation for heterogeneous catalysis has received much attention and is extremely ***,ultrafine PtRh alloy nanoparticles imprisoned by the cavities of reduced chiral covalent imine cage(PtRh@RCC3) are prepared successfully by an organic molecular cage(OMC) confinement strategy,while the soluble RCC3 can act as a homogenizer to homogenize the heterogeneous PtRh alloy in ***,the X-ray absorption near-edge structure(XANES) results show that the RCC3 can act as an electron-acceptor to withdraw electrons from Pt,leading to the formation of higher valence Pt atoms,which is beneficial to improving the catalytic activity for the reduction of *** to the synergistic effect of Pt/Rh atoms and the unique function of the RCC3,the reaction rate constants of Pt_(1)Rh_(16)@RCC3 are 49.6,8.2,and 5.5 times than those of the Pt_(1)Rh_(16)bulk,Pt@RCC3 and Rh@RCC3,*** work provides a feasible strategy to homogenize heterogeneous alloy nanoparticle catalysts in solution,showing huge potential for advanced catalytic application.

关键词： Soluble organic cage Heterogeneous catalysts Ultrafine alloy nanoparticle 4-Nitrophenol reduction reaction

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A metabolic acidity-activatable calcium phosphate probe with fluorescence signal amplification capabilities for non-invasive imaging of tumor malignancy

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science Bulletin 2022年第3期67卷 288-298页

作者： Qian Jia Ruili Zhang Yongdong Wang Haohao Yan Zheng Li Yanbin Feng Yu Ji Zuo Yang Yang Yang Kanyi Pu Zhongliang Wang Laboratory of Molecular Imaging and Translational Medicine(MITM) Engineering Research Center of Molecular&NeuroimagingMinistry of EducationSchool of Life Science and TechnologyXidian UniversityXi’an 710126China Academy of Advanced Interdisciplinary Research Xidian UniversityXi’an 710071China Department of Thoracic Surgery Shanghai Pulmonary HospitalSchool of MedicineTongji UniversityShanghai 200433China School of Materials Science and Engineering Tongji UniversityShanghai 201804China School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingapore 637457Singapore

Dysregulated energy metabolism has recently been recognized as an emerging hallmark of *** cells,which are characterized by abnormal glycolysis,exhibit a lower extracellular pH(6.5–7.0)than nor-mal tissues(7.2–7.4),providing a promising target for tumor-specific imaging and ***,most pH-sensitive materials are unable to distinguish such a subtle pH difference owing to their wide and continuous pH-responsive *** this study,we developed an efficient strategy for the fabrication of a tumor metabolic acidity-activatable calcium phosphate(CaP)fluorescent probe(termed MACaP9).Unlike traditional CaP-based biomedical nanomaterials,which only work within more acidic organelles,such as endosomes and lysosomes(pH 4.0–6.0),MACaP9 could not only specifically respond to the tumor extra-cellular pH but also rapidly convert pH variations into a distinct fluorescence signal to visually dis-tinguish tumor from normal *** superior sensitivity and specificity of MACaP9 enabled high-contrast visualization of a broad range of tumors,as well as small tumor lesions.

关键词： Calcium phosphate Activatable probe Cancer imaging Tumor microenvironment Tumor metabolism

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Tailoring the interface of WS₂ nanoparticles by photo-initiator for radiation curing and reinforcement of nano-structured acrylates

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Nano-Structures and Nano-Objects 2023年 36卷

作者： Yosef Tal, N. Dodiuk, H. Amir, E. Brontvein, O. Tenne, R. Kenig, S. Department of Polymer Materials Engineering Shenkar Collage Ramat-Gan 5252626 Israel Department of Chemical Research Support Weizmann Institute Rehovot 7610001 Israel Department of Molecular Chemistry and Materials Science Weizmann Institute Rehovot 7610001 Israel

Surface modification of tungsten disulfide (WS2) nanoparticles (NPs) by a photo-initiator (PI) for radical curing of acrylate nano-structured systems has been studied with the purpose of acquiring covalent bonding of ... 详细信息

