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The first chiral cerium halide towards circularly-polarized luminescence in the UV region

Science China Chemistry 2024年第6期67卷 1961-1968页

作者： Xinyi Niu Zhichao Zeng Zhaoyu Wang Haolin Lu Bing Sun Hao-Li Zhang Yongsheng Chen Yaping Du Guankui Long Tianjin Key Lab for rare earth materials and Applications Renewable Energy Conversion and Storage CenterSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China Tianjin Key Lab for rare earth materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China State Key Laboratory of Applied Organic Chemistry Key Laboratory of Special Function Materials and Structure Design(Ministry of Education)College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China The Centre of Nanoscale Science and Technology and State Key Laboratory of Elemento-Organic Chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China

Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting ***,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely *** fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/*** chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and *** emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV ***,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV *** work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral *** RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.

关键词： chiral rare-earth halide ultraviolet circularly-polarized luminescence d-f transition rare-earth halide perovskite chiral perovskite

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Electrostatically connected nanoarchitected electrocatalytic films for boosted water splitting

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Nano Research 2024年第3期17卷 1114-1122页

作者： Chao-Peng Wang Hao Sun Gang Bian Jia-Xi Wang Xixi Pang Guoqi Wang Jian Zhu Xian-He Bu School of materials Science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin 300350China Tianjin Key Laboratory of Metal and Molecule-Based Material Chemistry Nankai UniversityTianjin 300350China Tianjin Key Laboratory for rare earth materials and Applications Nankai UniversityTianjin 300350China

Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient ***,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)*** particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 ***,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V *** study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.

关键词： layer-by-layer(LbL)assembly layered double hydroxides(LDH) two-dimensional(2D)electrocatalysts oxygen evolution reaction(OER) water splitting

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The proximity between hydroxyl and single atom determines the catalytic reactivity of Rh1/CeO_(2) single-atom catalysts

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Nano Research 2024年第1期17卷 397-406页

作者： Danfeng Wu Shuyun Zhou Congcong Du Juan Li Jianyu Huang Hong-xia Shen Abhaya K.Datye Shan Jiang Jeffrey T.Miller Sen Lin Haifeng Xiong State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350002China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China College of Biology and Chemical Engineering Jiaxing UniversityJiaxing 314000China Department of Chemical&Biological Engineering University of New MexicoAlbuquerqueNM 8731-0001USA Davidson School of Chemical Engineering Purdue UniversityWest LafayetteIN 47907-2100USA Innovation Laboratory for Sciences and Technologies of Energy materials of Fujian Province(IKKEM) Xiamen 361102China Fujian Key Laboratory of rare-earth Functional materials Fujian Shanhai Collaborative Innovation Center of Rare-earth Functional MaterialsLongyan 366300China

The local structure of the metal single-atom site is closely related to the catalytic activity of metal single-atom catalysts(SACs).However,constructing SACs with homogeneous metal active sites is a challenge due to the surface heterogeneity of the conventional ***,we prepared two Rh1/CeO_(2)SACs(0.5Rh1/r-CeO_(2)and 0.5Rh1/c-CeO_(2),respectively)using two shaped CeO_(2)(rod and cube)exposing different facets,i.e.,CeO_(2)(111)and CeO_(2)(100).In CO oxidation reaction,the T100 of 0.5Rh1/r-CeO_(2)SACs is 120°C,while the T100 of 0.5Rh1/c-CeO_(2)SACs is as high as 200°*** in-situ CO diffuse reflectance infrared Fourier transform spectroscopy(CO-DRIFTS),we found that the proximity between OH group and Rh single atom on the plane surface plays an important role in the catalytic activity of Rh1/CeO_(2)SAC system in CO *** Rh single atom trapped at the CeO_(2)(111)crystal surface forms the Rh1(OH)adjacent species,which is not found on the CeO_(2)(100)crystal surface at room ***,during CO oxidation,the OH group far from Rh single atom on the 0.5Rh1/c-CeO_(2)disappears and forms Rh1(OH)adjacent species when the temperature is above 150°*** formation of Rh1(OH)adjacentCO intermediate in the reaction is pivotal for the excellent catalytic activity,which explains the difference in the catalytic activity of Rh single atoms on two different CeO_(2)*** formed Rh1(OH)adjacent-O-Ce structure exhibits good stability in the reducing atmosphere,maintaining the Rh atomic dispersion after CO oxidation even when pre-reduced at high temperature of 500°*** functional theory(DFT)calculations validate the unique activity and reaction path of the intermediate Rh1(OH)adjacentCO species *** work demonstrates that the proximity between metal single atom and hydroxyl can determine the formation of active intermediates to affect the catalytic performances in catalysis.

