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Self-templated formation of cobalt-embedded hollow N-doped carbon spheres for efficient oxygen reduction

Nano Research 2021年第8期14卷 2819-2825页

作者： Ayaz Mahsud Jianian Chen Xiaolei Yuan Fenglei Lyu Qixuan Zhong Jinxing Chen Yadong Yin Qiao Zhang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJoint International Research Laboratory of Carbon-Based Functional Materials and DevicesSoochow University199 Ren’ai RoadSuzhou 215123China School of Chemistry and Chemical Engineering Nantong UniversityNantong9 Seyuan RoadNantong226019China Department of Chemistry Materials Science and Engineering programand UCR Center for CatalysisUniversity of CaliforniaRiversideCA 92521USA

The slow kinetics at the cathode of oxygen reduction reaction(ORR)seriously limits the efficiencies of fuel cells and metal-air ***,the state-of-the-art ORR electrocatalyst,suffers from high cost,low earth abundance,and poor *** a self-templated strategy based on metal-organic frameworks(MOFs)is proposed for the fabrication of hollow nitrogen-doped carbon spheres that are embedded with cobalt nanoparticles(Co/HNC).The Co/HNC manifests better ORR activities,methanol tolerance,and stability than commercial Pt/*** high ORR performance of Co/NHC can be attributed to the hollow structure which provides enlarged electrochemically active surface area,the formation of more Co-N species,and the introduction of *** work highlights the significance of rational engineering of MOFs for enhanced ORR activity and stability and offers new routes to the design and synthesis of high-performance electrocatalysts.

关键词： cobalt self-templated metal organic framework hollow sphere oxygen reduction reaction

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Artificial solid-electrolyte interface facilitating uniform Zn deposition by promoting chemical adsorption

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science China materials 2022年第3期65卷 663-674页

作者： Jingjing Zhang Wei Peng Junhong Jin Shenglin Yang Aishui Yu Guang Li State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China Laboratory of Advanced Materials Institute of New Energy and Department of ChemistryCollaborative Innovation Center of Chemistry for Energy MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghai 200438China

Zn-air batteries are promising energy storage and conversion systems to replace the conventional lithiumbased ***,their applications have been greatly hindered by the formation of Zn dendrites and ZnO passivation layer on the Zn ***,we report the fabrication of an artificial protective layer comprised of N-doped threedimensional hollow porous multi-nanochannel carbon fiber with well-dispersed TiO_(2) nanoparticles(HMCNF).The incorporated TiO;nanoparticles and N dopants improve the ion flux distribution and promote the surface adsorption,facilitating the interfacial pseudocapacitive behaviors during Zn *** hierarchical architecture also induces homogenous electric field distribution at the anode/electrolyte ***,the deposition behavior of Zn is regulated,giving rise to enhanced utilization and rechargeability of *** integrated in alkaline Zn-air batteries,the HMCNF-coated Zn anodes exhibit improved electrochemical performances relative to those with the bare Zn anodes,demonstrating a versatile strategy to boost energy storage of metal anodes through optimizing surface adsorption properties.

关键词： regulated Zn deposition Zn adsorption artificial solid-electrolyte interface Zn anode Zn-air battery

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Air-Processed Efficient Organic Solar Cells from Aromatic Hydrocarbon Solvent without Solvent Additive or Post-Treatment:Insights into Solvent Effect on Morphology

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Energy & Environmental materials 2022年第3期5卷 977-985页

作者： Ruijie Ma Tao Yang Yiqun Xiao Tao Liu Guangye Zhang Zhenghui Luo Gang Li Xinhui Lu He Yan Bo Tang College of Chemistry Chemical Engineering and Materials ScienceKey Laboratory of Molecular and Nano ProbesMinistry of EducationCollaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of ShandongInstitute of Materials and Clean EnergyShandong Provincial Key Laboratory of Clean Production of Fine ChemicalsShandong Normal UniversityJinan 250014China College of New Materials and New Energies Shenzhen Technology UniversityShenzhen 518118 China Department of Chemistry Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional MaterialsEnergy Institute and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration&ReconstructionHong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina Department of Physics Chinese University of Hong KongNew Territories Hong KongChina Hong Kong University of Science and Technology-Shenzhen Research Institute No.9 Yuexing first RDHi-tech ParkNanshanShenzhen 518057China Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and DevicesSouth China University of Technology(SCUT)Guangzhou 510640China