Surface modification of tungsten disulfide (WS₂) nanoparticles (NPs) by a photo-initiator (PI) for radical curing of acrylate nano-structured systems has been studied with the purpose of acquiring covalent bonding of the acrylate matrix to the NPs surface. This surface functionalization was expected to photosensitize both the PI and the NPs thereby enhance the photocuring of the acrylate as well as improving its mechanical properties. The studied PI was the commonly used Bis(acyl) phosphane oxides (BAPOs). For surface modification of the WS₂ NPs, the BAPO was functionalized first with Tri(methoxy) silane (TMESI) to yield TMESI-BAPO moieties. Subsequently, the functionalized BAPO was chemisorbed to the WS₂ NPs resulting in WS₂ NPs surface modified by TMESI-BAPO pendant moieties. The functionalization and surface modification were confirmed using spectroscopic techniques as well as electron microscopy, and thermal measurements. Thermal gravimetric analysis (TGA) displayed 40 wt% weight loss for TMESI-BAPO modified WS₂ upon heating to 400 °C. The modified WS₂ NPs were incorporated into acrylate resin to study the curing kinetics and resulting mechanical properties compared to neat WS₂. Nanostructured acrylate with TEMSI-BAPO modified WS₂ NPs exhibited an increase of 83% in storage modulus and toughness compared to neat acrylate. © 2023 Elsevier B.V.

关键词： BAPO Interface Nanostructured acrylates Photo-initiator Radiation curing Surface modification WS2 Nanoparticles

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Synthesis and Electrochemical Properties of Two Cobalt(Ii) and Nickel(Ii) Metal-Organic Frameworks for Excellent Performance Supercapacitors

SSRN

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SSRN 2024年

作者： Wang, Xiao-Qing Zhu, Hongli Wang, Xiangting Yang, Jie Xu, Pengye Ling, Liaoxuan Jiao, Jingjing Department of Chemistry School of Chemistry and Chemical Engineering North University of China Taiyuan030051 China Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical Engineering Liaocheng University Liaocheng252000 China School of Materials Science and Engineering North University of China Taiyuan030051 China Shanghai Municipal Education Committee Key Laboratory of Molecular Imaging Probes and Sensors Shanghai Normal University Shanghai200234 China

Two novel metal-organic frameworks, [Co(HNTB)(bif)]·3H2O·DMA (1) and [(Ni2(μ2-O)(HNTB)2(bif)2]·2H2O·2H3O·2DMA (2), have been obtained based on a tripod-type carboxylic ligand (4,4',4"-Nitrilotrisbenzoic acid, H3NTB) and a rigid N-donor ligand (2,7-bis(1-imidazoly)fluorene, bif) by solvothermal method. The single-crystal X-ray diffraction results indicate that complex 1 exhibits a 2D layered structure and 2 is a 3D microporous structure with an anionic skeleton. Significantly, their electrochemical tests show that both of them own excellent capacitive performance. Complex 1 has a relatively high specific capacitance (301.2 F g-1 at 1 A g-1) with favorable cycling durability (retained 73.2% over 3000 cycles). Complex 2 exhibits a high specific capacitance (329.6 F g-1 at 1 A g-1) with a relatively poor cycling durability (retained 58.9% over 3000 cycles). Additionally, an asymmetrical ultra-capacitor with MOF as positive electrode and activated carbon (AC) as negative electrode was assembled. Complex 1 // AC exhibits a maximum energy density of 20.9 Wh kg-1 at 800.0 W kg-1 and a high cycle stability ( retained 89.2% over 8000 cycles). Complex 2 // AC owns an energy density of 19.3 Wh kg-1 at 750.0 W kg-1 and a satisfactory cycle stability ( retained 88.6% over 8000 cycles). © 2024, The Authors. All rights reserved.

