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Tuning the porosity of {Co12IICo8III（μ3-OH）24（X）}11+ supramolecular frameworks by reaction time for D2/H2 separation

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Science China Chemistry 2025年

作者： Zhuozhou Xie Zhu Zhuo Zi-Ang Nan Qing Li Xiufang Li Zi-Xiu Lu Linzhe Lü Jin Liu Luyao Liu Wenjing Wang Wei Wang Daqiang Yuan You-Gui Huang State key laboratory of Structure Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences Xiamen key laboratory of Rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of Sciences State key laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical EngineeringXiamen University

Systematicly tuning the porosities of porous materials is crucial for targeted gas mixture separation,yet it remains a longstanding *** a common strategy,altering the phenylene ring count in the organic building units has been exploited to adjust pore apertures in metal organic frameworks （mOFs） and covalent organic frameworks （COFs）,resulting in only a stepwise pore size variation of approximately 2.8?.Unlike mOFs and COFs,the porosities for supramolecular assembly frameworks are highly dependent on the packings of the molecular building units in the *** above strategy cannot be applied to supramolecular assembly frameworks and other strategies are required to adjust pore apertures in supramolecular frameworks,especially to achieve porous materials with the optimal pore size for D2/H2separation （～3?）.Here,we successfully modulate the porosity of supramolecular frameworks of[CoII1+12CoIII8L12（μ3-OH）24（X）]1clusters （L=mono-deprotonated 1-iminoisoindole-3-amine,X=ClO?4or Cl?） by controlling the duration of self-assembly *** simply adjusting the reaction time,we obtain three[CoII12CoIII8L12（μ3-OH）24（X）]11+supramolecular frameworks:[CoII12CoIII8（μ3-OH）24（ClO4）L12)]·（Cl）4·（HCO2）7（1）,[CoII12CoIII8L12（μ3-OH）24（Cl）]·（ClOI4）4·（Cl）6·（HCO2）·（H2O）10（2）,and[CoI12CoIII8L12（μ3-OH）24（Cl）]·（Cl）11·（H2O）12（3）.The different stacking patterns of the[CoII12CoIII8L12（μ3-OH）24（X）]11+clusters in these frameworks lead to significantly varied stabilities and *** 1 exhibits permanent porosity with interconnected channels and maintains stability under harsh *** contrast,compound 2 is nearly nonporous,and compound 3 becomes unstable upon *** pores of compound 1 show higher affinity to D2than H2,and the pore aperture diameter of compound 1 （～3.06?） meets the optimal porosity for D2/***,compound 1 demonstrates moderate D2/H2separation at 77 K (retention time:～7 min/g for D2/H2/Ne （10/10/80 vol%） in a flow of 5 mL

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Decentralized fault diagnosis of discrete-event systems with unreliable sensors using linear temporal logic

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Science China(Information Sciences) 2025年第1期68卷 322-341页

作者： Weijie DONG Shaoyuan LI Xiang YIN key laboratory of System Control and Information Processing Ministry of EducationDepartment of Automation Shanghai Jiao Tong University

In this paper,we investigate a decentralized diagnosis problem of a discrete-evnt system(DeS) subject to unreliable sensors,where the sensor observations of local diagnosers may be non-deterministic as a result of possible *** studies on decentralized robust diagnosis can only deal with different types of sensor failures separately,e.g.,all sensors suffer from the same type of sensor failures such as intermittent sensor failures or permanent sensor ***,since sensors of different local diagnosers may face different external environments and have different internal characteristics,sensors corresponding to different local diagnosers may also have their own fault *** this paper,we propose a flexible framework of decentralized diagnosis for DeS subject to unreliable sensors such that sensors of different local diagnosers are permitted to have different types of sensor *** this end,we extend the existing decentralized diagnosis framework to the case where there exist common sensors broadcasting their observations to all local *** apply linear temporal logic(LTL) to constrain infinite behaviors of private sensors of local diagnosers and common ***,a new notion of φ-codiagnosability is proposed as the necessary and sufficient condition for the existence of a decentralized diagnoser that works correctly under sensors,satisfying LTL-based sensor ***,we provide an effective approach to verify the φ-codiagnosability.