Most of the recent organic solar cells(OSCs)with top-of-the-line efficiencies are processed from organic solvents with a high vapor pressure such as CF in nitrogen-filled glovebox,which is not feasible for large-area ***,we cast active layers with both aromatic hydrocarbon solvents and halogenated solvents without any solvent additive or post-treatment,as well as interlayers with water and methanol in air(35%relative humidity)for efficient OSCs,except cathode electrode's evaporation is in *** to the PM6:Y6 system that is processed from CF,the PM6:BTP-ClBr2 system demonstrates good efficiency of 16.28%processed from CB and the device based on PM6:BTP-4Cl achieves 16.33%using TMB as its solvent for the active *** are among the highest efficiencies for CB-and TMB-processed binary OSCs to *** molecular packing and phase separation length scales of each combination depend strongly on the solvent,and the overall morphology is the result of the interplay between solvent evaporation(kinetics)and materials miscibility(thermodynamics).Different solvents are required to realize the optimal morphology due to the different miscibility between the donor and ***,17.36%efficiency was achieved by incorporating PC71BM for TMB-processed *** result provides insights into the effect of processing solvent and shows the potential of realizing high-performance OSCs in conditions relevant for industrial fabrication.

关键词： air-processing aromatic hydrocarbon solvent efficiency morphology organic solar cells

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An Electrochemical Study of Phthalate Esters – Potential Low-Cost, Nonvolatile, and Oxidatively-Stable Electrolyte Components

SSRN

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SSRN 2023年

作者： Zhao, Yineng Tenhaeff, Wyatt E. Materials Science Program University of Rochester RochesterNY14627 United States Department of Chemical Engineering University of Rochester RochesterNY14627 United States

Electrolytes with low volatility/flammability and high oxidative stability are desirable for safe high-voltage energy storage. Phthalate esters are a class of organic molecules that are low cost, nonvolatile, and much less flammable than commercial liquid electrolytes. They have long been used as plasticizers in polymers and recently were shown to enhance the performance of nitrile-bearing polymer electrolytes, but little is known about their electrochemical properties relevant to energy storage applications. In this work, the thermal and electrochemical stability of phthalate esters employed as liquid electrolyte solvent were comprehensively investigated. Their ionic conductivity and electrochemical stability were reported for the first time. The conductivity of 1M LiTFSI in dimethyl-phthalate (DMP) was 2.1×10-4 S/cm at 25°C and 1.1×10-3 S/cm at 60°C. Significant evaporation was not observed until 147°C in an open environment. The DMP/LiTFSI electrolyte was stable up to 4.8 V vs. Li/Li+, outperforming state-of-the-art liquid electrolytes based on organic carbonates. Such properties are desirable for phthalates as plasticizers in high-voltage polymer/liquid electrolytes. However, it was demonstrated that the phthalates do not form passivating interfacial reaction layers with lithium metal anodes, making them incompatible with unprotected Li metal anodes. © 2023, The Authors. All rights reserved.

关键词： Plasticizers

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表面自由能对二维结晶的影响

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science China materials 2023年第4期66卷 1511-1517页

作者：姚佳荣孙玲杰肖彦玲刘金雨揭建胜刘旭影杨方旭孙雅静李荣金胡文平 Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin University&Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China

二维分子晶体是一类具有优异光电性能的新兴材料.然而,由于人们对决定二维结晶的因素知之甚少,二维分子晶体的生长极具挑战.我们研究了有机半导体的二维结晶和表面自由能之间的关系,提出了利用表面自由能各向异性因子来衡量二维结晶趋... 详细信息

二维分子晶体是一类具有优异光电性能的新兴材料.然而,由于人们对决定二维结晶的因素知之甚少,二维分子晶体的生长极具挑战.我们研究了有机半导体的二维结晶和表面自由能之间的关系,提出了利用表面自由能各向异性因子来衡量二维结晶趋势的设想.以两个BTBT衍生物为例,我们发现具有大的g因子的分子有不受外界条件干扰的二维结晶趋势.这项工作为合理设计可二维结晶的有机半导体提供了指导.

关键词：表面自由能有机半导体分子晶体各向异性因子新兴材料 g因子外界条件光电性能

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Integrating computational and experimental insights into osmolyte-driven activation of Geobacillus kaustophilus L-asparaginase for acrylamide mitigation

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Journal of molecular Liquids 2025年 423卷

作者： Özdemir, F.İnci Servili, Burak Demirtaş, Özge Şükür, Gözde Tülek, Ahmet Yildirim, Deniz Gebze Technical University Department of Molecular Biology and Genetics Kocaeli Gebze41400 Turkey Kadir Has University of Science and Engineering Bioinformatics and Genetics Program İstanbul Fatih35430 Turkey Iğdır University Postgraduate Education Institute Department of Bioengineering and Sciences Iğdır Merkez76000 Turkey Cukurova University Faculty of Ceyhan Engineering Department of Chemical Engineering Adana Ceyhan01950 Turkey

