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Pillar effect induced by ultrahigh phosphorous/nitrogen doping enables graphene/MXene film with excellent cycling stability for alkali metal ion storage

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Journal of Energy Chemistry 2024年第6期93卷 146-156,I0004页

作者： Meng Qin Yiwei Yao Junjie Mao Chi Chen Kai Zhu Guiling Wang Dianxue Cao Jun Yan Key Laboratory of Superlight materials and Surface Technology Ministry of EducationCollege of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001HeilongjiangChina xiamen Key Laboratory of rare earth Photoelectric Functional materials and Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021FujianChina

Graphene's large theoretical surface area and high conductivity make it an attractive anode material for potassium-ion batteries(PIBs).However,its practical application is hindered by small interlayer distance and long ion transfer distance.Herein,this paper aims to address the issue by introducing MXene through a simple and scalable method for assembling graphene and realizing ultrahigh P doping content.The findings reveal that MXene and P-C bonds have a "pillar effect" on the structure of graphene,and the P-C bond plays a primary role.In addition,N/P co-doping introduces abundant defects,providing more active sites for K^(+) storage and facilitating K^(+) adsorption.As expected,the developed ultrahigh phosphorous/nitrogen co-doped flexible reduced graphene oxide/MXene(NPrGM) electrode exhibits remarkable reversible discharge capacity(554 mA hg^(-1) at 0.05 A g^(-1)),impressive rate capability(178 mA h g^(-1) at 2 A g^(-1)),and robust cyclic stability(0.0005% decay per cycle after 10,000 cycles at 2 A g^(-1)).Furthermore,the assembled activated carbon‖NPrGM potassium-ion hybrid capacitor(PIHC) can deliver an impressive energy density of 131 W h kg^(-1) and stable cycling performance with 98.1% capacitance retention after5000 cycles at 1 A g^(-1).Such a new strategy will effectively promote the practical application of graphene materials in PIBs/PIHCs and open new avenues for the scalable development of flexible films based on two-dimensional materials for potential applications in energy storage,thermal interface,and electromagnetic shielding.

关键词： Graphene MXene Phosphorous doping Pillar effect Potassium-ion batteries

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Efficient Spin-Flip between Charge-Transfer States for High-Performance Electroluminescence, without an Intermediate Locally Excited State

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Research 2024年第1期2023卷 339-349页

作者： Donghai Zhang Shanshan Jiang Xiaodong Tao Fulin Lin Lingyi Meng Xu-Lin Chen Can-Zhong Lu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian 350108China xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamenFujian 361021China University of Chinese Academy of Sciences Beijing 100049China

Thermally activated delayed fluorescence(TADF)materials with both high photoluminescence quantum yield(PLQY)and fast reverse intersystem crossing(RISC)are strongly desired to realize efficient and stable organic light-emitting diodes(OLEDs).Control of excited-state dynamics via molecular design plays a central role in optimizing the PLQY and RISC rate of TADF materials but remains challenging.Here,3 TADF emitters possessing similar molecular structures,similar high PLQYs(89.5%to 96.3%),and approximate energy levels of the lowest excited singlet states(S_(1)),but significantly different spin-flipping RISC rates(0.03×10^(6) s^(−1) vs.2.26×10^(6) s^(−1))and exciton lifetime(297.1 to 332.8μs vs.6.0μs)were systematically synthesized to deeply investigate the feasibility of spin-flip between charge-transfer excited states(^(3)CT–^(1)CT)transition.

关键词： transition lifetime desired

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High-entropy rare earth stannate ceramics:Acid corrosion resistant radiative cooling materials with high atmospheric transparency window emissivity and high near-infrared solar reflectivity

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Journal of Advanced Ceramics 2024年第5期13卷 630-640页

作者： Tao Chen Yanyan He Yanyu Pan Kaixian Wang Minzhong Huang Liyan Xue Yazhu Li Fan Yang Yanchun Zhou Heng Chen Fujian institute of Research on the Structure of Matter Chinese Academy of SciencesFuzhou 350002China College of Chemistry and materials Science Fujian Normal UniversityFuzhou 350117China xiamen institute of rare earth materials Haixi InstitutesChinese Academy of SciencesXiamen 361021China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China Key Laboratory of rare earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhou 341000China School of materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China