关键词： discrete event systems decentralized diagnosis codiagnosability automata

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Study on the hydrogen absorption properties of a YGdTbDyHo rare-earth high-entropy alloy

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International Journal of minerals,metallurgy and materials 2025年第1期32卷 127-135页

作者： Tongyue Li Ziliang Xie Wenjiao Zhou Huan Tong Dawen Yang Anjia Zhang Yuan Wu Xiping Song State key laboratory for Advanced metals and materials University of Science and Technology BeijingBeijing 100083China Whole Win(Beijing)materials Sci.&Tech.Co. Ltd.Beijing 100083China

This study investigated the microstructure and hydrogen absorption properties of a rare-earth high-entropy alloy(HeA),*** indicated that the YGdTbDyHo alloy had a microstructure of equiaxed grains,with the alloy elements distributed *** hydrogen absorption,the phase structure of the HeA changed from a solid solution with an hexagonal-close-packed(HCP)structure to a high-entropy hydride with an faced-centered-cubic(FCC)structure without any secondary phase *** alloy demonstrated a maximum hydrogen storage capacity of 2.33 H/m(hydrogen atom/metal atom)at 723 K,with an enthalpy change(ΔH)of-141.09 kJ·mol^(-1)and an entropy change(ΔS)of-119.14 J·mol^(-1)·K^(-1).The kinetic mechanism of hydrogen absorption was hydride nucleation and growth,with an apparent activation energy(e_(a))of 20.90 kJ·mol^(-1).Without any activation,the YGdTbDyHo alloy could absorb hydrogen quickly(180 s at 923 K)with nearly no incubation period *** reason for the obtained value of 2.33 H/m was that the hydrogen atoms occupied both tetrahedral and octahedral *** results demonstrate the potential application of HeAs as a high-capacity hydrogen storage material with a large H/m ratio,which can be used in the deuterium storage field.

关键词： rare-earth high-entropy alloy hydrogen absorption capacity pressure–composition–temperature curves kinetics

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Defects‑Rich Heterostructures Trigger Strong Polarization Coupling in Sulfides/Carbon Composites with Robust electromagnetic Wave Absorption

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Nano-micro Letters 2025年第1期17卷 528-547页

作者： Jiaolong Liu Siyu Zhang Dan Qu Xuejiao Zhou moxuan Yin Chenxuan Wang Xuelin Zhang Sichen Li Peijun Zhang Yuqi Zhou Kai Tao mengyang Li Bing Wei Hongjing Wu mengyang Li Bing Wei Hongjing Wu School of Physics Xidian UniversityXi’an 710071People’s Republic of China School of Advanced materials and Nanotechnology State Key Discipline Laboratory of Wide Band Gap Semiconductor TechnologyXidian UniversityXi’an 710071People’s Republic of China School of microelectronics Xidian UniversityXi’an 710071People’s Republic of China School of Telecommunication engineering Xidian UniversityXi’an 710071People’s Republic of China mOe key laboratory of material Physics and Chemistry Under extraordinary School of Physical Science and TechnologyNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China The ministry of education key laboratory of micro and Nano Systems forAerospace School of Mechanical EngineeringNorthwestern PolytechnicalUniversityXi’an 710072People’s Republic of China

Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic *** methods,however,constrain their delicate ***,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon *** unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in m_(x)S_(y)/carbon composites(m-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial ***“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first ***,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric *** defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.

关键词： Defects-rich heterointerfaces Sulfides Polarization coupling electromagnetic wave absorption

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Deliberate design of mOF-based pre-catalyst rationalizing the structural reconstruction toward efficient oxygen evolution reaction

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Science China Chemistry 2025年