关键词： crystal plane Rh1/CeO_(2)single-atom catalyst proximity of Rh and hydroxyl coordination structure CO oxidation

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Non-bonding modulations between single atomic cerium and monodispersed selenium sites towards efficient oxygen reduction

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Nano Research 2024年第6期17卷 4753-4763页

作者： Leilei Yin Shuai Zhang Mingzi Sun Siyuan Wang Bolong Huang Yaping Du Tianjin Key Lab for rare earth materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin 300350China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina Research Centre for Carbon-Strategic Catalysis The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina

Currently,dual atomic catalysts(DACs)with neighboring active sites for oxygen reduction reaction(ORR)still meet lots of challenges in the synthesis,especially the construction of atomic pairs of elements from different blocks of the periodic ***,a“rare earth(Ce)-metalloid(Se)”non-bonding heteronuclear diatomic electrocatalyst has been constructed for ORR by rational coordination and carbon support defect ***,the optimized Ce-Se diatomic catalysts(Ce-Se DAs/NC)displayed a half-wave potential of 0.886 V *** hydrogen electrode(RHE)and excellent stability,which surpass those of separate Ce or Se single atoms and most single/dual atomic catalysts ever *** addition,a primary zinc-air battery constructed using Ce-Se DAs/NC delivers a higher peak power density(209.2 mW·cm^(−2))and specific capacity(786.4 mAh·gZn^(−1))than state-of-the-art noble metal catalysts Pt/*** calculations reveal that the Ce-Se DAs/NC has improved the electroactivity of the Ce-N_(4)region due to the electron transfer towards the nearby Se specific activity(SA)***,the more electron-rich Se sites promote the adsorptions of key intermediates,which results in the optimal performances of ORR on Ce-Se DAs/*** work provides new perspectives on electronic structure modulations via non-bonded long-range coordination micro-environment engineering in DACs for efficient electrocatalysis.

关键词： catalyst rare earth oxygen reduction reaction(ORR) metalloid non-bonding modulation

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Synthesis,Structure and Chemical Bonding of Polyantimony Clusters Containing Coinage Metals[M_(2)Sb_(14)]^(4-)(M=Cu,Ag)

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Chinese Journal of Chemistry 2024年第6期42卷 617-622页

作者： Wei-Xing Chen Yu-He Xu Cui-Cui Wang Lei Qiao Zi-Yan Guo Wen-Juan Tian Zhong-Ming Sun State Key Laboratory of Element-Organic Chemistry Tianjin Key Lab for Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin300350 China institute of Molecular Science Shanxi UniversityTaiyuanShanxi030006 China

Binary polyantimony clusters,namely[Cu_(2)Sb_(14)]^(4–) and [Ag_(2)Sb_(14)]^(4–),containing coinage metals,were successfully synthesized and characterized,in which two homoatomic Sb73–subunits are bridged by two coinage metals in η^(4):η^(1) and η^(1):η^(1) coordination modes,***[M_(2)Sb_(14)]^(4-),two bridging Cu ions and two Sb atoms form a planar rhombic unit,which was revealed to have antiaromatic properties by theoretical *** electron structure and bonding analysis confirmed the presence of delocalized bonds in the rhombic unit and the metallophilic interaction between two formal M^(+) ions.

