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

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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 diodes.However,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 reported.To 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/S-MCC.The 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 CPL.The 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 region.Notably,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV CPL.Our work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral OIHMH.The 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

Enhanced cyclic stability of partially disordered spinel cathodes through direct fluorination with gaseous fluorine

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rare Metals 2024年第4期43卷 1635-1646页

作者： Yong-Nian Ma Ling-Chen Kong Shao-Shan Chen Yong Wang Li-Dong Sun Cong Peng Meng-Meng Qin Yu Li Wei Feng Tianjin Key Laboratory of Composite and functional materials School of Materials Science and EngineeringTianjin University institute of advanced Technology and Equipment Beijing University of Chemical Technology

Spinel-type cathodes are considered an optimal substitute for conventional layered oxide cathodes owing to their use of inexpensive and earth-abundant manganese as the redox-active element.Moreover,the introduction of cation disorder can effectively suppress the detrimental two-phase reaction to realize high capacities in a wide voltage range.However,the continuous capacity decay during cycles has hindered the widespread application of these cathode materials.inorganic fluorides exhibit excellent electrochemical stability at high voltage;therefore,in this study,the direct F2 gas reaction with a partially disordered spinel cathode(Li1.6Mn1.6O3.7F0.3,LMOF1.6) was initially applied to investigate the impacts of fluorination on the surface structure and electrochemical performances.The inorganic fluorinated layer,mainly containing LiF,was distributed uniformly on the surface of LMOF1.6nanoparticles after fluorination for an appropriate time without the turbulence caused by the valency of manganese cation,which improved the capacity retention and rate capability by the suppression of structural damage,parasitic reaction,and cation dissolution.The LMOF1.6cathode fluorinated for 0.5 h exhibited a capacity of283.6 mAh·g-1at 50 mA·g-1and an enhanced capacity retention of 29.6% after 50 cycles in the voltage range of1.5-4.8 V,as compared to the pristine LMOF1.6 with only27.9% capacity retention.

关键词： Spinel-type cathodes Direct fluorination Capacity retention ability High rate capability

Polarization engineering in porous organic polymers for charge separation efficiency and its applications in photocatalytic aerobic oxidations

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science China Chemistry 2024年第3期67卷 1000-1007页

作者： Kun Wu Pei-Wen Cheng Xin-Yi Liu Ji Zheng Xiao-Wei Zhu Mo Xie Puxin Weng Weigang Lu Dan Li College of Chemistry and materials science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China Guangdong rare earth Photofunctional materials engineering Technology Research center School of Chemistry and EnvironmentJiaying UniversityMeizhou 514015China

Photocatalytic aerobic oxidation reactions are largely governed by the efficiency of charge separation and subsequent reactive oxygen species(ROS) generation. Herein, we report a polarization engineering strategy to promote the charge separation and ROS generation efficiency by substituting the benzene unit with furan/thiophene in porous organic polymers(POPs). Benefiting from the extent of local polarization, the thiophene-containing POP(JNU-218) exhibits the best photocatalytic performance in aerobic oxidation reactions, with a yield much higher than those for the furan-containing POP(JNU-217) and the benzenecontaining POP(JNU-216). Experimental studies and theoretical calculations reveal that the increase of local polarization can indeed reduce the exciton binding energy, and therefore facilitate the separation of electron-hole pairs. This work demonstrates a viable strategy to tune charge separation and ROS generation efficiency by modulating the dipole moments of the building blocks in porous polymeric organic semiconductors.

关键词： porous organic polymer local polarization photocatalytic aerobic oxidation charge separation reactive oxygen species exciton binding energy

Strategy of preparing SmCo based films with high coercivity and remanence ratio achieved by temperature and chemical optimization

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Journal of rare earths 2024年第7期42卷 1289-1297页

作者： Yansong Gong Zhaoguo Qiu Sizhe Liang Xinrui Zheng Hongxia Meng Zhigang Zheng Deyang Chen Shengfu Yuan Weixing Xia Dechang Zeng J.P.Liu school of materials science and engineering South China University of Technology Zhongshan R&D center for materials Surface and Thin Films Technology of the South China University of Technology Gent Materials Surface Technology(Guangdong) Co.Ltd. institute for advanced materials South China Academy of Advanced OptoelectronicsSouth China Normal University Yangjiang Branch Guangdong Laboratory Materials Science and Technology Yangjiang Advanced Alloys Laboratory Laboratory of rare-earth Magnetic functional materials Ningbo Institute of Material Technology and EngineeringChinese Academy of Sciences Department of Physics University of Texas at Arlington