作者： Yunhui Chen meng Tian Zhongqi Zhang Guangzhao Wang Yan Guo Jing Wu Dawei Qi Zhenhua Yan Xiangyu Liu Xi Liu State key laboratory of High-efficiency Coal Utilization and Green Chemical engineering College of Chemistry and Chemical EngineeringNingxia University key laboratory of extraordinary Bond engineering and Advanced materials Technology of Chongqing School of Electronic Information Engineering Yangtze Normal University Frontiers Science Center for New Organic matter Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) State Key Laboratory of Advanced Chemical Power Sources College of Chemistry Nankai University School of Chemistry and Chemical engineering In-situ Center for Physical Sciences Frontiers Science Center for Transformative Molecules Shanghai Jiao Tong University

metal-organic frameworks （mOFs）,that have emerged as promising electrocatalysts in oxygen evolution reaction （OeR）,usually undergo structural reconstruction to form metal hydroxides as active ***,it remains a great challenge to design and synthesize ideal mOF-based pre-catalysts for properly cognizing and utilizing the reconstruction process toward efficient OeR ***,the well-defined mOF-808 is post-modified by 2-hydroxyphosphonoacetic acid （HPAA） to form a micro-adsorber that enables to capture of metal ions ***3+and Ni2+ions are synergistically anchored into the microadsorber,developing a Fe/Ni-containing pre-catalyst that can be dynamically electrooxidized to be an active and stable dual-site electrocatalyst denoted by R-mOF-HPAA@FeNi with abundant metal *** a result,R-mOF-HPAA@FeNi exhibits an excellent OeR performance with a low overpotential of 272 mV and Tafel slope of 35.9 m V dec-1,as well as long-term stability over 300 h at 10 m A *** and theoretical calculations suggest the resulting catalyst mainly follows a lattice oxygen mechanism （LOm） of dual-metal-site mechanism （DmSm）.Owing to the chelating role of HPAA,the post-synthesized mOF-HPAA behaves as a trap to uniformly and firmly adhere Fe3+and Ni2+ions,leading to a functionalized mOF-based pre-catalyst which can be structurally evolved into atomic level-distributed OeR electrocatalysts.

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mutual regulation of microglia and astrocytes after Gas6 inhibits spinal cord injury

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Neural Regeneration Research 2025年第2期20卷 557-573页

作者： Jiewen Chen Xiaolin Zeng Le Wang Wenwu Zhang Gang Li Xing Cheng Peiqiang Su Yong Wan Xiang Li Department of Spine Surgery The First Affiliated HospitalSun Yat-sen UniversityGuangzhouGuangdong ProvinceChina Guangdong Province key laboratory of Orthopedics and Traumatology GuangzhouGuangdong ProvinceChina

Invasive inflammation and excessive scar formation are the main reasons for the difficulty in repairing nervous tissue after spinal cord *** and astrocytes play key roles in the spinal cord injury micro-environment and share a close ***,the mechanisms involved remain *** this study,we found that after spinal cord injury,resting microglia(m0)were polarized into pro-inflammatory phenotypes(mG1 and mG3),while resting astrocytes were polarized into reactive and scar-forming *** expression of growth arrest-specific 6(Gas6)and its receptor Axl were significantly down-regulated in microglia and astrocytes after spinal cord *** vitro experiments showed that Gas6 had negative effects on the polarization of reactive astrocytes and pro-inflammatory microglia,and even inhibited the cross-regulation between *** further demonstrated that Gas6 can inhibit the polarization of reactive astrocytes by suppressing the activation of the Yes-associated protein signaling ***,in turn,inhibited the polarization of pro-inflammatory microglia by suppressing the activation of the nuclear factor-κB/p65 and Janus kinase/signal transducer and activator of transcription signaling *** vivo experiments showed that Gas6 inhibited the polarization of pro-inflammatory microglia and reactive astrocytes in the injured spinal cord,thereby promoting tissue repair and motor function ***,Gas6 may play a role in the treatment of spinal cord *** can inhibit the inflammatory pathway of microglia and polarization of astrocytes,attenuate the interaction between microglia and astrocytes in the inflammatory microenvironment,and thereby alleviate local inflammation and reduce scar formation in the spinal cord.

