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Aggregate 2024年第6期5卷 392-399页

作者： Junru Chen Xianhe Zhang Zongliang Xie Bin Liu Department of Chemical and Biomolecular Engineering National University of SingaporeSingaporeSingapore Integrative Sciences and Engineering Program NUS Graduate SchoolNational University of SingaporeSingaporeSingapore Institute for Functional Intelligent Materials National University of SingaporeSingaporeSingapore

Ultralong thermally activated delayed fluorescence(UTADF)materials play an important role in realizing time-dependent color-tunable *** typical carbazole(Cz)derivatives have been reported to exhibit UTADF ***,a 10-fold difference in TADF lifetime was found between commercial Cz derivatives and the corresponding lab-synthesized ones,which indicated that UTADF may not be derived from the single Cz derivatives as *** reveal the real mechanism,we synthesized three Cz derivatives and one isomer to form three host-guest pairs for optical *** photophysical properties revealed that UTADF originated from the intermolecular charge transfer between host and guest,while the ultralong organic phosphorescence was from the *** to the rich color variations in luminescence displayed by 4-(1H-benzo[f]indol-1-yl)−4′-(9H-carbazol-9-yl)-[1,1′-biphenyl]−3,3′-dicarbonitrile/4,4′-di(9H-carbazol-9-yl)-[1,1′-biphenyl]−3,3′-dicarbonitrile(CBP-2CN)at different delay times,it can be applied to realize multi-dimensional encryption in both delay time and luminescent color.

关键词： energy transfer intermolecular charge transfer ultralong organic phosphorescence ultralong thermally activated delayed fluorescence

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Composition-dependent catalytic performance of Au_(x)Ag_(25-x) alloy nanoclusters for oxygen reduction reaction

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Nano Research 2024年第11期17卷 9490-9497页

作者： Chuan Mu Biao Wang Qiaofeng Yao Qian He Jianping Xie Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Fuzhou 350207 China Department of Chemical and Biomolecular Engineering National University of Singapore 4 Engineering Drive 4 Singapore 117585 Singapore School of Physical Science and Technology Southwest University Chongqing 400715 China Key Laboratory of Organic Integrated Circuits Ministry of Education and Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of Chemistry School of Science Tianjin University Tianjin 3700072 China Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin 300072 China Department of Materials Science and Engineering National University of Singapore 9 Engineering Drive 1 Singapore 117575 Singapore

Oxygen reduction reaction(ORR)occurs at the cathode of electrochemical devices like fuel cells and in the Huron-Dow process,reducing oxygen to water or hydrogen *** the past years,various electrocatalysts with enhanced activity,selectivity,and durability have been developed for ***,an atomic-level understanding of how materials composition affects electrocatalytic performance has not yet been achieved,which prevents us from designing efficient catalysts based on the requirements of practical *** is partially because of the polydispersity of traditional catalysts and their unknown structure dynamics in the electrocatalytic *** we establish a full-spectrum of atomically precise and robust Au_(x)Ag_(25-x)(MHA)18(x=0–25,and MHA=6-mercaptohexanoic acid)nanoclusters(NCs)and systematically investigate their composition-dependent catalytic performance for ORR at the atomic *** results show that,with the increasing number of Au atoms in Au_(x)Ag_(25-x)(MHA)18 NCs,the electron transfer number gradually decreases from 3.9 for Ag25(MHA)18 to 2.1 for Au25(MHA)18,indicating that the dominant oxygen reduction product alters from water to hydrogen *** functional theory simulations reveal that the Gibbs free energy of OOH adsorption(ΔGOOH*)on Au25 is closest to the idealΔGOOH*of 4.22 eV to produce H_(2)O_(2),while Ag alloying makes theΔGOOH*deviate from the optimal value and leads to the production of *** study suggests that alloy NCs are promising paradigms for unveiling composition-dependent electrocatalytic performance of metal nanoparticles at the atomic level.