关键词： Supercapacitor

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Highly Stable Silicon Anodes Enabled by Sub-10 nm Pores and Particles

arXiv

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arXiv 2025年

作者： Ghildiyal, Pankaj Wagner, Brandon Chen, Jianjun Nguyen, Tu Belamkar, Aishwarya Guo, Juchen Mangolini, Lorenzo SiLi-ion Inc. Multidisciplinary Research Building 3401 Watkins Dr RiversideCA92507 United States Materials Science and Engineering Program University of California Riverside RiversideCA92521 United States Department of Chemical and Environmental Engineering University of California Riverside RiversideCA92521 United States Department of Mechanical Engineering University of California Riverside RiversideCA92521 United States

Silicon anodes offer high energy densities for next-generation lithium-ion batteries;however, their application is limited by severe volume expansion during cycling. Making silicon porous or nanostructured mitigates this expansion but often increases lithium inventory losses due to the inherent high surface area of nanomaterials. This study introduces a simple bottom-up process that overcomes this limitation. The approach relies on small silicon particles (-3), all while maintaining good processability. The resulting silicon-dominant anodes achieve remarkable stability in full pouch cells with NMC811 and LFP cathodes, retaining ~80% capacity for more than 400 cycles without pre-lithiation, graphite blending, or pre-cycling. © 2025, CC BY.

关键词： Lithium-ion batteries

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Creating Continuously Graded Microstructures with Electric Fields via Locally Altering Grain Boundary Complexions

arXiv

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arXiv 2023年

作者： Yan, Qizhang Hu, Chongze Luo, Jian Department of Nano and Chemical Engineering University of California San Diego La Jolla CA92093 United States Program in Materials Science and Engineering University of California San Diego La Jolla CA92093 United States Department of Aerospace Engineering and Mechanics University of Alabama TuscaloosaAL35487 United States

Tailoring microstructures represents a daunting goal in materials science. Here, an innovative proposition is to utilize grain boundary (GB) complexions (a.k.a. interfacial phases) to manipulate microstructural evolution, which is challenging to control via only temperature and doping. Herein, we use ZnO as a model system to tailor microstructures using applied electric fields as a new knob to control GB structures locally via field-driven stoichiometry (defects) polarization. Specifically, continuously graded microstructures are created under applied electric fields. By employing aberration-corrected scanning transmission electron microscopy (AC STEM) in conjunction with density functional theory (DFT) and ab initio molecular dynamics (AIMD), we discover cation-deficient, oxygen-rich GBs near the anode with enhanced GB diffusivities. In addition, the field-driven redistribution of cation vacancies is deduced from a defect chemistry model, and subsequently verified by spatially resolved photoluminescence spectroscopy. This bulk stoichiometry polarization leads to preferential formation of cation-deficient (oxidized) GBs near the anode to gradually promote grain growth towards the anode. This mechanism can be utilized to create continuously graded microstructures without abnormal grain growth typically observed in prior studies. This study exemplifies a case of tailoring microstructural evolution via altering GB complexions locally with applied electric fields, and it enriches fundamental GB science. © 2023, CC BY.

关键词： Density functional theory

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High-Performance Silicon Anodes Enabled by Multifunctional Ultrafine Silica Nanoparticle-Embedded Carbon Coatings for Lithium-Ion Batteries

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Advanced Energy materials 2025年第0期

作者： Sun, Zhefei Yin, Quanzhi Zhou, Shenghui Chen, Haoyu Wen, Sifan Yang, Huiping Wu, Xiaoyu Pan, Jianhai Han, Jiajia Yang, Hui Zhuang, Zilong Feng, Shijie Zhang, Li Peng, Dong-Liang Zhang, Qiaobao State Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen361005 China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Tan Kah Kee Innovation Laboratory Collaborative Innovation Center of Chemistry for Energy Materials Xiamen University Fujian Xiamen361005 China State Key Laboratory of Material Processing and Die & Mould Technology Department of Mechanics School of Aerospace Engineering Huazhong University of Science and Technology Hubei Wuhan430074 China Department of Mechanical Engineering University of Wisconsin-Madison MadisonWI53706 United States Materials Science and Engineering Program University of California San Diego La JollaCA92093 United States Longmen Laboratory Henan Luoyang471023 China