关键词： astrocytes Axl cell polarization Gas6 Hippo signal inflammatory micro-environment intercellular interaction microglia single-cell sequencing spinal cord injury

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Upcycling of polyethylene terephthalate to1,4-cyclohexanedimethanol in water

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Science China Chemistry 2025年

作者： Shuhui Fang Zhiwen Gao Xinrui Shi min Zhang Wei Zhang Yue Liu State key laboratory of Petroleum molecular & Process engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular Engineering East China Normal University engineering Center for Sustainable Carbon Science and Technology East China Normal University Institute of eco-Chongming

The recycling of waste polyethylene terephthalate（PeT）, an extensively used polymer as plastic and fiber materials, has become an urgent topic due to the rapid generation and accumulation of plastic waste into the environment. Current chemical recycling approaches to depolymerize and convert PeT into 1,4-cyclohexanedimethanol（CHDm）, an important chemical in the production of advanced polyesters, predominantly use organic solvents, such as alcohols or dioxane. Herein, we developed an environmentally friendly and economically viable pathway for converting PeT to CHDm using water as the solvent. In this process, PeT is sequentially hydrolyzed in water, hydrogenated to 1,4-cyclohexane dicarboxylic acid（CHDA）, and then reduced to CHDm. The PeT conversion rate is self-enhanced in aqueous medium via acid-catalyzed hydrolysis by the generated CHDA intermediate. A Pd-based catalyst（e.g., Pd/C） selectively hydrogenates the arene ring of the PeT monomer, terephthalic acid intermediate, and a Ru-Sn/C bimetallic catalyst reduces its COOH to CH2OH group. At optimized reaction conditions, a complete conversion of PeT and 80.1% yield of CHDm are obtained. Alternatively, this approach can also efficiently produce CHDA from PeT, with a yield up to 86.4%.

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Dissecting the cell microenvironment of ovarian endometrioma through single-cell RNA sequencing

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Science China Life Sciences 2025年第1期68卷 116-129页

作者： Jiangpeng Wu Siyu Xia Wenting Ye Yan Sun Jing Cai Fubing Yu Haiping Wen Xiuwei Yi Taikang Li mingwei Chen Jiayun Chen Ge Song Chuanbin Yang Yali Song Jigang Wang Department of Reproductive medicine Dongguan Maternal and Child Health Care Hospital Department of Urology and Shenzhen Clinical Research Centre for GeriatricsShenzhen People's HospitalSouthern University of Science and Technology State key laboratory for Quality ensurance and Sustainable Use of Dao-di Herbs Artemisinin Research Centerand Institute of Chinese Materia MedicaChina Academy of Chinese Medical Sciences Reproductive medicine Center Foshan Women and Children Hospital State key laboratory of Antiviral Drugs School of PharmacyHenan University

Ovarian endometrioma（Oe）, also known as “chocolate cysts,” is a cystic mass that develops in the ovaries due to endometriosis and is a common gynecological condition characterized by the growth of endometrial tissue outside the uterus, leading to symptoms such as dysmenorrhea, pelvic pain, and infertility. However, the precise molecular and cellular mechanisms driving this pathophysiology remain largely unknown, posing challenges for diagnosis and treatment. Here, we employed integrated single-cell transcriptomic profiling of over 52,000 individual cells from endometrial tissues of Oe patients and healthy donors and identified twelve major cell populations. We identified notable alterations in cell type-specific proportions and molecular signatures associated with Oe. Notably, the activation of IGFBP5+macrophages with pro-inflammatory properties, NK cell exhaustion, and aberrant proliferation of IQCG+and KLF2+epithelium are key features and may be the potential mechanisms underlying the pathogenesis of Oe. Collectively, our data contribute to a better understanding of Oe at the single cell level and may pave the way for the development of novel therapeutic strategies.

关键词： ovary high-throughput sequencing transcriptomics gene expression analysis ligand-receptor analysis

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Nano high-entropy oxide cathode with enhanced stability for direct borohydride fuel cells

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Journal of energy Chemistry 2025年第1期100卷 309-316页

作者： Lei Zhang Lingfeng Kuang Lianke Zhang Wen Chu Haiying Qin Jing Zhang Junjing He Hualiang Ni Hongzhong Chi New energy materials Research Center College of Materials and Environmental Engineering Hangzhou Dianzi University School of materials Science and engineering Zhejiang University key laboratory of memS of ministry of education School of Integrated Circuits Southeast University

