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Building Li-S batteries with enhanced temperature adaptability via a redox-active COF-based barrier-trapping electrocatalyst

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Journal of Energy Chemistry 2025年第2期101卷 702-712页

作者： Jie Xu Acheng Zhu Zhangyu Zheng Yiming Qi Yuwen Cheng Yongjie Cao Bo Peng Lianbo Ma Yonggang Wang School of materials Science and Engineering Key Laboratory of Efficient Conversion and Solid-state Storage of Hydrogen & Electricity of Anhui Province Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials of Ministry of Education Anhui University of Technology Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and innovative materials Institute of New Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Fudan University

Covalent organic frameworks（COFs） are promising materials for mitigating polysulfide shuttling in lithium-sulfur（Li-S） batteries,but enhancing their ability to convert polysulfides across a wide temperature range remains a challenge,Herein,we introduce a redox-active COF（RaCOF） that functions as both a physical barrier and a kinetic enhancer to improve the temperature adaptability of Li-S batteries,The RaCOF constructed from redox-active anthraquinone units accelerates polysulfide conversion kinetics through reversible C=O/C-OLi transformations within a voltage range of 1,7 to 2.8 V（***+/Li）,optimizing sulfur redox reactions in ether-based *** conventional COFs,RaCOF provides bidentate trapping of polysulfides,increasing binding energy and facilitating more effective polysulfide ***-situ XRD and ToF-SIMS analyses confirm that RaCOF enhances polysulfide adsorption and promotes the transformation of lithium sulfide（Li2S）,leading to better sulfur cathode ***,RaCOF-modified Li-S batteries demonstrate low self-discharge（4.0% decay over a 7-day rest）,excellent wide-temperature performance（stable from-10 to+60℃）,and high-rate cycling stability（94% capacity retention over 500 cycles at 5.0 C）.This work offers valuable insights for designing COF structures aimed at achieving temperature-adaptive performance in rechargeable batteries.

关键词： Covalent organic framework Lithium-sulfur batteries Redox-active property Wide-temperature adaptability

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A low redox potential and long life organic anode material for sodium-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 557-564页

作者： Zhi Li Yang Wei Kang Zhou Xin Huang Xing Zhou Jie Xu Taoyi Kong Junwei Lucas Bao Xiaoli Dong Yonggang Wang Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and innovative materials Institute of New EnergyCollaborative Innovation Center of Chemistry for Energy Materials(iChEM)Fudan UniversityShanghai 200433China Department of Chemistry Boston CollegeChestnut HillMA 02467USA School of materials Science and Engineering Anhui University of TechnologyMa’anshan 243002AnhuiChina

Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ***,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials(>1 V).Organic electrodes with low redox potential that can be used as anode are ***,a novel organic anode material (tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na_(4)TDC) has been developed with low redox potential (<0.7 V) and excellent cyclic *** three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per ***,the Na_(4)TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg cm^(-2).By pairing with a thick Na_(3)V_(2)(PO_(4))_(3)cathode (20.6 mg cm^(-2)),the as-fabricated full cell exhibited high operating voltage (2.8 V),excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na_(4)TDC anode material for SIBs.

关键词： Organic anode material Low redox potential Composite anode Sodium-ion batteries

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Design of multifunctional interfaces on ceramic solid electrolytes for high-performance lithium-air batteries

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Green Energy & Environment 2025年第1期10卷 183-192页

作者： Yunxin Shi Ziyang Guo Changhong Wang Mingze Gao Xiaoting Lin Hui Duan Yonggang Wang Xueliang Sun College of Energy Material and Chemistry College of Chemistry and Chemical EngineeringInner Mongolia UniversityHohhot010021China Department of Mechanical and materials Engineering Western UniversityLondonONN6A 5B9Canada Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and innovative materials Institute of New EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Fudan UniversityShanghai200433China Eastern institute for Advanced Study Eastern Institute of TechnologyNingboZhejiang315100China

