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Deciphering Water Oxidation Catalysts:The Dominant Role of Surface chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi * Zhichuan JXu Chun‑Hua Yan State Key Laboratory of Applied Organic chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China Key Laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State Key Laboratory of Baiyunobo rare Earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

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Activatable chemiluminescence probe based on four-arm PEGconjugated-pyropheophorbide-a for in vivo autofluorescence-free imaging of peroxynitrite

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Science China chemistry 2025年

作者： Jianmei Ke Lei Ding Ronggui Lian Cheng Zheng Wenjun Li Aixian Zheng Yupeng Sun Ming Wu Yongyi Zeng Xiaolong Liu Maochun Hong Xiaolong Zhang The United Innovation of Mengchao Hepatobiliary technology Key Laboratory of Fujian Province Mengchao Hepatobiliary Hospital of Fujian Medical University Ganjiang Innovation Academy Chinese Academy of Sciences School of rare Earths University of Science and Technology of China College of chemistry Fuzhou University State Key Laboratory of Structure chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Peroxynitrite（ONOO-） is a highly reactive nitrogen species that plays pivotal roles in cell signal transduction and physiological or pathological progresses. However, commonly used ONOO-optical imaging probes are still hampered by high background/autofluorescence（fluorescence probe）, short emission wavelength, or poor selectivity in the case of chemiluminescence. Herein,we report a facile method to prepare an activatable chemiluminescence probe（PPA-PEG） with good biocompatibility and functionality for in vivo autofluorescence-free imaging of ONOO-. The PPA-PEG consists of pyropheophorbide-a（PPA）, a typical deep red photosensitizer that acts as both the recognition and signaling element, and 4-arm poly（ethylene glycol）(4-arm PEG), which improves the biosafety and water solubility of probe. These components can self-assemble into nanoparticles（namely PPA-PEG nanoprobe） in aqueous solution. The PPA-PEG nanoprobe showed an ultra-low chemiluminescence signal before interacting with ONOO-, but exhibited good selectivity, high sensitivity and a fast response toward ONOO-. The PPAPEG was successfully applied to image cellular ONOO-changes, as well as the endogenous ONOO-changes in inflammation models and subcutaneous or orthotopic hepatocellular carcinoma（HCC） tumors models in living mice. In vitro and in vivo studies verified the good detection and imaging capabilities of PPA-PEG for peroxynitrite, demonstrating suitable tissue penetration and a high signal-to-background ratio（SBR）. Thus, our nanoprobe can serve as a valuable activatable chemiluminescence imaging tool for studying important peroxynitrite-related chemical and biological applications.

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Enhancing anion conductivity in a highly alkali-stable eta topologic Cu(Ⅰ) framework via strong electrostatic repulsion

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Science China chemistry 2025年

作者： Xiaolu Wang Shaohui Guo Chao Suo Fuqiang Zhang Junhao Wang Wenjing Wang Daqiang Yuan Linfeng Liang Xianming Zhang College of chemistry Taiyuan University of Technology institute of Crystalline Materials Shanxi University School of chemistry and Materials Science Shanxi Normal University State Key Laboratory of Structural chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Metal-organic frameworks （MOFs） based on anion exchange membranes （AEMs） have garnered considerable interest,particularly for their potential to enhance ion conductivity by pre-introducing anions into *** approach is recognized as straightforward and effective for improving ion ***,developing high-performance AEMs is limited by the inherent instability and low resistance of *** study presents a novel 1,3,5-triazineμ3-bridged neutral Cu（I） framework,designated SXU-120 （where SXU represents Shanxi University）.This framework is synthesized using melamine,a widely available industrial product,as the starting material,achieving a high space-time yield exceeding 1.1 kg *** organic ligands and metal ions in SXU-120 are 3-connected,forming a rare eta topology with the point symbol 8～***-120 exhibits exceptional stability,even in a 10 M KOH solution,due to its high density of uncoordinated–NH2and carbonyl ***,the framework’s unique one-dimensional channels,characterized by their electronegativity,interact electrostatically with OH-ions,thereby accelerating OH-ion transfer along these ***,the OH-conductivity of this material reaches an impressive 0.49 S cm-1at 90°C under full humidity for 100 h,representing the highest OH-conductivity reported for MOF-based conductors to *** properties make SXU-120 a promising candidate for efficient AEM materials in next-generation industrial applications.