关键词： Polyantimony cluster Copper Silver Antiaromaticity Metallophilic interaction Quantum chemical calculations

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Significant effect of ordered micro-domain on cell boundary phase distribution and demagnetization curve squareness of Sm_(2)Co_(17)-type magnet

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rare Metals 2024年第4期43卷 1724-1735页

作者： Zhuang Liu Hai-Chen Wu Chao-Yue Zhang Chao-Qun Zhu Guo-Xin Chen Huan-Ming Lu Ren-Jie Chen Aru Yan CISRI&NIMTE Joint Innovation Center for rare earth Permanent Magnets Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo315201China University of Chinese Academy of Sciences Beijing100049China Analytical Center Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo315201China

Cu-rich cell boundary phase is difficult to precipitate evenly,resulting in a generally poor demagnetization curve squareness for Fe-rich Sm_(2)Co_(17)-type magnet,which is a key factor limiting the further improvement of magnetic energy *** this study,we report that nanoscale strip-like ordered micro-domains distributed in1:7H disordered matrix phase of the solid solution precursor is a new factor significantly affecting the precipitation and distribution of the cell boundary *** strip-like and continuous micro-twin structure with twin boundaries neatly perpendicular to the C-axis is observed after sintering *** solution treatment,sequential and long strip-like micro-twins gradually transform into disordered state along the basal plane,forming narrow disordered 1:7H(TbCu_(7)-type structure)phase between the separated strip-like ordered *** disordering transformation takes place via broken down of the long strip-like ordered micro-domains,which is accomplished by narrowing along the width direction followed by reduction of the ***,a new model revealing the effect of the ordered micro-domains on the formation of the cell boundary phase is *** boundaries enriched in Cu have already existed in the precursor with long strip-like ordered ***,the Cu-rich cell boundary phase acting as strong pinning centers cannot be precipitated homogeneously and distributed continuously after aging,resulting in a poor demagnetization curve squareness of Sm_(2)Co_(17)-type *** results indicate that significant broken down of the nanoscale ordered micro-domains in solution precursor is the key factor improving the distribution of cell boundary phase in Sm_(2)Co_(17)-type magnets.

关键词： Sm_(2)Co_(17) magnets Solution precursor Ordered micro-domains Disordering transformation Cellular structure

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Exceptional reversed yield strength asymmetry in a rare-earth free Mg alloy containing quasicrystal precipitates

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Journal of Magnesium and Alloys 2024年第2期12卷 687-699页

作者： Qiang Yang Shuhui Lv Zixiang Yan Zefeng Xie Xin Qiu State Key Laboratory of rare earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022PR China School of materials Science and Engineering Changchun University of Science and Technology130022PR China

This work reports an exceptional reversed yield strength asymmetry at room temperature for a rare-earth free magnesium alloy containing a mass of fine dispersed quasicrystal(I-phase)*** exhibiting traditional basal texture,it owns an exceptional CYS/TYS as high as~*** back-scattered diffraction(EBSD)and transmission electron microscopy(TEM)examinations indicate pyramidal and prismatic dislocations plus tensile twinning being activated after immediate yielding in compression while basal and non-basal dislocations in tension.I-phase particles transferred the concentrated stress by self-twinning to provide the driving force for tensile twin initiating in neighboring grains,thereby significantly increasing the critical resolved shear stress of tensile twinning to possibly the level of pyramidal slip,finally leading to the dominance of pyramidal slip plus tensile twinning in texture *** results in a higher contribution on yield strength by~55 MPa in compression than in tension,which reasonably agrees with the experimental yield strength difference(~38 MPa).It can be concluded that I-phase particles influence deformation modes in tension and in compression,finally result in reversed yield strength asymmetry.