In response to the development of the concepts of“carbon neutrality”and“carbon peak”,it is critical to developing materials with high near-infrared(NIR)solar reflectivity and high emissivity in the atmospheric transparency window(ATW;8–13μm)to advance zero energy consumption radiative cooling technology.To regulate emission and reflection properties,a series of high-entropy rare earth stannate ceramics(HE-RE_(2)Sn_(2)O_(7):(Y_(0.2)La_(0.2)Nd_(0.2)Eu_(0.2)Gd_(0.2))_(2)Sn_(2)O_(7),(Y_(0.2)La_(0.2)Sm_(0.2)Eu_(0.2)Lu_(0.2))_(2)Sn_(2)O_(7),and(Y_(0.2)La_(0.2)Gd_(0.2)Yb_(0.2)Lu_(0.2))_(2)Sn_(2)O_(7))with severe lattice distortion were prepared using a solid phase reaction followed by a pressureless sintering method for the first time.Lattice distortion is accomplished by introducing rare earth elements with different cation radii and mass.The as-synthesized HE-RE_(2)Sn_(2)O_(7)ceramics possess high ATW emissivity(91.38%–95.41%),high NIR solar reflectivity(92.74%–97.62%),low thermal conductivity(1.080–1.619 W·m^(−1)·K^(−1)),and excellent chemical stability.On the one hand,the lattice distortion intensifies the asymmetry of the structural unit to cause a notable alteration in the electric dipole moment,ultimately enlarging the ATW emissivity.On the other hand,by selecting difficult excitation elements,HE-RE_(2)Sn_(2)O_(7),which has a wide band gap(Eg),exhibits high NIR solar reflectivity.Hence,the multi-component design can effectively enhance radiative cooling ability of HE-RE_(2)Sn_(2)O_(7)and provide a novel strategy for developing radiative cooling materials.

关键词： radiative cooling materials high-entropy ceramics(HECs) rare earth stannate(RE_(2)Sn_(2)O_(7)) high atmospheric transparency window emissivity high near-infrared(NIR)solar reflectivity

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Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and Electrocatalysis with Model Molecules

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Nano-Micro Letters 2024年第7期16卷 74-97页

作者： Wei Guo Linhui Yu Ling Tang Yan Wan Yangming Lin CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021People’s Republic of China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China institute of Urban Environment Chinese Academy of SciencesXiamen 361021People’s Republic of China

Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Over the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction mechanisms.However,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental methods.In this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon catalysis.Using both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically studied.Combined with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular level.Furthermore,the outlook of model carbon catalysis has also been proposed in this work.

关键词： Metal-free carbon catalysts Model catalyst Electrocatalysis Active site Reaction mechanisms

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ⅢA-ⅡB multicomponent perovskite rare earth ferrites with promising electromagnetic wave absorption properties

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Journal of rare earths 2024年第6期42卷 1118-1127,I0005页

作者： Yanyan He Tao Chen Yanyu Pan Minzhong Huang Kaixian Wang Liyan Xue Yazhu Li Fengzhi Tan Fan Yang Tongkuan Xu Heng Chen School of Light Industry and Chemical Engineering Dalian Polytechnic UniversityDalian116034China xiamen institute of rare earthmaterials Haixi InstitutesChinese Academy of SciencesXiamen36021China Fujian institute of Research on the Structure of Matter Chinese Academyof SciencesFuzhou350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China xiamen Key-Laboratoryof rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen361021China Key Laboratory of rare earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhou3410ooChina