High-entropy materials have become high-activity electrocatalysis owing to their high-entropy effect and multiple active ***,we synthesize a series of carbon-supported nano high-entropy oxides（HeOs/C）,specifically （PtFeCoNiCu）O/C,using a carbothermal shock （CTS） method for application as a cathode catalyst in direct borohydride fuel cells （DBFCs）.The microstructure of the prepared catalysts was characterized by X-ray photoelectron spectroscopy,X-ray absorption fine structure,and transmission electron *** prepared （PtFeCoNiCu）O/C,with particle sizes ranging from 2 to 4 nm,demonstrates 3.94 transferred electrons towards the oxygen reduction reaction in an alkaline environment,resulting in a minimal H2O2yield of 2.6%.Additionally,it exhibits a Tafel slope of 61 mV dec-1,surpassing that of commercial Pt/C (82 mV dec-1).Furthermore,after 40,000 cycles of cyclic voltammetry（CV） testing,the half-wave potential of （PtFeCoNiCu）O/C shows a positive shift of 3 mV,with no notable decline in the limiting current *** （PtFeCoNiCu）O/C is used as a cathode catalyst in DBFCs,the DBFC achieves a maximum power density of 441 mW cm-2at 60°C and sustains a cell voltage of approximately 0.73 V after 52 h at 30°*** findings confirm that HeO/C is a promising cathode catalyst for DBFCs.

关键词： Direct borohydride fuel cells (DBFC)

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Recombinant chitinase-3-like protein 1 alleviates learning and memory impairments via m2 microglia polarization in postoperative cognitive dysfunction mice

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Neural Regeneration Research 2025年第9期20卷 2727-2736页

作者： Yujia Liu Xue Han Yan Su Yiming Zhou minhui Xu Jiyan Xu Zhengliang ma Xiaoping Gu Tianjiao Xia Department of Anesthesiology Nanjing Drum Tower HospitalAffiliated Hospital of Medical SchoolNanjing UniversityNanjingJiangsu ProvinceChina medical School Nanjing UniversityNanjingJiangsu ProvinceChina Jiangsu key laboratory of molecular medicine Nanjing UniversityNanjingJiangsu ProvinceChina State key laboratory of Pharmaceutical Biotechnology Nanjing UniversityNanjingJiangsu ProvinceChina Department of Anesthesiology Zhongshan HospitalFudan UniversityShanghaiChina

Postoperative cognitive dysfunction is a seve re complication of the central nervous system that occurs after anesthesia and surgery,and has received attention for its high incidence and effect on the quality of life of *** date,there are no viable treatment options for postoperative cognitive *** identification of postoperative cognitive dysfunction hub genes could provide new research directions and therapeutic targets for future *** identify the signaling mechanisms contributing to postoperative cognitive dysfunction,we first conducted Gene Ontology and Kyoto encyclopedia of Genes and Genomes pathway enrichment analyses of the Gene expression Omnibus GSe95426 dataset,which consists of mRNAs and long non-coding RNAs differentially expressed in mouse hippocampus3 days after tibial *** dataset was enriched in genes associated with the biological process"regulation of immune cells,"of which Chill was identified as a hub ***,we investigated the contribution of chitinase-3-like protein 1 protein expression changes to postoperative cognitive dysfunction in the mouse model of tibial fractu re *** were intraperitoneally injected with vehicle or recombinant chitinase-3-like protein 124 hours post-surgery,and the injection groups were compared with untreated control mice for learning and memory capacities using the Y-maze and fear conditioning *** addition,protein expression levels of proinflammatory factors(interleukin-1βand inducible nitric oxide synthase),m2-type macrophage markers(CD206 and arginase-1),and cognition-related proteins(brain-derived neurotropic factor and phosphorylated NmDA receptor subunit NR2B)were measured in hippocampus by western *** with recombinant chitinase-3-like protein 1 prevented surgery-induced cognitive impairment,downregulated interleukin-1βand nducible nitric oxide synthase expression,and upregulated CD206,arginase-1,pNR2B,and brain-derived neurotropic factor expr

关键词： Chil1 hippocampus learning and memory m2 microglia neuroinflammation postoperative cognitive dysfunction(POCD) recombinant CHI3L1

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