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Molecular surface functionalization of In_(2)O_(3) to tune interfacial microenvironment for enhanced catalytic performance of CO_(2) electroreduction

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Nano Research 2024年第3期17卷 1242-1250页

作者： Suwen WangQiang GaoCui Xu Shuai Jiang Mengyang Zhang Xianjun Yin Hui-Qing Peng Bin Liu Yu-Fei Song State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

Indium-based materials(e.g.,In_(2)O_(3))are a class of promising non-noble metal-based catalysts for electroreduction of carbon dioxide(CO_(2)).However,competitive hydrogen reduction reaction(HER)on indium-based catalysts hampers CO_(2) reduction reaction(CO_(2)RR)*** herein tune the interfacial microenvironment of In_(2)O_(3) through chemical graft of alkyl phosphoric acid molecules using a facile solution-processed strategy for the first time,which is distinguished from other researches that tailor intrinsic activity of In_(2)O_(3) *** surface functionalization of alkyl phosphoric acids over In_(2)O_(3) is demonstrated to remarkably boost CO_(2) *** example,octadecylphosphonic acid modified In_(2)O_(3) exhibits Faraday efficiency for H_(2) H_(2) H_(2)(FE)of as low as 6.6%and FEHCOOH of 86.5%at-0.67 V ***,which are far superior to parent In_(2)O_(3) counterparts(FE of 24.0%and FEHCOOH of 63.1%).Moreover,the enhancing effect of alkyl phosphoric acid functionalization is found to be closely related to the length of alkyl *** virtue of comprehensive experimental characterizations and molecular dynamics simulations,it is revealed that the modification of alkyl phosphoric acids significantly alters the interface microenvironment of the electrocatalyst,which changes the electrocatalyst surface from hydrophilic and aerophobic to hydrophobic and *** this case,the water molecules are pushed away and more CO_(2) molecules are trapped,increasing local CO_(2) concentration at In_(2)O_(3) active sites,thus leading to the significantly enhanced CO_(2)RR and suppressed *** work highlights the importance of regulating the interfacial microenvironment of inorganic catalysts by molecular surface functionalization as a means for promoting the electrochemical performance in electrosynthesis and beyond.

关键词： carbon dioxide(CO_(2))electroreduction interfacial microenvironment molecular surface functionalization In_(2)O_(3)catalyst water and CO_(2)diffusion

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Efficient and Stable Photoassisted Lithium‑Ion Battery Enabled by Photocathode with Synergistically Boosted Carriers Dynamics

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Nano-Micro Letters 2025年第3期17卷 440-454页

作者： Zelin Ma Shiyao Wang Zhuangzhuang Ma Juan Li Luomeng Zhao Zhihuan Li Shiyuan Wang Yazhou Shuang Jiulong Wang Fang Wang Weiwei Xia Jie Jian Yibo He Junjie Wang Pengfei Guo Hongqiang Wang State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi’an 710072People’s Republic of China State Key Laboratory of Solidification Processing School of Materials Science and Engineering DepartmentNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China Research and Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518063People’s Republic of China Key Laboratory of Applied Surface and Colloid Chemistry Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringNational Ministry of EducationShaanxi Normal UniversityXi’an 710119People’s Republic of China

Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active *** work proposes a general approach of creating bulk heterojunction to boost the carrier mobility of photocathodes by simply laser assisted embedding of plasmonic *** employed in PLIBs,it was found effective for synchronously enhanced photocharge separation and transport in light charging ***,experimental photon spectroscopy,finite difference time domain method simulation and theoretical analyses demonstrate that the improved carrier dynamics are driven by the plasmonic-induced hot electron injection from metal to TiO_(2),as well as the enhanced conductivity in TiO2 matrix due to the formation of oxygen vacancies after Schottky *** from these merits,several benchmark values in performance of TiO2-based photocathode applied in PLIBs are set,including the capacity of 276 mAh g^(−1) at 0.2 A g^(−1) under illumination,photoconversion efficiency of 1.276%at 3 A g^(−1),less capacity and Columbic efficiency loss even through 200 *** results exemplify the potential of the bulk heterojunction strategy in developing highly efficient and stable photoassisted energy storage systems.