关键词： Magnesium alloy Reversed yield strength asymmetry Transmission electron microscopy(TEM) Twinning Dislocations

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Enhanced mechanical property by introducing bimodal grains structures in Cu-Ta alloys fabricated by mechanical alloying

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Journal of materials Science & Technology 2024年第5期172卷 104-112页

作者： Ningyu Li Yongqin Chang Mingyang Li Yuxiang Chen Xinrui Luo Shichao Pei Fan Yang School of materials Science and Engineering University of Science and Technology BeijingBeijing 100083China Xi’an rare Metal materials institute Co.Ltd Xi’an 710016China

Dispersion-strengthened copper alloys can achieve ultra-high strength,but usually at the expense of *** this study,a strategy for overcoming strength-ductility tradeoffof Cu alloys is realized through the introduction of bimodal grains ***-Ta alloys with only 0.5 at.%Ta content were successfully prepared by mechanical alloying combined with spark plasm *** samples prepared by one-step and two-step ball milling methods are named as Cu-Ta(Ⅰ)and Cu-Ta(Ⅱ),*** microstructural characterizations revealed that ultra-fine equiaxed grains with uniformly dispersed Ta precipitates were obtained in the Cu-Ta *** strength of 377 MPa for yield strength together with elongation of∼8%was obtained in Cu-Ta(Ⅰ).Bimodal grains structures composed of fine-grain zones and coarse-grain zones were successfully introduced into Cu-Ta(Ⅱ)by a two-step ball milling approach,and both yield strength(463 MPa)and elongation(∼15%)were significantly synergistic *** hardness values of both Cu-Ta(Ⅰ)and Cu-Ta(Ⅱ)were almost kept nearly constant with the increase of annealing time,and the softening temperatures of Cu-Ta(Ⅰ)and Cu-Ta(Ⅱ)are 1018 and 1013℃,reaching 93.9%and 93.5%T m of pure Cu(1083℃),*** reveals that the Cu-0.5 at.%Ta alloys exhibit excellent thermal stability and exceptional softening *** nanoclusters with semi-coherent structures play an essential role in enhancing the strength and microstructural stability of *** structures are beneficial to the activation of back stress strengthening and the initiation and propagation of microcracks,thus obtaining the extraordinary combination of strength and *** study provides a new way to fabricate dispersion-strengthened Cu alloys with high strength,high elongation,excellent thermal stability and softening resistance,which have potential application value in the field of the future fusion reactor.

关键词： Cu-Ta alloy Mechanical alloying Ta precipitates Bimodal structures Mechanical property

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Surface-induced interaction of colloidal particles in isotropic liquid crystals

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Communications in Theoretical Physics 2024年第7期76卷 114-122页

作者： Hualing Zhang Kaifeng Weng Rui Ma Department of Physics College of Physical Science and TechnologyXiamen UniversityXiamen 361005China Fujian Provincial Key Laboratory for Soft Functional materials Research Research Institute for Biomimetics and Soft MatterXiamen UniversityXiamen 361005China

In this work,we study the interaction between two colloidal particles in a liquid crystal that is in the isotropic *** interaction is caused by surface-induced polarization of the liquid crystal molecules in the vicinity of the *** find that the interaction is short-ranged in both 2D and 3D *** symmetric homeotropic anchoring conditions,the interaction is *** under anti-symmetric homeotropic anchoring conditions,the interaction is repulsive at short distances but attractive at intermediate *** particle size has a strong impact on the effective interaction force.

关键词： surface-induced interaction colloidal particles liquid crystals

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Carbon-based supports for the electrocatalysis under industrially relevant conditions

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Science China Chemistry 2024年第4期67卷 1051-1055页

作者： Xue Yang Xianrui Gu Yang Song Guolin Hou Cheng Wang Lichen Liu Wei Lin Center for Renewable Energy SINOPEC Research Institute of Petroleum ProcessingBeijing 100083China Engineering Research Center of Advanced rare earth materials Department of ChemistryTsinghua UniversityBeijing 100084China

1 *** materials are ideal catalyst supports for functional metal components due to their appropriate physicochemical characteristics,such as high surface areas,tunable pore structures,variable morphologies and versatile surface properties based on chemical modifications,low cost and facile preparations from diverse precursors[1,2].

关键词： versatile facile supports

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