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Endogenous/exogenous dual stimulation“ROS engineering”amplification combined with autophagy-augmented for efficient ferroptosis therapy

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Nano Research 2025年第1期18卷 597-606页

作者： Pengye Du Pengpeng Lei Yuan Liang Ran An Yi Wei Shuyu Liu Jianhao Zheng Hongjie Zhang State Key Laboratory of rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Department of chemistry Tsinghua UniversityBeijing 100084China

“Reactive oxygen species(ROS)engineering”is one of the most promising anti-tumor treatments developed in recent *** explosion of ROS will cause oxidative stress,thereby inducing tumor cell ***,ROS accumulation in tumor cells is eliminated by endogenous cellular self-regulation *** this work,a kind of endogenous/exogenous dual stimulation nanoagent noted as UMZC is *** reaction occurs between NH_(2)-MIL-88B(Fe)contained in UMZC and the overexpression of endogenous H_(2)O_(2)to generate ROS,amplified by endogenous H_(2)S of colon tumor *** addition,NH_(2)-MIL-88B(Fe)also functions to deplete glutathione(GSH)for stopping it from consuming *** nanoparticles at the core of UMZC convert near-infrared into visible light,which excites zinc phthalocyanine to initiate the photochemical reaction that generates more ROS,thus alleviating the lack of tissue penetration depth for visible *** agonist chitosan oligosaccharides induce enhancement of cellular autophagy for disrupting cellular metabolic stress and the resistance to oxidative stress of tumor cells,allowing“ROS engineering”to fully exert anti-tumor *** of ROS generation,GSH depletion,and induced cellular autophagy caused by nanoagents have promoting effects on the occurrence of ***,the nanoagents show the ability to effectively treat colon tumors.

关键词： reactive oxygen species(ROS)engineering upconversion nanoparticles cellular autophagy ferroptosis tumor therapy

Laser Сonoscopiс Research Technique For Single Crystals LiNbO<sub>3</sub>: Mg

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Journal of Modern Physics 2013年第5期4卷 12-17页

作者： O. Y. Pikoul N. V. Sidorov M. N. Palatnikov O. V. Makarova Far Eastern State University of Transportation Khabarovsk Russia tananayev institute of chemistry and technology of rare elementsand Mineral Raw Materials Apatity Russia

Optical homogeneity and subtle features of structural distortions in a series of single crystals of lithium niobate (LiNbO3) of congruent composition doped Mg2+ [0.01 - 5.5 mol%] Investigated by laser conoscopic metho... 详细信息

关键词： Lithium Niobate Conoscopic Patterns Optical Homogeneity

提高锌离子电池低温性能和抑制阴极溶解:V2O5的局部结构和电化学串扰控制（英文）

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Science China Materials 2025年

作者：王俊鹏刘佳玉富达阙兰芳李明春卢灿忠谢奕明 Engineering Research Center of Environment-Friendly Functional Materials Ministry of Education Institute of Materials Physical Chemistry Huaqiao University Xiamen Key Laboratory of rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institutes Chinese Academy of Sciences CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

深入了解温度和相变之间的关系对于提高锌离子电池的电化学效率至关重要.然而,电化学相互作用的复杂性,特别是与长时间结构演变有关的相互作用,仍然是一个谜.在本研究中,我们利用V2O5作为晶体的初始结构模型,通过施加不同的机械研磨强...

深入了解温度和相变之间的关系对于提高锌离子电池的电化学效率至关重要.然而,电化学相互作用的复杂性,特别是与长时间结构演变有关的相互作用,仍然是一个谜.在本研究中,我们利用V2O5作为晶体的初始结构模型,通过施加不同的机械研磨强度来细致地控制晶体缺陷,从而揭开电极反应动力学和整体电化学降解的衰变机制.研究表明,经过研磨的V2O5（GVO）具有稳定的晶体结构,可以抑制钒的溶解/穿梭,减轻电化学过程引起的锌阳极副产物.因此,GVO作为正极材料,在室温和低温下均具有优异的Zn存储容量,在室温和-20℃下分别为380和246 mA h g-1.值得注意的是,GVO阴极在-20℃和1 A g-1条件下,经过1500次循环后,容量保持率为99%,保持比容量为160 mA h g-1这项工作为水锌离子电池（AZIBs）在宽温度范围内的电化学串扰行为提供了新的见解.

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Amino acid assisted aqueous synthesis of highly stable CsPbBr_(3)nanocrystals for cell imaging

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Nano Research 2025年第1期18卷 675-683页

作者： Xue Li Yanan Guo Guoying Tan Qingyi Liu Nan Song Yu Tang State Key Laboratory of Applied Organic chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China State Key Laboratory of Baiyunobo rare Earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030China