关键词： Photoassisted lithium-ion batteries Bulk heterojunction Carrier dynamics TiO2 nanofiber Plasmonic metal nanocrystals

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Ten-Minute Synthesis of a New Redox-Active Aqueous Binder for Flame-Retardant Li-S Batteries

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Energy & Environmental Materials 2024年第2期7卷 48-57页

作者： Tianpeng Zhang Borui Li Zihui Song Wanyuan Jiang Siyang Liu Runyue Mao Xigao Jian Fangyuan Hu School of Materials Science and Engineering State Key Laboratory of Fine ChemicalsFrontiers Science Center for Smart Materials Oriented Chemical Engineering Technology Innovation Center of High Performance Resin Materials(Liaoning Province)Key Laboratory of Energy Materials and Devices(Liaoning Province)Dalian University of TechnologyDalian 116024China State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart Materials Oriented Chemical EngineeringSchool of Chemical Engineering Technology Innovation Center of High Performance Resin Materials(Liaoning Province)Key Laboratory of Energy Materials and Devices(Liaoning Province)Dalian University of TechnologyDalian 116024China

As a critical role in battery systems,polymer binders have been shown to efficiently suppress the lithium polysulfide shuttling and accommodate volume changes in recent ***,preparation processes and safety,as the key criterions for Li-S batteries'practical applications,still attract less ***,an aqueous multifunction binder(named PEI-TIC)is prepared via an easy and fast epoxy-amine ring-opening reaction(10 min),which can not only give the sulfur cathode a stable mechanical property,a strong chemical adsorption and catalytic conversion ability,but also a fire safety *** Li-S batteries based on the PEI-TIC binder display a high discharge capacity(1297.8 mAh g^(-1)),superior rate performance(823.0 mAh g^(-1)at 2 C),and an ultralow capacity decay rate of 0.035%over more than 800 *** under 7.1 mg cm^(-2)S-loaded,the PEI-TIC electrode can also achieve a high areal capacity of 7.2 mA h g^(-1)and excellent cycling stability,confirming its application ***,it is also noted that TG-FTIR test is performed for the first time to explore the flame-retardant mechanism of polymer *** work provides an economically and environmentally friendly binder for the practical application and inspires the exploration of the flame-retardant mechanism of all electrode components.

关键词： 3D cross-linked network environmentally friendly flame retardant Li-S batteries multifunction binder

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Oxygen vacancy-rich CoMoO4/Carbon nitride S-scheme heterojunction for boosted photocatalytic H_(2)production:Microstructure regulation and charge transfer mechanism

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Journal of Materials science & Technology 2024年第31期198卷 176-185页

作者： Jiani Qin Yanli Dong Xiaojuan Lai Bo Su Bao Pan Chuanyi Wang Sibo Wang School of Environmental Science and Engineering Shaanxi University of Science and TechnologyXi'an 710021China Key Laboratory of Chemical Additives for China National Light Industry School of Chemistry and Chemical EngineeringShaanxi University of Science and TechnologyXi'an 710021China State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350116China

Developing highly efficient S-scheme photocatalysts is a subject of immense interest for harnessing solar energy towards sustainable hydrogen ***,a novel S-scheme heterojunction of oxygen vacancy-rich CoMoO_(4)/CN(CMO/CN)photocatalyst was rationally constructed through loading CoMoO_(4)nanorods on carbon nitride(CN)nanosheets via a direct one-pot calcination *** CMO/CN S-scheme heterojunction exhibited enhanced surface area,fine CN dispersion,rich oxygen vacancies,and accelerated charge separation/transfer efficiency,which were conducive to improving photocatalytic H_(2)evolution *** note,the optimal 3%CMO/CN sample displayed the highest H_(2)production rate of 8.35 mmol g^(-1)h^(-1),which is 4.6 folds that of pristine *** situ irradiated X-ray photoelectron spectroscopy(XPS)and electron paramagnetic resonance(EPR)characterizations confirmed the S-scheme charge transfer path between CN and CMO,which greatly promoted spatial charge *** functional theory(DFT)calculations together with contact angle tests revealed the reduced activation energies for H_(2)O dissociation and enhanced hydrophilicity of the CMO/*** CMO/CN photocatalysts also presented high stability and fine *** work may provide insights into the combination of defect engineering and heterojunction designing for high-efficiency solar-to-chemical energy conversion.