SmCo based films with excellent intrinsic magnetic properties have promising applications in microelectro-mechanical system（MEMS）.However,due to the complexity of phase composition and uncontrollable crystallization degree of SmCo hard magnetic phase in the film,both the coercivity（Hc） and remanence（Mr） of films are difficult to enhance simultaneously.In this paper,SmCo based films were deposited with a Cr underlayer and capping layer on single crystal Si substrates via magnetron sputtering process.The effects of annealing parameters and Sm/Co atomic ratio on the phase structure and coercivity of films are discussed.By adjusting the Sm/Co atomic ratio from 1:5 to 1:4,Co soft magnetic phase disappears and the single phase SmCo5is obtained,leading to the increase of coercivity of the films from30 to 34 kOe.The influence of deposition temperature and Cu doping on magnetic properties of SmCo based films was investigated.When the deposition temperature increases from room temperature to250℃,the coercivity will further increase from 34 to 51 kOe.However,a severe kink is observed in the demagnetization curves due to the poor exchanged coupling.An analysis of transmission electron microscopy（TEM） confirms that the average size of non-hard magnetic amorphous phase exceeds the effective exchanged coupling length of SmCo5,which contributes to the decoupling and low remanence ratio.Therefore,doping Cu and applying a post-annealing process can significantly improve the crystallization degree of the films.Both the coercivity and the remanence ratio of the demagnetization curves are greatly enhanced.We propose a plausible strategy to prepare the SmCo based films with high coercivity and remanence ratio by temperature and chemical optimization,which can be utilized in high performed MEMS devices.

关键词： Coercivity Crystallization conditions Phase composition rare earths Remanence ratio SmCo based films

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 table.Herein,a“rare earth(Ce)-metalloid(Se)”non-bonding heteronuclear diatomic electrocatalyst has been constructed for ORR by rational coordination and carbon support defect engineering.Encouraging,the optimized Ce-Se diatomic catalysts(Ce-Se DAs/NC)displayed a half-wave potential of 0.886 V vs.reversible hydrogen electrode(RHE)and excellent stability,which surpass those of separate Ce or Se single atoms and most single/dual atomic catalysts ever reported.In 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/C.Theoretical 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)sites.Meanwhile,the more electron-rich Se sites promote the adsorptions of key intermediates,which results in the optimal performances of ORR on Ce-Se DAs/NC.This 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

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 electrolyzers.Here,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)fashion.In 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 h.Furthermore,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 battery.This 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

Growth,optical dispersion and magnetic behavior of Dy^(3+) doped yttrium iron garnet crystals

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Journal of rare earths 2024年第6期42卷 1110-1117,I0004页

作者： Yating Fang Hui Shen Yudie Ma Shijie Liao Shuang Xia Tian Tian Ding Zhou Yunfeng Ma Jiayue Xu institute of Crystal Growth School of Materials Science and EngineeringShanghai Institute of Technology national engineering center of Electromagnetic Radiation Control materials School of Electronic Science and EngineeringUniversity of Electronic Science and Technology of China