Lead halide perovskite nanocrystals(NCs)exhibit excellent optoelectronic performance and have drawn great interests in the fields of biological imaging and ***,the poor stability of CsPbX_(3)(X=Cl,Br,I)in water is still a challenge to hinder their practical *** this work,a facile strategy has been developed for aqueous synthesis of CsPbX_(3) nanocrystals,in which L-glutamic acid(LGlu)has been used to replace oleic acid in the synthetic *** from the synergic effects of L-Glu and oleylamine(OAm),CsPbBr_(3)nanocrystals(L-Glu/OAm-CsPbBr_(3)NCs)with high water stability have been directly prepared under a mild condition at room temperature in water,facilitated by the process of crystal phase transformation from Cs_(4)PbBr_(6) to CsPbBr_(3).L-Glu/OAm-CsPbBr_(3)NCs exhibit a high quantum yield of 85%and a narrow full width at half maximum of 16 nm,demonstrating their efficient luminescence in ***,L-Glu on the surface have contributed greatly to an acidic environment and passivation of surface defects,improving the water stability and dispersibility of CsPbBr_(3)***,L-Glu/OAm-CsPbBr_(3)NCs exhibit great biocompatibility due to the presence of L-Glu,resulting in their good performance for HeLa cell ***,we propose a facile and effective method to prepare CsPbBr_(3)nanocrystals with excellent water stability by using L-Glu and OAm as cooperated ligands and expand their application in cell imaging.

关键词： aqueous synthesis cell imaging lead halide perovskite nanocrystals L-glutamic acid phase transformation

Carbon-supported CeNCl as an efficient catalyst for CO_(2)cycloaddition

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Nano Research 2025年第1期18卷 157-163页

作者： Li Liu Lingling Zhang Xiang Chu Baokang Geng Huilin Wang Zongxiang Li Xiao Wang Shuyan Song Hongjie Zhang School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State Key Laboratory of rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Sinocare Incorporation Changsha 410221China Department of chemistry Tsinghua UniversityBeijing 100084China

The cycloaddition reaction of CO_(2)with epoxide not only effectively reduces the concentration of CO_(2)in the atmosphere,but also has excellent industrial application value and up to 100%atom utilization,but there are difficulties in separation and recovery of traditional homogeneous catalysts,harsh reaction conditions of traditional heterogeneous catalysts,and activation of CO_(2)*** this paper,an easily synthesized heterogeneous catalyst CeNCl/C was used to catalyze the cycloaddition reaction of CO_(2)with styrene oxide,with a high yield of 92.7%,a high selectivity of 96.7%,a turnover numbers(TON)value of 349,and a good stability demonstrated in six cycle tests(equivalent to 216 h of testing).Through comprehensive studies,it was shown that CeNCl/C contains Lewis acid-base centers as active centers,which can effectively reduce the energy barrier required for ring opening of the reaction substrate,enhance the adsorption and activation of CO_(2),and promote the formation of intermediates,which led to the acquisition of excellent catalytic activity.

关键词： CO_(2)cycloaddition heterogeneous catalysis CeNCl Lewis acid/base

Formation and evolution of supercritical geofluid

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Science China Earth Sciences 2025年第1期68卷 39-51页

作者： Huaiwei NI Yilin XIAO Xiaolin XIONG Xiandong LIU Chunxiao GAO Yi-Xiang CHEN Yunguo LI Wan-Cai LI Xuan GUO Yang-Yang WANG Dong-Bo TAN Li ZHANG State Key Laboratory of Lithospheric and Environmental Coevolution University of Science and Technology of China Deep Space Exploration Laboratory/School of Earth and Space Sciences University of Science and Technology of China Guangzhou institute of Geochemistry Chinese Academy of Sciences School of Earth Sciences and Engineering Nanjing University State Key Lab of Superhard Materials Jilin University

In this work, we provide a comprehensive review on the formation, evolution, properties, and effects of supercritical geofluid. In Earth's interior, enhanced miscibility between H2O and silicate by the addition of special components or by the increase of pressure and temperature gives rise to supercritical geofluid with a significant amount of both H2O and silicate *** formation of supercritical geofluid in magmatic-hydrothermal systems, typified by pegmatite system, is governed by meltfluid critical curve. The formation of supercritical geofluid in metamorphic systems, typified by subducted slab, is governed by the second critical end point. Experimental results suggest that the presence of boron and fluorine in pegmatite system makes it possible to form supercritical geofluid at crustal depths, but the release of supercritical geofluid from subducted slab is withheld until almost 100 km depth. A major presence of both H2O and depolymerized structural units（monomers, dimers, etc.） endows supercritical geofluid with unique physical properties including low density, low elastic moduli, low viscosity, high diffusivity,and high electrical conductivity. Supercritical geofluid can effectively mobilize a variety of elements even including high field strength elements and heavy rare earth elements. The chemical signatures of supercritical geofluid can be inherited by metasomatized mantle and mantle-derived melts, and this could give an explanation of the oxidation of arc magmas. Phase separation of supercritical geofluid through the mechanism of spinodal decomposition leads to formation of a melt network. Multiphase fluid inclusions recovered from subduction zone rocks and pegmatites are possible relics of supercritical geofluid. Supercritical geofluid can cause electrical anomaly and low seismic velocity near the top of subducted slab, and can be linked with intermediate-focus earthquakes. Supercritical geofluid may have played a crucial role in the formation of pe

关键词： Supercritical geofluid Miscibility Subduction zone Pegmatite

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