High-energy-density lithium(Li)–air cells have been considered a promising energy-storage system,but the liquid electrolyte-related safety and side-reaction problems seriously hinder their *** address these above issues,solid-state Li–air batteries have been widely ***,many commonly-used solid electrolytes generally face huge interface impedance inLi–air cells and also showpoor stability towards ambient air/Li ***,we fabricate a differentiating surface-regulated ceramic-based composite electrolyte(DSCCE)by constructing disparately LiI-containing polymethyl methacrylate(PMMA)coating and Poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)layer on both sides of Li_(1.5)Al_(0.5)Ge_(1.5)(PO_(4))_(3)(LAGP).The cathode-friendly LiI/PMMA layer displays excellent stability towards superoxide intermediates and also greatly reduces the decomposition voltage of discharge products in Li–air ***,the anode-friendly PVDF-HFP coating shows low-resistance properties towards ***,Li dendrite/passivation derived from liquid electrolyte-induced side reactions and air/I-attacking can be obviously suppressed by the uniformand compact composite *** a result,the DSCCE-based Li–air batteries possess high capacity/low voltage polarization(11,836mAh g^(-1)/1.45Vunder 500mAg^(-1)),good rate performance(capacity ratio under 1000mAg^(-1)/250mAg^(-1) is 68.2%)and longterm stable cell operation(~300 cycles at 750 mA g^(-1) with 750 mAh g^(-1))in ambient air.

关键词： Li-air batteries Li_(1.5)Al_(0.5)Ge_(1.5)(PO_(4))_(3) Polymers Composite electrolyte Ambient air

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Strength through unity: Alkaline phosphatase-responsive AIEgen nanoprobe for aggregation-enhanced multi-mode imaging and photothermal therapy of metastatic prostate cancer

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Chinese Chemical Letters 2025年第2期36卷 289-296页

作者： Ze Wang Hao Liang Annan Liu Xingchen Li Lin Guan Lei Li Liang He Andrew K.Whittaker Bai Yang Quan Lin State Key Laboratory of Supramolecular Structure and materials College of Chemistry Jilin University Department of Endocrinology Lequn Branch the First Hospital of Jilin University Department of Urology the First Hospital of Jilin University australian institute for Bioengineering and Nanotechnology the University of Queensland

Prostate cancer(PCa) is characterized by high incidence and propensity for easy metastasis, presenting significant challenges in clinical diagnosis and treatment. Tumor microenvironment(TME)-responsive nanomaterials provide a promising prospect for imaging-guided precision therapy. Considering that tumor-derived alkaline phosphatase(ALP) is over-expressed in metastatic PCa, it makes a great chance to develop a theranostics system with ALP responsive in the TME. Herein, an ALP-responsive aggregationinduced emission luminogens(AIEgens) nanoprobe AMNF self-assembly was designed for enhancing the diagnosis and treatment of metastatic PCa. The nanoprobe exhibited self-aggregation in the presence of ALP resulted in aggregation-induced fluorescence, and enhanced accumulation and prolonged retention period at the tumor site. In terms of detection, the fluorescence(FL)/computed tomography(CT)/magnetic resonance(MR) multi-mode imaging effect of nanoprobe was significantly improved post-aggregation, enabling precise diagnosis through the amalgamation of multiple imaging modes. Enhanced CT/MR imaging can achieve assist preoperative tumor diagnosis, and enhanced FL imaging technology can achieve “intraoperative visual navigation”, showing its potential application value in clinical tumor detection and surgical guidance. In terms of treatment, AMNF showed strong absorption in the near infrared region after aggregation, which improved the photothermal treatment effect. Overall, our work developed an effective aggregation-enhanced theranostic strategy for ALP-related cancers.

