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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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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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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy Chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia Key Laboratory of Chemistry and Physics of Rare earth materials School of Chemistry and Chemical Engineering Inner Mongolia University State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Institute of Catalysis Department of Chemistry Zhejiang University National Key Laboratory of Baiyunobo Rare earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Nanorods

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Boosting Oxygen Evolution Reaction Performance on NiFe‑Based Catalysts Through d‑Orbital Hybridization

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Nano-Micro Letters 2025年第1期17卷 281-292页

作者： Xing Wang Wei Pi Sheng Hu Haifeng Bao Na Yao Wei Luo State Key Laboratory of New Textile materials and Advanced Processing Technology Key Laboratory of New Textile Materials and Applications of Hubei ProvinceSchool of Materials Science and EngineeringWuhan Textile UniversityWuhan 430200People’s Republic of China College of Chemistry and Molecular sciences Wuhan UniversityWuhan 430072People’s Republic of China

Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based *** introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in ***,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this *** and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER *** critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.

关键词： NiFe-based catalysts d-orbital coupling Oxygen evolution reaction Anion exchange membrane electrolyzer

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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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Crustal magma oxidation state and endowments in porphyry copper deposits

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Science China earth sciences 2025年第1期 226-236页

作者： Yumin AI Massimo CHIARADIA Chao WU Huayong CHEN Key Laboratory of Mineralogy and Metallogeny Guangzhou Institute of Geochemistry Chinese Academy of Sciences University of Chinese Academy of sciences Department of earth sciences University of Geneva Guangdong Provincial Key Laboratory of Mineral Physics and materials

Porphyry copper deposits（PCDs） supply the majority of the world's copper（Cu） as well as significant amounts of molybdenum（Mo） and gold（Au）. The formation of these deposits is controlled by a variety of geological factors, among which the magmatic oxidation is one of the focuses of current research. This study investigates the redox characteristics of arc magmas by analyzing the ratio of vanadium（V） to scandium（Sc） and its correlation with the oxygen fugacity （fO2） of magmas from arcs of various crustal thicknesses globally. We compiled an extensive dataset of published V/Sc values and studied the partition coefficients of Vand Sc between minerals and silicate melts across various magmatic environments. The results demonstrate that fractional crystallization of magnetite markedly reduces V/Sc values of the residual melt. Furthermore, magnesium number（Mg#） at the onset of magnetite fractionation is strongly positively correlated with fO2of the equilibrium magma. Based on this,the oxidation of arc magmas from different crustal thicknesses can be evaluated. The result suggests that magmas generated in crusts thicker than 20 km tend to be more oxidized with increasing crust thickness. This trend is attributed to enhanced intracrustal differentiation processes involving garnet and amphibole, particularly in mature island and continental arcs. In contrast,magmas in thinner arc crusts（materials, display higher oxidation states than most of their thicker crust counterparts. These findings suggest that both subduction dynamics and crustal thickness play a vital role in determining the oxidation state of arc magmas and, consequently, their capacity to generate PCDs. Highly oxidized, primitive arc magmas are less favorable for PCD formation due to that they tend to experience magnetite fractionation and thus sulfide saturation in the early stage of magma evolution, a process leading to copper depletion. On the contra

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Formation and evolution of supercritical geofluid

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Science China earth sciences 2025年第1期 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

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Synthesis and crystal structure of sodium praseodymium polyphosphate, NaPr(PO_3)_4

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Journal of Rare earths 2009年第1期27卷 1-3页

作者： K.Horchani-Naifer J.Amami M.Férid Research Unit of Rare earth materials National Research Center in Sciences of Materials

Reaction of Na2CO3, Pr6O11 and H3PO4 gave the sodium praseodymium polyphosphate NaPr（PO3）*** title compound crystallized in the monoclinic P21/n space group with a=0.9965（4） nm, b=1.31437（4） nm, c=0.72271（3） nm, β=90.429（3）°, V=0.9465（4） nm3, Z=4, R=0.0493 and wR=0.1266 for 1855 independent *** structure of NaPr（PO3）4 consisted of PrO8 polyhedra sharing oxygen atoms with phosphoric group PO4 to form a three-dimensional framework, delimiting intersecting tunnels in which the sodium ion was *** Na＋ ion was bonded to seven oxygen atoms.