Y_(3)Fe_(5)O_(12)(YIG)crystals are highly desirable for the fabrication of mid-infrared isolators with the rapid growth of optical communications,although it is rather challenging to grow large size and high-quality single crystals.Dy^(3+)doping is expected to improve the optical and magneto-optical prope rties.However,high quality Dy:YIG crystals and the adjustment of Dy^(3+)on the structure and optical behavior of YIG crystal remain unclear,impeding its practical applications.Herein,a series of Y_(3-x)Dy_(x)Fe_(5)O_(12)(x=0,0.5,1.0,1.5,3)solid solution crystals was grown by the flux-Bridgman method and single crystals up to 25 mm were obtained.With the introduction of Dy^(3+),lattice parameters are gradually enlarged from 1.2379 nm(YIG)to 1.2420 nm(DyIG).Typical Dy^(3+)absorption peaks are observed around 1070,1265 and 1670 nm.The refractive index decreases from 2.37(500 nm)to 2.10(2500 nm)for YIG crystal,and it reduces from 2.47(500 nm)to 2.16(2500 nm)for DyIG crystal.The optical bandgaps remain almost unchanged for Dy:YIG crystals.The optical dispersion of the refractive indices was finely fitted by the Wemple and DiDomenico(WDD)and the Sellmeier models,respectively.With the increase of Dy^(3+)content,the saturation magnetization(Ms)decreases significantly from 23.62 emu/g(YIG)to 5.33 emu/g(DyIG).Small coercive field is persisted for this system,endowing small external magnetic field.These results provide valuable references for the manipulation of rare earths on the properties of magnetooptical crystals,which is beneficial to the design of high-performance garnet crystals for the application of optical switching and non-reciprocal related devices.

关键词： Magneto-optical crystal Yttrium iron garnet Dy^(3+)doping Crystal growth Optical dispersion rare earths

Giant low-field reversible magnetocaloric effect at liquid helium temperature of niobium and iron co-substituted EuTiO_(3) compounds

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Journal of rare earths 2024年第4期42卷 710-715页

作者： Zhihong Hao Quanyi Liu Huicai Xie Yan Zhang Zhaojun Mo school of rare earth and New materials engineering Ganzhou Innovation Center of Rare Earth Permanent Magnet Material Advanced Manufacturing and Intelligent Equipment TechnologyGannan University of Science and TechnologyGanzhou341000China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou34119China school of materials science and engineering Taiyuan University of Science and TechnologyTaiyuan030024China

Giant magnetocaloric effect(MCE)materials in the liquid helium temperature region have attracted a lot of attention in the field of low-temperature magnetic refrigeration(MR).In this study,a series of niobium(Nb)and iron(Fe)co-substituted EuTiO_(3) perovskites with cubic structure(space group pm3m)was successfully fabricated,and their magnetic properties as well as cryogenic magnetocaloric effects were investigated in detail.As expected,the introduction of Nb and Fe can significantly modulate the magnetic phase transition and magnetocaloric effect of the EuTiO_(3) compounds.With increasing Fe concentration,two local minima corresponding to the AFM-FM magnetic phase transition near 5.0 K and FM-PM transition near 10 K with no hysteresis in the thermomagnetic curves are observed,which is attributed to an enhancement of FM coupling.At the same time,the gradually widened-ΔSM-T curves and the two peaks with a broad shoulder lead to considerable refrigeration capacity(RC).With the field change ofΔH=2 T,the calculated values of-ΔS_(M)^(max) for the EuTi_(0.9375-x)Nb_(0.0625)Fe_(x)O_(3)(x=0.075,0.1,0.125,0.15)compounds are 24.2,17.6,14.5 and 14.0 J/(kg·K),respectively.The corresponding RC values were calculated to be 144.6,138.3,151.2 and 159 J/kg,respectively.Especially,the values of-ΔS_(M)^(max) for EuTi_(0.8625)Nb_(0.0625)Fe_(0.075)O_(3) are 8.6 and 15.1 J/(kg·K)under low field changes of 0.5 and 1 T,respectively.The giant low-field reversible magnetocaloric effect makes them attractive candidates for magnetic refrigeration in the liquid helium temperature region.

关键词： Magnetocaloric effect Refrigeration capacity Magnetic entropy change rareearths

Atomically Dispersed Ruthenium Catalysts with Open Hollow Structure for Lithium-Oxygen Batteries

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Nano-Micro Letters 2024年第2期16卷 154-164页

作者： Xin Chen Yu Zhang Chang Chen Huinan Li Yuran Lin Ke Yu Caiyun Nan Chen Chen Beijing advanced Innovation center for materials Genome engineering Institute of Solid State ChemistryUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China engineering Research center of advanced rare earth materials Department of ChemistryTsinghua UniversityBeijing 100084People’s Republic of China Beijing Key Laboratory of Energy Conversion and Storage materials Institution College of ChemistryBeijing Normal UniversityBeijing 100875People’s Republic of China

Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.

关键词： Atomically dispersed Open hollow structure Discharge product Lithium Oxygen battery