关键词： metal nanoclusters synthesis electrocatalysis structure-property relationship

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Towards atom-level understanding of metal oxide catalysts for the oxygen evolution reaction with machine learning

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npj Computational Materials 2024年第1期10卷 2430-2440页

作者： Jaclyn R.Lunger Jessica Karaguesian Hoje Chun Jiayu Peng Yitong Tseo Chung Hsuan Shan Byungchan Han Yang Shao-Horn Rafael Gómez-Bombarelli Department of Materials Science and Engineering Massachusetts Institute of TechnologyCambridgeMA 02139USA Center for Computational Science and Engineering Massachusetts Institute of TechnologyCambridgeMA 02139USA Department of Chemical and Biomolecular Engineering Yonsei UniversitySeoul 03722Republic of Korea Department of Computational and Systems Biology Massachusetts Institute of TechnologyCambridgeMA 02139USA Department of Materials Science and Engineering University of TorontoTorontoON M5SCanada Department of Mechanical Engineering Massachusetts Institute of TechnologyCambridgeMA 02139USA Research Laboratory of Electronics Massachusetts Institute of TechnologyCambridgeMA 02139USA

Green hydrogen production is crucial for a sustainable future,but current catalysts for the oxygen evolution reaction(OER)suffer from slow kinetics,despite many efforts to produce optimal designs,particularly through the calculation of descriptors for *** this study,we develop a dataset of density functional theory calculations of bulk and surface perovskite oxides,and adsorption energies of OER intermediates,which includes compositions up to quaternary and facets up to(555).We demonstrate that per-site properties of perovskite oxides such as Bader charge or band center can be tuned through element substitution and faceting,and develop a machine learning model that accurately predicts these properties directly from the local chemical *** leverage these per-site properties to identify promising perovskites with high theoretical OER *** identified design principles and promising materials provide a roadmap for closing the gap between current artificial catalysts and biological enzymes such as photosystem II.

关键词： perovskite oxides kinetics

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Surface reconstruction,modification and functionalization of natural diatomites for miniaturization of shaped heterogeneous catalysts

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Nano Materials science 2023年第3期5卷 293-311页

作者： Bowen Li Tian Wang Qiujian Le Runze Qin Yuxin Zhang Hua Chun Zeng Department of Chemical and Biomolecular Engineering Faculty of EngineeringNational University of Singapore10 Kent Ridge Crescent119260Singapore State Key Laboratory of Mechanical Transmissions College of Materials Science and EngineeringChongqing UniversityChongqing400044PR China

Since the discovery of mesoporous silica in 1990s,there have been numerous mesoporous silica-based nanomaterials developed for catalytic applications,aiming at enhanced catalytic activity and ***,there have also been considerable interests in endowing them with hierarchical porosities to overcome the diffusional limitation for those with long unimodal *** processes of making mesoporous silica largely rely on chemical sources which are relatively expensive and impose environmental concerns on their *** this regard,it is desirable to develop hierarchical silica supports from natural ***,we present a series of work on surface reconstruction,modification,and functionalization to produce diatomite-based catalysts with original morphology and macro-meso-micro porosities and to test their suitability as catalyst supports for both liquid-and gas-phase *** wet-chemical routes were developed to introduce mesoporosity to both amorphous and crystalline ***,we have used computational modeling to affirm that the diatomite morphology can improve catalytic performance based on fluid dynamics ***,one could obtain this type of catalysts from numerous natural diatoms that have inherently intricate morphologies and shapes in micrometer *** principle,such catalytic nanocomposites acting as miniaturized industrial catalysts could be employed in microfluidic reactors for process intensification.