Osmolytes play a critical role in enhancing the stability and activity of enzymes for industrial applications. This study systematically investigated the effects of various osmolytes on the activity, optimal pH, temperature, stability, metal ion effects, storage, and acrylamide mitigation performance of L-asparaginase from the thermophilic Geobacillus kaustophilus (GkASNase). The experimental findings were further supported by computationally integrated tools such as homology modeling, docking, and molecular dynamics (MD) simulations. Among the selected osmolytes (maltose, sorbitol, trehalose, glycine, and sucrose), GkASNase showed the highest stability during 30 days of storage in the presence of maltose and arginine. Maltose increased GkASNase activity approximately 2-fold at 37 °C and 55 °C. In the presence of osmolytes, the Km values of GkASNase decreased and the Vmax values increased compared to controls at 37 °C and 55 °C. In the presence of osmolytes, the acrylamide mitigation performance of GkASNase increased by 1.7-fold in a 15 min reaction. The computational analysis indicates that L-asparagine as substrate enhances protein compactness and stability, while arginine as osmolyte increases flexibility and optimizes water distribution around the enzyme. These findings provide novel insights into enzyme stabilization that have implications for therapeutic and biotechnological applications. © 2025 Elsevier B.V.

关键词： Maltose

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Robust dioxin-linked metallophthalocyanine tbo topology covalent organic frameworks and their photocatalytic properties

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National science Review 2025年第1期 132-145页

作者： Yucheng Jin Qianjun Zhi Hailong Wang Xiaoning Zhan Dongdong Qi Baoqiu Yu Xu Ding Tianying Wang Heyuan Liu Mingxue Tang Jie Liu Jianzhuang Jiang Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry and Chemical Engineering School of Chemistry and Biological Engineering University of Science and Technology Beijing School of Materials Science and Engineering China University of Petroleum (East China) Center for High Pressure Science and Technology Advanced Research

Constructing 3D functional covalent organic frameworks（COFs） with both robust linkage and planar macro cycle building blocks still remains a challenge due to the difficulty in adjusting both the crystallinity and the dominant 2D *** addition,it is also challenging to selectively convert inert C（sp3）-H bonds into value-added ***,robust 3D COFs,USTB-28-M（M=Co,Ni,Cu）,have been polymerized from the nucleophilic aromatic substitution reaction of D3h-symmetric2,3,6,7,14,15-hex ahydroxyltriptycene with D4h-symmetric hexadecafluorophthalocyanine(MPcF16) under solvothermal *** chemically stable dioxin-linked COFs show isostructural tbo topology made up of three kinds of polyhedron subunits,exhibiting high Brunauer-Emmett-Teller surface areas of≤1477 *** particular,the multiple polyhedron subunits in USTB-28-M could trap N-hydroxyphthalimide at their corners for easily forming stable phthalimide-N-oxyl radicals under visible-light *** generated radicals efficiently promote the aerobic oxidation of alkyl benzenes with an inert C（sp3）-H bond into various *** the three investigated COFs,the USTB-28-Co radical initiator exhibits the best photocatalytic oxidation activity,converting ethylbenzene into acetophenone with a turnover frequency of 63 h-1,which is much higher than those of the monomer CoPcF16(8 h-1) and 2D dioxin-linked counterparts(13 h-1).This is due to the much prolonged lifetime of the excited state for USTB-28-Co based on the femtosecond transient absorption *** present work not only presents 3D functional COFs with robust connection and permanent porosity,but also illustrates the uniqueness of porous structures of 3D COFs for high-performance photocatalysis.

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Unveiling interatomic distances influencing the reaction coordinates in alanine dipeptide isomerization: An explainable deep learning approach

arXiv

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arXiv 2024年

作者： Okada, Kazushi Kikutsuji, Takuma Okazaki, Kei-Ichi Mori, Toshifumi Kim, Kang Matubayasi, Nobuyuki Division of Chemical Engineering Department of Materials Engineering Science Graduate School of Engineering Science Osaka University Osaka Toyonaka560-8531 Japan Research Center for Computational Science Institute for Molecular Science Aichi Okazaki444-8585 Japan Graduate Institute for Advanced Studies SOKENDAI Aichi Okazaki444-8585 Japan Institute for Materials Chemistry and Engineering Kyushu University Fukuoka Kasuga816-8580 Japan Interdisciplinary Graduate School of Engineering Sciences Kyushu University Fukuoka Kasuga816-8580 Japan