关键词： S-scheme CoMoO_(4) Carbon nitride Oxygen vacancy Photocatalysis

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Synthesis of poly(thiourethane-alt-thioester)by alternating ring-opening copolymerization of N-thiocarboxyanhydrides and episulfides

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science China Chemistry 2024年第9期67卷 3091-3097页

作者： Wei Xiong Tianjun Yue Haiwang Lai Chunyan Lyu Weimin Ren Hua Lu Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalian 116081China

Polythiourethanes(PTU)and polythioesters(PTE)derived from renewable sources are emerging sustainable polymers for their excellent degradability and ***,P(TU-alt-TE)copolymers have been rare and challenging to ***,we report the efficient synthesis of novel P(TU-alt-TE)copolymers via the alternating copolymerization of N-thiocarboxyanhydrides(NTA)/episufides(ES)and provide mechanistic insight into the alternating chain propagation process via density functional theory(DFT)*** incorporation of ESs into traditional peptide backbone is capable of adjusting the glass transition temperature below thermal decomposition temperature,which confers better thermal processability by regulating the rigidity of the backbone and the hydrogen bond interaction among the polymer *** PTUs with tailored properties are accessible by altering the feeding ratio of NTAs and(bifunctional)***,the thiourethane in the backbone can endow interesting underwater adhesion properties to the *** the broad scope of NTA and ES monomers,this method is expected to provide a promising and general route to a wide range of P(TU-alt-TE)copolymers with diverse properties.

关键词： poly(thiourethane-alt-thioester) alternating ring-opening copolymerization N-thiocarboxyanhydrides episulfides

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Hierarchical metal-peptide assemblies with chirality-encoded spiral architecture and catalytic activity

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science China Chemistry 2023年第1期66卷 228-241页

作者： Jiayu Liu Jiaxing Zhang Liwei Zhang Yuefei Wang Hao Wei Yuhe Shen Jiwei Min Xi Rong Wei Qi Rongxin Su Zhimin He School of Chemical Engineering and Technology State Key Laboratory of Chemical EngineeringTianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Tianjin Key Laboratory of Membrane Science and Desalination Technology Tianjin 300072China

We report the coordination assembly of the ferrocene-diphenylalanine(Fc-FF)with divalent copper ions(Cu^(2+))into metalpeptide assemblies(MPAs)with hierarchical spiral *** MPA particles are composed of helically organized nanofibers which can be correlated to the logarithmic *** MPAs are hierarchically porous with abundant Fc and Cu2+active sites and show much higher catalytic activity than natural laccase toward the decolorization ***,a series of hierarchical structures of the MPAs can be synthesized by controlling the temperature and enantiomeric excess(ee).The peptide enantiomers with higher ee values will self-assemble into highly complex and ordered structures,which show higher surface area and porosity and thus enhanced catalytic activity compared with those assembled by peptides with lower ee *** results provide new insights into the vital role of chirality in directing the self-assembly of biomolecules into highly ordered complex functional structures.

关键词： peptide metal coordination spiral particles chirality catalysis

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Targeted regeneration and upcycling of spent graphite by defect‐driven tin nucleation

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Carbon Energy 2024年第4期6卷 91-103页

作者： Zhiheng Cheng Zhiling Luo Hao Zhang Wuxing Zhang Wang Gao Yang Zhang Long Qie Yonggang Yao Yunhui Huang Kun Kelvin Fu State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanChina Key Laboratory of Automobile Materials(Jilin University) Ministry of EducationDepartment of Materials Science and EngineeringJilin UniversityChangchunChina Electronic Materials Research Laboratory(Key Lab of Education Ministry) School of Electronic and Information Engineeringand Instrumental Analysis CenterXi'an Jiaotong UniversityXi'anChina Department of Mechanical Engineering University of DelawareNewarkUSA

The recycling of spent batteries has become increasingly important owing to their wide applications,abundant raw material supply,and sustainable *** with the degraded cathode,spent anode graphite often has a relatively intact structure with few defects after long ***,most spent graphite is simply burned or discarded due to its limited value and inferior performance on using conventional recycling methods that are complex,have low efficiency,and fail in performance ***,we propose a fast,efficient,and“intelligent”strategy to regenerate and upcycle spent graphite based on defect‐driven targeted *** Sn as a nanoscale healant,we used rapid heating(~50 ms)to enable dynamic Sn droplets to automatically nucleate around the surface defects on the graphite upon cooling owing to strong binding to the defects(~5.84 eV/atom),thus simultaneously achieving Sn dispersion and graphite *** a result,the regenerated graphite showed enhanced capacity and cycle stability(458.9 mAh g^(−1) at 0.2 A g^(−1) after 100 cycles),superior to those of commercial *** from the self‐adaption of Sn dispersion,spent graphite with different degrees of defects can be regenerated to similar structures and *** analysis indicates that targeted regeneration and upcycling have significantly lower energy consumption(~99%reduction)and near‐zero CO_(2) emission,and yield much higher profit than hydrometallurgy,which opens a new avenue for direct upcycling of spend graphite in an efficient,green,and profitable manner for sustainable battery manufacture.