关键词： polyphosphate praseodymium crystal structure infrared spectroscopy rare earths

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Fluoride Conversion Coating on Biodegradable AZ31B Magnesium Alloy

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Journal of materials Science & Technology 2014年第7期30卷 666-674页

作者： Tingting Yan Lili Tan Bingchun Zhang Ke Yang Faculty of materials Science and Engineering Kunming University of Science and Technology Institute of Metal Research Chinese Academic of Sciences

A fluoride conversion coating was successfully prepared on AZ31B magnesium alloy by chemical reaction in hydrofluoric acid. Morphologies, composition, bonding strength, corrosion properties, in vitro cytotoxicity and antibacterial properties of the coating were investigated, respectively. The scanning electron microscopy observations revealed a dense coating with some irregular pores. The thin-film X-ray diffraction analysis indicated that the coating was mainly composed of MgO and MgF2. The electrochemical impedance spectroscopy results showed that the fluoride conversion coating significantly improved the corrosion resistance of AZ31B. The hydroxyapatite formed on the surface of the fluoride coated AZ31 B after being immersed in the simulated blood plasma indicated the good bioactivity of the material. The in vitro cytotoxicity test showed that the fluoride coated AZ31B alloy was not toxic to BMMSCs （human bone marrow-derived mesenchymal stem cells）. It was also found that the fluoride coated AZ31 B alloy had antibacterial capability.

关键词： AZ31B magnesium Fluoride coating Corrosion resistance Cytotoxicity Antibacterial

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Role of matrix phase and electric field gradient in Na_(1/2)Bi_(1/2)TiO_(3)eBaTiO_(3) :ZnO composites

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Journal of Materiomics 2022年第2期8卷 498-510页

作者： Lalitha Kodumudi Venkataraman Till Fromling Jurgen Rodel Department of materials and earth sciences Technical University of DarmstadtGermany

Na_(1/2)Bi_(1/2)TiO_(3)-based materials exhibit potential for applications in high-power *** com-posites of Na_(1/2)Bi_(1/2) TiO_(3)-yBaTiO_(3)(NBTyBT;y denotes mole%)with ZnO inclusions were demonstrated to stabilize a ferroelectric equilibrium that led to enhanced thermal depolarization temperature(T_(d))and increased mechanical quality factor(Q_(m)).This work addresses the influence of the matrix NBTyBT phase by investigating two limiting choices based on symmetry(tetragonal/rhombohedral)and polar(relaxor/ferroelectric)*** the composites constituting the tetragonal NBT9BT(non-ergodic relaxor at room temperature)matrix phase exhibit improved T d,the critical temperatures in the composites with rhombohedral NBT3BT(displaying spontaneous ferroelectric order at room temperature)exhibit only marginal ***,NBT3BT composites feature a 45%increase in Q m,while the corresponding increase is roughly three-fold for the NBT9BT composites.A 3-D Finite Element Method is used to simulate the electric field gradient at the matrix/inclusion interface,with the effective field distribution estimated to be higher than the applied field for highly conducting ZnO *** electrical properties indicate that,while the deviatoric stress at the matrix/inclusion interface stabilizes the ferroelectric equilibrium for the relaxor matrix phase,the stresses disrupt the long-range order for the ferroelectric matrix *** results establish the volume-limit of the second phase to stabilize a ferroelectric equilibrium,in addition to substantiating the role of residual stress evidenced by changes in the polar ***,a comparison of the composites with different NBTyBT phases is presented,with NBT6BT:ZnO composites demonstrating an optimal increase in both T_(d) and Q_(m).

关键词： Thermal depolarization Na_(1/2)Bi_(1/2)TiO_(3) BaTiO_(3) NBT-Based Lead-free composites Hard-type

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