Silicon (Si) holds immense promise as viable anode for next-generation high-energy-density Li-ion batteries (LIBs). However, its poor ionic/electronic conductivity and significant volumetric changes during cycling lead to rapidly deteriorated LIB performance. Here, a novel multifunctional coating featuring ultrafine SiO2 nanoparticles (2-C) to resolve these challenges is proposed. This unique uSiO2-C coating provides high-efficient electron and ion transport pathways, while also improves interfacial stability and mitigates volume changes during cycling, thereby enhancing the conductivity and structural integrity of Si@uSiO2-C, as corroborated by extensive experimental and computational studies. In addition, the abundant interfaces in uSiO2-C coating facilitate Li+ transport and the evenly distributed ultrafine SiO2 nanoparticles impart high electrochemical reactivity and mechanical robustness. Consequently, the Si@uSiO2-C anode achieves a high reversible capacity of 2093 mAh g−1 at 0.2 A g−1, with a high initial Coulombic efficiency of 88.3%, superior rate capability and durability (1000 cycles, 928 mAh g−1 at 1.0 A g−1, 75% capacity retention). Full cells paired with commercial LiFePO4 cathodes demonstrate high cyclability, maintaining 80% capacity retention over 500 cycles at 4 C. This work highlights the vital role of multifunctional coating in promoting the electrochemical performance of Si-based anodes for high-performance LIBs. © 2025 Wiley-VCH GmbH.

关键词： SiO2 nanoparticles

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Vibrational properties differ between halide and chalcogenide perovskite semiconductors, and it matters for optoelectronic performance

arXiv

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arXiv 2024年

作者： Ye, Kevin Menahem, Matan Salzillo, Tommaso Knoop, Florian Zhao, Boyang Niu, Shanyuan Hellman, Olle Ravichandran, Jayakanth Jaramillo, Rafael Yaffe, Omer Department of Materials Science and Engineering Massachusetts Institute of Technology CambridgeMA02139 United States Department of Chemical and Biological Physics Weizmann Institute of Science Rehovot76100 Israel Department of Industrial Chemistry University of Bologna Bologna Italy Linköping University LinköpingSE-581 83 Sweden Mork Family Department of Chemical Engineering and Materials Science University of Southern California Los AngelesCA90089 United States Department of Molecular Chemistry and Material Science Weizmann Institute of Science Rehovot76100 Israel Ming Hsieh Department of Electrical and Computer Engineering University of Southern California Los AngelesCA90089 United States University of Southern California Los AngelesCA90089 United States

We report a comparative study of temperature-dependent photoluminescence and structural dynamics of two perovskite semiconductors, the chalcogenide BaZrS3 and the halide CsPbBr3. These materials have similar crystal structures and direct band gaps, but we find that they have quite distinct optoelectronic and vibrational properties. Both materials exhibit thermally-activated non-radiative recombination, but the non-radiative recombination rate in BaZrS3 is four orders-of-magnitude faster than in CsPbBr3, for the crystals studied here. Raman spectroscopy reveals that the effects of phonon anharmonicity are far more pronounced in CsPbBr3 than in BaZrS3. Further, although both materials feature a large dielectric response due to low-energy polar optical phonons, the phonons in CsPbBr3 are substantially lower in energy than in BaZrS3. Our results suggest that electron-phonon coupling in BaZrS3 is more effective at non-radiative recombination than in CsPbBr3, and that BaZrS3 may also have a substantially higher concentration of non-radiative recombination centers than CsPbBr3. The low defect concentration in CsPbBr3 may be related to the ease of lattice reconfiguration, typified by anharmonic bonding. It remains to be seen to what extent these differences are inherent to the chalcogenide and halide perovskites and to what extent they can be affected by materials processing. © 2024, CC BY.