关键词： Heterogeneous catalysis Diatomites Silica Catalytic materials Miniaturization Sustainable chemistry

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Organic Radical-Boosted Ionic Conductivity in Redox Polymer Electrolyte for Advanced Fiber-Shaped Energy Storage Devices

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Nano-Micro Letters 2025年第8期17卷 202-218页

作者： Jeong-Gil Kim Jaehyoung Ko Hyung-Kyu Lim Yerin Jo Hayoung Yu Min Woo Kim Min Ji Kim Hyeon Su Jeong Jinwoo Lee Yongho Joo Nam Dong Kim Institute of Advanced Composite Materials Korea Institute of Science and Technology92 Chudong-roBongdong-eupWanju-gunJeollabuk-do 55324Republic of Korea Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology291 Daehak-roYuseong-guDaejeon 34141Republic of Korea Division of Chemical and Bioengineering Kangwon National UniversityChuncheon 24341Republic of Korea Department of Materials Science and Engineering Gwangju Institute of Science and TechnologyGwangju 61005Republic of Korea

Fiber-shaped energy storage devices(FSESDs)with exceptional flexibility for wearable power sources should be applied with solid electrolytes over liquid electrolytes due to short circuits and leakage issue during *** the solid options,polymer electrolytes are particularly preferred due to their robustness and flexibility,although their low ionic conductivity remains a significant ***,we present a redox polymer electrolyte(HT_RPE)with 4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl(HT)as a multi-functional *** acts as a plasticizer that transforms the glassy state into the rubbery state for improved chain mobility and provides distinctive ion conduction pathway by the self-exchange reaction between radical and oxidized *** synergetic effects lead to high ionic conductivity(73.5 mS cm−1)based on a lower activation energy of 0.13 eV than other redox ***,HT_RPE with a pseudocapacitive characteristic by HT enables an outstanding electrochemical performance of the symmetric FSESDs using carbon-based fiber electrodes(energy density of 25.4 W h kg^(−1) at a power density of 25,000 W kg^(−1))without typical active materials,along with excellent stability(capacitance retention of 91.2%after 8,000 bending cycles).This work highlights a versatile HT_RPE that utilizes the unique functionality of HT for both the high ionic conductivity and improved energy storage capability,providing a promising pathway for next-generation flexible energy storage devices.

关键词： Redox polymer electrolyte Hydroxy-TEMPO Ionic conductivity Self-exchange reaction Fiber-shaped energy storage devices

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Enhancing waste sorting and recycling efficiency: robust deep learning-based approach for classification and detection

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Neural Computing and Applications 2025年第6期37卷 4567-4583页

作者： Sayem, Faizul Rakib Islam, Md. Sakib Bin Naznine, Mansura Nashbat, Mohammad Hasan-Zia, Mazhar Kunju, Ali K Ansaruddin Khandakar, Amith Ashraf, Azad Majid, Molla Ehsanul Kashem, Saad Bin Abul Chowdhury, Muhammad E. H. Department of Electrical and Electronic Engineering University of Dhaka Dhaka Bangladesh Department of Biomedical Engineering Military Institute of Science and Technology Dhaka Bangladesh Department of Computer Science & Engineering Rajshahi University of Engineering & Technology Rajshahi6204 Bangladesh Chemical Engineering Department University of Doha for Science and Technology Doha Qatar Department of Electrical Engineering Qatar University Doha2713 Qatar Computer Applications Department Academic Bridge Program Qatar Foundation Doha Qatar Department of Computing Science AFG College With the University of Aberdeen Doha Qatar

Given the severity of waste pollution as a major environmental concern, intelligent and sustainable waste management is becoming increasingly crucial in both developed and developing countries. The material composition and volume of urban solid waste are key considerations in processing, managing, and utilizing city waste. Deep learning technologies have emerged as viable solutions to address waste management issues by reducing labor costs and automating complex tasks. However, the limited number of trash image categories and the inadequacy of existing datasets have constrained the proper evaluation of machine learning model performance across a large number of waste classes. In this paper, we present robust waste image classification and object detection studies using deep learning models, utilizing 28 distinct recyclable categories of waste images comprising a total of 10,406 images. For the waste classification task, we proposed a novel dual-stream network that outperformed several state-of-the-art models, achieving an overall classification accuracy of 83.11%. Additionally, we introduced the GELAN-E (generalized efficient layer aggregation network) model for waste object detection tasks, obtaining a mean average precision (mAP50) of 63%, surpassing other state-of-the-art detection models. These advancements demonstrate significant progress in the field of intelligent waste management, paving the way for more efficient and effective solutions. © The Author(s) 2024.