关键词： AIE ALP responsive Enhanced multi-mode imaging Enhanced photothermal therapy Prostate cancer

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Magnetron sputtered nickel oxide with suppressed interfacial defect states for efficient inverted perovskite solar cells

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Journal of Energy Chemistry 2025年第1期100卷 348-355页

作者： Guoqiang Ma Qin Tan Zhaoning Li Jingwei Xiu Jiafeng Wang Tianle Cheng Dong He Qiang Sun Xuhang Ma Francesco Lamberti Zhubing He Department of materials Science and Engineering Institute of Innovative Materials(I2M)Shenzhen Key Laboratory of Full Spectral Solar Electricity Generation(FSSEG)Southern University of Science and Technology(SUSTech)Shenzhen 518055GuangdongChina Core Research Facilities Southern University of Science and TechnologyShenzhen 518055GuangdongChina Department of Chemical Sciences Department of Industrial EngineeringUniversity of PadovaVia Gradenigo 6a35131 PadovaItaly

Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impair device performance in a long-term view,even with surface molecule *** this study,we developed high-quality magnetron-sputtered NiOxthin films through detailed process optimization,and compared systematically sputtered and spin-coated NiOxthin film surfaces from materials to *** sputtered NiOxfilms exhibit improved crystallinity,smoother surfaces,and significantly reduced Ni3+or Ni vacancies compared to their spin-coated ***,the interface between the perovskite and sputtered NiOxfilm shows a substantially reduced density of defect *** solar cells (PSCs) fabricated with our optimally sputtered NiOxfilms achieved a high power conversion efficiency (PCE) of up to 19.93%and demonstrated enhanced stability,maintaining 86.2% efficiency during 500 h of maximum power point tracking under one standard sun ***,with the surface modification using (4-(2,7-dibromo-9,9-dimethylacridin-10(9H)-yl)butyl)p hosphonic acid (DMAcPA),the device PCE was further promoted to 23.07%,which is the highest value reported for sputtered NiOxbased PSCs so far.

关键词： Nickle oxide Magnetron sputter Defect Stability Perovskite solar cell

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Platinum modification of metallic cobalt defect sites for efficient electrocatalytic oxidation of 5-hydroxymethylfurfural

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Journal of Energy Chemistry 2025年第2期101卷 463-473页

作者： Haoyu Zhan Baixue Cheng Yankun Lu Danning Xing Xingshuai Lv Huining Huang Thomas Frauenheim Tao Wang Peng Zhou State Key Laboratory of Bio-fibers and Eco-textiles College of Materials Science and Engineering Collaborative Innovation Center of Shandong Marine Biobased Fibers and Ecological Textiles Institute of Marine Biobased Materials Qingdao University Shandong institute of Advanced Technology College of Chemistry and Chemical Engineering Ocean University of China Tianjin Key Laboratory of Advanced Functional Porous materials Institute for New Energy Materials & Low-Carbon Technologies School of Materials Science and EngineeringTianjin University of Technology School of Science Constructor University Beijing Computational Science Research Center College of Chemistry and Molecular Engineering Qingdao University of Science and Technology

Co3O4possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural（HMF）.However,the enrichment and activation effects of Co3O4on OH-and HMF are weak,which limits its further *** defect engineering can regulate the electronic structure,optimize the adsorption of intermediates,and improve the catalytic activity by breaking the symmetry of the material,which is rarely involved in the upgrading of *** this work,we prepare Co3O4with metal defects and load the precious metal platinum at the defect sites（PtVco）.The results of in-situ characterizatio ns,electrochemical measurements,and theoretical calculations indicate that the reduction of Co-Co coordination number and the formation of Pt-Co bond induce the decrease of electron filling in the antibonding orbitals of Co *** resulting upward shift of the d-band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH species,thus exhibiting excellent HMF oxidation activity(including a lower onset potential（1.14 V） and 19 times higher current density than pure Co3O4at 1.35 V).In summary,this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail,provides a new option for improving the HMF oxidation activity of cobalt-based materials,broadens the application field of metal defect based materials,and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.