关键词： Raman spectroscopy

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Lithium-ion battery functionality over broad operating conditions via local high concentration fluorinated ester electrolytes

RSC Applied Interfaces

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RSC Applied Interfaces 2024年第5期1卷 1077-1092页

作者： Quilty, Calvin D. Marin Bernardez, Edelmy J. Nicoll, Andrew Hossain, MD Jamil Kingan, Arun Arnot, David J. Mohamed, Hafsa A. Tong, Xiao Jaye, Cherno Fischer, Daniel A. Wang, Lei Qi, Yue Takeuchi, Esther S. Marschilok, Amy C. Yan, Shan Bock, David C. Takeuchi, Kenneth J. Department of Chemistry Stony Brook University Stony Brook 11794 NY United States Institute of Energy: Sustainability Environment and Equity (I:SEE) Stony Brook University Stony Brook 11794 NY United States School of Engineering Brown University Providence 02912 RI United States Department of Materials Science and Chemical Engineering Stony Brook University Stony Brook 11794 NY United States Science Undergraduate Laboratory Internship (SULI) Program Brookhaven National Laboratory Upton 11973 NY United States Department of Chemistry University of Rochester Rochester 14627 NY United States Department of Chemistry The College of Wooster Wooster 44691 OH United States Center for Functional Nanomaterials Brookhaven National Laboratory Upton 11973 NY United States Material Measurement Laboratory National Institute of Standards and Technology Gaithersburg 20899 MD United States Interdisciplinary Science Department Brookhaven National Laboratory Upton 11973 NY United States

Facilitating widespread adoption of electric vehicles will require next-generation battery systems that can operate reliably over a large temperature range, at high operating voltage, and under fast charging rates. Herein, a novel class of nonflammable fluorinated ester-based local high concentration electrolytes (LHCEs) are described. When cycled in commercially relevant graphite/LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) pouch cells, these electrolytes demonstrate improved capacity retention compared to carbonate-based electrolytes under multiple usage conditions including high voltage (4.5 V), fast charge (4C, 15 minutes), and low temperature (−20 °C) without sacrificing capacity retention at elevated temperature (40 °C). Low carbon, high fluoride cathode electrolyte interphases formed by the LHCE system yield a significant reduction in charge transfer impedance during cycling and contribute to capacity retention. These results demonstrate that using fluorinated esters in a LHCE modality enables creation of a new class of nonflammable electrolytes that can successfully operate over broad operating conditions. © 2024 RSC.

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Kinetic investigation of the energy storage process in graphene fiber supercapacitors: Unraveling mechanisms,fabrications, property manipulation, and wearable applications

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Carbon Energy 2025年第01期 137-177页

作者： Juan Zhang Wenwen Liu Minzhi Du Qingli Xu Minren Hung Ruifang Xiang Meng Liao Xinhou Wang Bingjie Wang Aiping Yu Kun Zhang Key Laboratory of Textile Science and Technology (Donghua University) Ministry of Education College of Textiles Donghua University Department of Chemical Engineering Waterloo Institute for Nanotechnology University of Waterloo Laboratory of Advanced Materials State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan University College of Mechanical Engineering Donghua University

Graphene fiber supercapacitors(GFSCs) have garnered significant attention due to their exceptional features, including high power density, rapid charge/discharge rates, prolonged cycling durability, and versatile weaving ***, inherent challenges in graphene fibers(GFs), particularly the restricted ion-accessible specific surface area(SSA) and sluggish ion transport kinetics, hinder the achievement of optimal capacitance and rate *** existing reviews on GFSCs, a notable gap exists in thoroughly exploring the kinetics governing the energy storage process in GFSCs. This review aims to address this gap by thoroughly analyzing the energy storage mechanism,fabrication methodologies, property manipulation, and wearable applications of GFSCs. Through theoretical analysis of the energy storage process, specific parameters in advanced GF fabrication methodologies are carefully summarized,which can be used to modulate nano/micro-structures, thereby enhancing energy storage kinetics. In particular, enhanced ion storage is realized by creating more ion-accessible SSA and introducing extra-capacitive components,while accelerated ion transport is achieved by shortening the transport channel length and improving the accessibility of electrolyte ions. Building on the established structure–property relationship, several critical strategies for constructing optimal surface and structure profiles of GF electrodes are summarized. Capitalizing on the exceptional flexibility and wearability of GFSCs, the review further underscores their potential as foundational elements for constructing multifunctional e-textiles using conventional textile technologies. In conclusion, this review provides insights into current challenges and suggests potential research directions for GFSCs.

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