关键词： Deep learning for waste management Intelligent waste management Object detection in waste management Sustainable waste processing Urban solid waste Waste image classification

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Highly efficient vanadium redox flow batteries enabled by a trilayer polybenzimidazole membrane assembly

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Carbon Energy 2024年第7期6卷 191-204页

作者： Trung Tuyen Bui Mingyu Shin Mohammad Rahimi Anders Bentien Yongchai Kwon Dirk Henkensmeier Hydrogen·Fuel Cell Research Center Korea Institute of Science and Technology(KIST)SeoulRepublic of Korea Department of Chemical and Biomolecular Engineering Seoul National University of Science and TechnologySeoulRepublic of Korea Department of Biological and Chemical Engineering Aarhus UniversityAarhusDenmark KIST School Division of Energy and Environment TechnologyUniversity of Science and TechnologySeoulRepublic of Korea Graduate School of Energy and Environment Korea UniversitySeoulRepublic of Korea

A novel polybenzimidazole(PBI)-based trilayer membrane assembly is developed for application in vanadium redox flow battery(VRFB).The membrane comprises a 1μm thin cross-linked poly[2,2′-(p-oxydiphenylene)−5,5′-bibenzimidazole](OPBI)sandwiched between two 20μm thick porous OPBI membranes(p-OPBI)without further lamination *** trilayer membrane demonstrates exceptional properties,such as high conductivity and low area-specific resistance(ASR)of 51 mS cm^(−1) and 81mΩ cm^(2),*** with vanadium electrolyte increases the ASR of trilayer membrane only to 158mΩ cm^(2),while that of Nafion is 193mΩ cm^(2).VO^(2+) permeability is 2.73×10^(-9) cm^(2) min^(−1),about 150 times lower than that of Nafion *** addition,the membrane has high mechanical strength and high chemical stability against VO^(2+).In VRFB,the combination of low resistance and low vanadium permeability results in excellent performance,revealing high Coulombic efficiency(>99%),high energy efficiency(EE;90.8% at current density of 80mA cm^(−2)),and long-term *** EE is one of the best reported to date.

关键词： polybenzimidazole porous membrane proton conductivity trilayer VRFBs

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Organic Radical-Boosted Ionic Conductivity in Redox Polymer Electrolyte for Advanced Fiber-Shaped Energy Storage Devices

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Nano-Micro Letters 2025年第8期 210-226页

作者： Jeong-Gil Kim Jaehyoung Ko Hyung-Kyu Lim Yerin Jo Hayoung Yu Min Woo Kim Min Ji Kim Hyeon Su Jeong Jinwoo Lee Yongho Joo Nam Dong Kim Institute of Advanced Composite Materials Korea Institute of Science and Technology Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology Division of Chemical and Bioengineering Kangwon National University Department of Materials Science and Engineering Gwangju Institute of Science and Technology

Fiber-shaped energy storage devices（FSESDs） with exceptional flexibility for wearable power sources should be applied with solid electrolytes over liquid electrolytes due to short circuits and leakage issue during deformation. Among the solid options, polymer electrolytes are particularly preferred due to their robustness and flexibility, although their low ionic conductivity remains a significant challenge. Here, we present a redox polymer electrolyte（HT＿RPE） with 4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl（HT） as a multi-functional additive. HT acts as a plasticizer that transforms the glassy state into the rubbery state for improved chain mobility and provides distinctive ion conduction pathway by the self-exchange reaction between radical and oxidized species. These synergetic effects lead to high ionic conductivity(73.5 mScm-1)based on a lower activation energy of 0.13 eV than other redox additives. Moreover, HT＿RPE with a pseudocapacitive characteristic by HT enables an outstanding electrochemical performance of the symmetric FSESDs using carbon-based fiber electrodes(energy density of 25.4 Whkg-1at a power density of 25,000 W kg-1) without typical active materials, along with excellent stability（capacitance retention of 91.2% after 8,000 bending cycles）. This work highlights a versatile HT＿RPE that utilizes the unique functionality of HT for both the high ionic conductivity and improved energy storage capability, providing a promising pathway for next-generation flexible energy storage devices.