关键词： Adsorption enhancement Biomass upgrading Coordination environment Electrocatalysis Metallic defect

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A cellulose-based lithium-ion battery separator with regulated ionic transport and high thermal stability for extreme environments

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Nano Research 2025年第1期18卷 315-322页

作者： Kun-Peng Yang Song Xie Zi-Meng Han Hao-Cheng Liu Chong-Han Yin Wen-Bin Sun Zhang-Chi Ling Huai-Bin Yang De-Han Li Qing-Fang Guan Shu-Hong Yu Department of Chemistry New Cornerstone Science LaboratoryInstitute of Biomimetic Materials&ChemistryAnhui Engineering Laboratory of Biomimetic MaterialsDivision of Nanomaterials&ChemistryHefei National Research Center for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei 230026China institute of innovative materials Department of Materials Science and EngineeringDepartment of ChemistrySouthern University of Science and TechnologyShenzhen 518055China

Separators play a critical role in lithium-ion ***,the restrictions of thermal stability and inferior electrical performance in commercial polyolefin separators significantly limit their applications under harsh ***,we report a cellulose-assisted self-assembly strategy to construct a cellulose-based separator massively and *** an ultrahigh ionic conductivity in electrolytes of 3.7 mS·cm^(-1) and the ability to regulate ion transport,the obtained separator is a promising alternative for high-performance lithium-ion *** addition,integrated with high thermal stability,the cellulose-based separator endows batteries with high safety at high temperatures,greatly expanding the application scenarios of energy storage devices in extreme environments.

关键词： lithium-ion batteries bio-inspired materials battery separators cellulose nanofiber ultrahigh ionic conductivity high safety

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Ca2+ cation-mediated microenvironment for electrochemical hydrodimerization of furfural

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Science China Chemistry 2025年

作者： Wei Du Shuangshuang Cha Can Lei Mengxin Qu Zhongqiang Deng Ming Gong Xinhe Bao Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and innovative materials Fudan University State Key Laboratory of Catalysis National Laboratory for Clean Energy Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences

Furfural is one of the most important biomass-based platform molecules as sustainable precursors for chemicals and fuels. The electrochemical hydrodimerization of furfural can generate hydrofuroin, which is a promising precursor for gasoline or jet ***, steering the selectivity toward hydrodimerization under near-neutral conditions that suppress polymerization and disproportionation of furfural remains challenging. Herein, we discovered that tuning the electrolyte cations could be an effective and alternative strategy for modulating furfural reduction to the traditional electrocatalyst design. Under the optimal Ca2+cations,hydrofuroin yield could be much improved from other cations with hydrofuroin selectivity of 95.5%. The systematic characterization of the ion-centered double layer reflected the suitable sizes and charges of hydrated Ca2+for suppressing the hydrogen evolution reaction from activation of surrounding water molecules as well as encouraging furfural accumulation via non-covalent interaction for directing the electron transfer to furfurals. Ions with smaller or larger sizes can either activate local water molecules or form a crowded ionic interface that casts an adverse effect on furfural enrichment. This work not only presents an effective strategy for facilitating biomass valorization via hydrodimerization but also emphasizes the essential role of the ion-centered microenvironment for steering the electrocatalytic pathways.

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Spatial distribution of landslides in response to the geomorphometric constraints in Darma Valley,Kumaun Himalaya

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山地科学学报（英文） 2025年第1期22卷 48-70页

作者： Mohd SHAWEZ Vikram GUPTA Anand Kumar GUPTA Gautam RAWAT Geomorphology Environmental and Engineering GeologyWadia Institute of Himalayan GeologyDehradun 248001India Academy of Scientific and innovative Research Ghaziabad 201002India Geomorphology Environmental and Engineering GeologyWadia Institute of Himalayan GeologyDehradun 248001India Academy of Scientific and innovative Research Ghaziabad 201002India Department of Geology Sikkim UniversityGangtok 737102India