关键词： battery recycling spent graphite targeted regeneration upcycling graphite

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Optimal weight support vector regression ensemble with cluster-based subsampling for electricity price forecasting

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Journal of Intelligent and Fuzzy Systems 2024年第1期1卷 1-16页

作者： Li, Yuerong Zhang, Yuhua Che, Jinxing School of Science Nanchang Institute of Technology Jiangxi Nanchang China Key Laboratory of Engineering Mathematics and Advanced Computing Nanchang Institute of Technology Jiangxi Nanchang China

Accurate prediction of short-term electricity price is the key to obtain economic benefit and also an important index of power system planning and management. Support vector regression (SVR) based ensemble works have gained remarkable achievements in terms of high accuracy and steady performance, but they are highly dependent on data representativeness and have a high computational complexity O (k ∗ N 3) of data samples and parameter selection. To further improve the data representativeness and reduce its computational complexity, this paper develops a new approach to forecast electricity price via optimal weighted ensemble. In the model, the cluster-based subsampling algorithm is proposed to categorize the inputs being seasonally decomposed into several groups, and representative data are drawn from each group in a certain proportion to ensure that each subset trained with SVR has the same representativeness and features. Moreover, the optimal weighted combination method is presented to assign weights to the sub-SVRs to obtain the optimal support vector regression ensemble model (OWSSVRE). The experimental results show that the improved support vector regression ensemble model with the same features and representativeness of the subset has better performance in electricity price forecasting. As a result, it is suitable to support decision making in the energy and other sectors. © 2024 - IOS Press. All rights reserved.

关键词： K-means clustering

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Massively parallel algorithms for fully dynamic all-pairs shortest paths

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Frontiers of Computer science 2024年第4期18卷 201-203页

作者： Chilei WANG Qiang-Sheng HUA Hai JIN Chaodong ZHENG National Engineering Research Center for Big Data Technology and System Services Computing Technology and System LabCluster and Grid Computing LabSchool of Computer Science and TechnologyHuazhong University of Science and TechnologyWuhan 430074China State Key Laboratory for Novel Software Technology Nanjing UniversityNanjing 210023China

1 Introduction In recent years,the Massively Parallel Computation(MPC)model has gained significant ***,most of distributed and parallel graph algorithms in the MPC model are designed for static graphs[1].In fact,the graphs in the real world are constantly *** size of the real-time changes in these graphs is smaller and more *** graph algorithms[2,3]can deal with graph changes more efficiently[4]than the corresponding static graph ***,most studies on dynamic graph algorithms are limited to the single machine ***,a few parallel dynamic graph algorithms(such as the graph connectivity)in the MPC model[5]have been proposed and shown superiority over their parallel static counterparts.

关键词： dynamic shortest gained

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STRAP binds to and promotes the repair of N1-methyldeoxyadenosine in DNA

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Chinese Chemical Letters 2024年第3期35卷 204-207页

作者： Meijuan Zhou Qian Liu Mengting Pan Ying Yang Xiaoxia Dai Changjun You State Key Laboratory of Chemo/Biosensing and Chemometrics Hunan Provincial Key Laboratory of Biomacromolecular Chemical BiologyMolecular Science and Biomedicine LaboratoryCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

N1-methyladenosine(m1A)is an important RNA modification that functions in various biological processes by interacting with cellular ***,the binding proteins of N1-methyldeoxyadenosine(1mdA)in DNA remain largely ***,we employed a quantitative proteomics strategy to identify the potential binding proteins of 1mdA in human *** results revealed that serine–threonine kinase receptor-associated protein(STRAP)can bind to 1mdA-carrying *** further demonstrated that STRAP participates in alkylating agent-induced DNA damage response and can promote the repair of 1mdA embedded in ***,we investigated the effects of STRAP on 1mdA-induced perturbation in transcription using a shuttle vector-and next-generation sequencing-based assay,and found that STRAP is involved in the transcriptional bypass of 1mdA in human ***,our study revealed STRAP as a novel 1mdA-binding protein in human cells and provided new insight into the biological implications of STRAP and 1mdA modification in human diseases.

关键词： N1-methyldeoxyadenosine 1mdA-binding protein STRAP DNA repair Transcription

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