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Porphyrin-Grafted Poly(ethylene terephthalate) as a Reusable and Highly Selective Colorimetric Probe for Mercuric Ion Contaminants in Aqueous Samples

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ACS Applied Materials and Interfaces 2024年第30期16卷 39195-39205页

作者： Atayde, Eduardo C. Takenaka, Yasumasa Abe, Hideki Wu, Ming-Rou Wu, Kevin C.-W. Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Department of Chemistry National Tsing Hua University Department of Chemical Engineering National Taiwan University Bioplastic Research Team RIKEN Center for Sustainable Resource Science Department of Chemical Engineering and Materials Science Yuan Ze University Department of Chemical Engineering Chung Yuan Christian University

Heavy metals are the most hazardous water pollutants, with severe health and environmental consequences. Among these, mercuric (Hg2+) ions are known to cause detrimental health issues in both humans and aquatic life. ... 详细信息

Heavy metals are the most hazardous water pollutants, with severe health and environmental consequences. Among these, mercuric (Hg²⁺) ions are known to cause detrimental health issues in both humans and aquatic life. Due to this, several analytical techniques have been devised to detect and quantify the amount of this ion. However, most of these require advanced instrumentation, prolonged analysis time, and sample preparation. In this study, a low-cost and highly reusable colorimetric probe was developed by grafting porphyrin to poly(ethylene terephthalate) sheets using an oxazoline polymer as covalent adhesive. Upon exposure to trace amounts of Hg²⁺ in solution, the fabricated material visually transitioned from faint brownish pink to green by the complexation mechanism. Additionally, the transparency of this probe allowed the quantitative spectrophotometric determination of the Hg²⁺ concentration in aqueous samples. It was also shown that the material is highly stable, which can be reused for more than 50 times without significant decline in its performance, hence, making it suitable for the onsite monitoring of mercuric ion contamination in different bodies of water. © 2024 The Authors. Published by American chemical Society.

关键词： colorimetric probe mercuric ion oxazoline PET porphyrin

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Efficient predictions of formation energies and convex hulls from density functional tight binding calculations

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Journal of Materials science & Technology 2023年第10期141卷 236-244页

作者： Anshuman Kumar Zulfikhar A.Ali Bryan M.Wong Materials Science&Engineering Program University of California-RiversideRiverside92521CAUSA Department of Physics&Astronomy University of California-RiversideRiverside92521CAUSA Materials Science&Engineering Program Department of Chemical&Environmental EngineeringDepartment of Physics&Astronomyand Department of ChemistryUniversity of California-RiversideRiverside92521CAUSA

Defects in materials significantly alter their electronic and structural properties,which affect the per-formance of electronic devices,structural alloys,and functional ***,calculating all the possible defects in complex materials with conventional Density Functional Theory(DFT)can be compu-tationally *** enhance the efficiency of these calculations,we interfaced Density Functional Tight Binding(DFTB)with the Clusters Approach to Statistical Mechanics(CASM)software package for the first *** SiC and ZnO as representative examples,we show that DFTB gives accurate results and can be used as an efficient computational approach for calculating and pre-screening formation ener-gies/convex *** DFTB+CASM implementation allows for an efficient exploration(up to an order of magnitude faster than DFT)of formation energies and convex hulls,which researchers can use to probe other complex systems.

关键词： CASM DFTB DFT Formation energy Convex hull

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