The Kumaun Himalaya is well-known as a geologically and tectonically complex region that amplifies mass wasting processes,particularly *** study attempts to investigate the interplay between landslide distribution and the litho-tectonic regime of Darma Valley,Kumaun Himalaya.A landslide inventory comprising 295 landslides in the area has been prepared and several morphotectonic proxies such as valley floor width to height ratio(Vf),stream length gradient index(SL),and hypsometric integral(HI)have been used to infer tectonic *** analysis,including basic,linear,aerial,and relief aspects,of 59 fourth-order sub-basins,has been carried out to estimate erosion potential in the study *** result demonstrates that 46.77％of the landslides lie in very high,20.32％in high,21.29％in medium,and 11.61％in low erosion potential zones *** order to determine the key parameters controlling erosion potential,two multivariate statistical methods namely Principal Component Analysis(PCA)and Agglomerative Hierarchical Clustering(AHC)were *** reveals that the Higher Himalayan Zone(HHZ)has the highest erosion potential due to the presence of elongated sub-basins characterized by steep slopes and high *** clusters created through AHC exhibit positive PCA values,indicating a robust correlation between PCA and ***,the landslide density map shows two major landslide *** of these hotspots lies in the vicinity of highly active Munsiyari Thrust(MT),while the other is in the Pandukeshwar formation within the MT's hanging wall,characterized by a high exhumation *** SL and low Vf values along these hotspots further corroborate that the occurrence of landslides in the study area is influenced by tectonic *** study,by identifying erosion-prone areas and elucidating the implications of tectonic activity on landslide distribution,empowers policymakers and government agencies to develop strategies for hazard asse

关键词： Landslides Geomorphometric analysis Multivariate statistical analysis Darma valley Kumaun Himalaya

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HfC–HfO2 modified high/superhigh temperature thermal protection coating for superior hot corrosion resistance and antioxidation performance

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Journal of Advanced Ceramics 2025年第1期14卷 177-191页

作者： Zhiyun Ye Shuqi Wang Shuang Yu Xinrui Zhao Yongchun Zou Guoliang Chen Lei Wen Lina Zhao Guangxi Zhang Yaming Wang Jiahu Ouyang Dechang Jia Yu Zhou State Key Laboratory of Precision Welding&Joining of materials and Structures Harbin Institute of TechnologyHarbin 150001China institute for Advanced Ceramics Harbin Institute of TechnologyHarbin 150001China Key Laboratory of Advanced Structure-Function Integrated materials and Green Manufacturing Technology Harbin Institute of TechnologyHarbin 150001China National Center for materials Service Safety University of Science and Technology BeijingBeijing 100083China Xi’an Aerospace Composites Research institute Academy of Aerospace Propulsion TechnologyXi’an 710025China

With advances in the thrust-weight ratio,the service temperature of gas turbine engines even exceeds 1500℃,which is urgent for the development of high/superhigh-temperature thermal protection systems(TPSs)for long-term *** alloys are increasingly viewed as promising structural materials for high-temperature applications because of their superior high-temperature mechanical strength,but the“pest”catastrophic oxidation greatly restricts their further *** this study,a HfC–HfO2-modified silicide coating was prepared via an innovative method of halide-activated pack cementation(HAPC)combined with liquid-plasma-assisted particle deposition and sintering of niobium alloys,resulting in a composite coating with excellent hot corrosion resistance and high-temperature oxidation *** modified multilayer coating is characterized by the synergistic combination of a dense NbSi2 inner layer and a HfC–HfO2 porous outer layer,resulting in a significant improvement in high-temperature performance compared with that of the single NbSi2 *** corrosion gain of the composite coating is only 13.94 mg·cm−2 after a corrosion time of 200 h at 900℃,and an intact oxide scale surface is observed after oxidation at 1500℃for 500 *** improvement is attributed to the formation of a robust Hf-rich skeleton provided by the deposited HfC–HfO2 layer,which can accelerate the formation of a highly stable corroded layer/oxide *** addition,multiple stress release mechanisms of the composite coating at high temperatures also provide substantial contributions to long-term *** these merits make HfC–HfO2-modified composite coatings on niobium alloys competitive for the development of high/superhigh-temperature thermal protection systems for long-term service.

关键词： thermal protection coating niobium alloys hot corrosion resistance high-temperature oxidation resistance stress releasemechanism

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