The present work shows that the free energy landscape associated with alanine dipeptide isomerization can be effectively represented by specific interatomic distances without explicit reference to dihedral angles. Conventionally, two stable states of alanine dipeptide in vacuum, i.e., C7eq (β-sheet structure) and C7ax (left handed α-helix structure), have been primarily characterized using the main chain dihedral angles, φ (C-N-Cα-C) and ψ (N-Cα-C-N). However, our recent deep learning combined with "Explainable AI" (XAI) framework has shown that the transition state can be adequately captured by a free energy landscape using φ and θ (O-C-N-Cα) [T. Kikutsuji, et al. J. Chem. Phys. 156, 154108 (2022)]. In perspective of extending these insights to other collective variables, a more detailed characterization of transition state is required. In this work, we employ the interatomic distances and bond angles as input variables for deep learning, rather than the conventional and more elaborate dihedral angles. Our approach utilizes deep learning to investigate whether changes in the main chain dihedral angle can be expressed in terms of interatomic distances and bond angles. Furthermore, by incorporating XAI into our predictive analysis, we quantified the importance of each input variable and succeeded in clarifying the specific interatomic distance that affects the transition state. The results indicate that constructing a free energy landscape based on using the identified interatomic distance can clearly distinguish between the two stable states and provide a comprehensive explanation for the energy barrier crossing. Copyright © 2024, The Authors. All rights reserved.

关键词： Isomerization

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Red/NIR emission carbonized polymer dots based on citric acid-benzoylurea and their application in lymph nodes imaging

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Chinese chemical Letters 2023年第11期34卷 225-230页

作者： Feishi Shan Tingrui Zhang Chengshuang Liao Xue Yue Jing Zhang Li Yan Yanman Liu Zhixing Cao Min Wang Yahui Zhang Leyong Wang Zhouyu Wang Xiaoqi Yu Sichuan Engineering Research Center for Molecular Targeted Diagnostic&Therapeutic Drugs Asymmetric Synthesis and Chiral Technology Key Laboratory of Sichuan ProvinceResearch and Application of Small Organic Chiral Molecules Key Laboratory of Yibin CityDepartment of ChemistryXihua UniversityChengdu 610039China State Key Laboratory of Southwestern Chinese Medicine Resources Pharmacy SchoolChengdu University of Traditional Chinese MedicineChengdu 611137China State Key Laboratory of Analytical Chemistry for Life Science Key Laboratory of Mesoscopic Chemistry of MOEJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Identification of lymph nodes(LNs)is critical for studies of the structure,the role in disease development,and the efficacy of disease *** polymer dots(CPDs)are expected to be potential LNs-targeted imaging agents due to their excellent properties with special structure,better photoluminescence(PL)and great ***,a red/near infrared(NIR)emission CPDs(RCPDs)with one and two-photon bioimaging based on citric acid(CA)and benzoylurea(BU)are ***,the RCPDs are capable of targeting LNs for *** homing has been demonstrated to be the cellular mechanism of RCPDs target LNs *** work has developed a new nanomaterial for targeted imaging of LNs,while the biological applications of CPDs have been expanded and deepened.

关键词： Carbonized polymer dots Red/NIR emission LNs-targeting Lymphocyte homing

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Phase equilibria and thermodynamics assessment of the Co–Fe–Nb ternary system

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Intermetallics 2024年 168卷

作者： Hutabalian, Yohanes Hermana, Gita Novian Laksono, Andromeda Dwi Chen, Sinn-wen Department of Chemical Engineering National Tsing Hua University Taiwan Hsinchu30013 Taiwan Research and Development Center PT. Gotion Indonesia Materials Jakarta12950 Indonesia Department of Advanced Materials Engineering Bandung Polytechnic for Manufacturing West Java Bandung40135 Indonesia Department of Materials Science and Engineering National Taiwan University of Science and Technology Taiwan Taipei10672 Taiwan Study Program of Materials and Metallurgical Engineering Institut Teknologi Kalimantan Soekarno-Hatta Street Km. 15 Karang Joang East Kalimantan Balikpapan76127 Indonesia High Entropy Materials Center National Tsing Hua University Taiwan Hsinchu30013 Taiwan

The Co–Fe–Nb materials system is a crucial material for magnetic applications. Despite its importance, the phase equilibria and thermodynamic characteristics of this ternary system have not been explored in detail. This study employs the Calphad method to model the phase equilibria of the Co–Fe–Nb ternary system. To obtain the ternary interaction parameters, the experimental data on the isothermal sections at temperatures ranging from 700 °C to 1300 °C was evaluated. These findings indicate that the Co–Fe–Nb system contains no ternary compound, and the (Co,Fe)7Nb6 phase exists as a single solid solution. Significant solubility of the third element in the binary compounds of Co2Nb (Laves C14) and Fe2Nb (Laves C15) is also observed. The results are in good agreement with the experimental data. Furthermore, a liquidus projection of the system is presented, for the first time, revealing eight primary solidification phases in the Co–Fe–Nb ternary system. © 2024

关键词： Phase equilibria

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