Perovskite-type rare-earth ferrites(REFeO_(3))are promising materials for absorbing electromagnetic(EM)wave pollution.However,insufficient dielectric loss and poor impedance matching are key factors that limit the broader implementation of REFeO_(3).Herein,a series of multicomponent perovskite-type ferrites with strong EM wave absorption capabilities was prepared.Through the synergistic effect of chemical constitution regulation and entropy regulation,optimization of the dielectric loss and impedance matching is achieved by strengthening the structural defect mechanism,thus further adjusting the EM wave absorption performance.Compared with(LaGdSmNdBa)FeO_(3)(HE-1)and(LaGdPrSmNdBa)FeO_(3)(HE-2),(LaGdBa)FeO_(3)(ME-1)and(LaGdSmBa)FeO_(3)(ME-2)exhibit favorable performance,with optimal minimum reflection loss(RL_(min))of-56.35 dB(at 11.12 GHz)and-63.25 dB(at 7.22 GHz)and effective absorption bandwidth(EAB)of 4.46 and 4.72 GHz,respectively.This multicomponent design provides a new strategy for the development of EM wave absorption materials.

关键词： rare earths Multicomponent design rare earth ferrites Entropy regulation Electromagnetic wave absorption

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X-ray-activated Bi^(3+)/Pr^(3+)co-doped LiYGeO_4 phosphor with UV and NIR dual-emissive persistent luminescence

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Journal of rare earths 2024年第5期42卷 955-961,I0005页

作者： Xianggui Yin Hongyun Zhong Lin Liu Junpeng Shi Xia Sun Yun Zhang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen361021China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China

X-ray-activated luminescence materials have broad application prospects in photodynamic therapy of deep tissue.Among them,X-ray-activated persistent luminescence materials(PLMs)exhibiting multiple emission peaks have drawn extensive attention for the ir capacity to achieve a combination of bioimaging and therapeutic functions.Here,we developed a novel PLM,LiYGeO_4:Bi^(3+),Pr^(3+),that simultaneously exhibits UV and NIR dual persistent luminescence(PersL)emissions after irradiation by X-ray.The material can be re peatedly excited by X-ray and emits similar lumine scence intensity every time,which shows good PersL stability.In addition,LiYGeO_4:Bi^(3+),Pr^(3+)exhibits photostimulated PersL properties by stimulation with a red light-emitting diode(LED)or NIR laser after long-term decay.This work provides a new choice of X-ray-excited PLMs with UV and NIR dual emission and the novel phosphor shows promise as a potential candidate for the integration of treatment and diagnosis of deep tumors.

关键词： Co-doping X-ray-activated Dual emissions Persistent luminescence rare earths

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Novel 2D bifunctional layered rare-earth hydroxides@GO catalyst as a functional interlayer for improved liquid-solid conversion of polysulfides in lithium-sulfur batteries

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Chinese Chemical Letters 2024年第5期35卷 434-440页

作者： Haodong Wang Xiaoxu Lai Chi Chen Pei Shi Houzhao Wan Hao Wang Xingguang Chen Dan Sun CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and materials Fujian Normal UniversityFuzhou 350007China xiamen institute of rare earth materials Haixi InstitutesChinese Academy of SciencesXiamen 361021China School of Microelectronics Hubei UniversityWuhan 430062China xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen 361021China

The detrimental“shuttle effect”of lithium polysulfides(LiPSs)together with sluggish multi-order reaction kinetics are the main drawbacks hindering lithium-sulfur(Li-S)batteries from commercial success.Here,we first propose the implementability of layered rare-earth hydroxides(LREHs)in Li-S batteries to optimize electrochemical performance.In this work,a two-dimensional(2D)rare-earth-based composite constructed by the layered gadolinium hydroxy chloride[Gd_(2)(OH)_(5)(H_(2)O)_(n)]Cl nanoplates(LGdH NPs)and graphene oxide(GO)was designed as a sulfur immobilizer for Li-S batteries.Combining the experimental results and density functional theory(DFT)calculations,it is revealed that the LGdH@GO composite not only provides a strong anchoring of the intermediates during cycling,but also acts as an effective catalyst to accelerate the liquid-solid conversion of polysulfides.The Li-S batteries assembled by LGdH@GO modified separators delivered a superior rate performance with a specific capacity of 605.34 mAh/g at 5 C,as well as excellent cycle stability with a decay rate of 0.087%over 500 cycles at 2 C.This study provided a deep understanding of the mechanism to suppress the“shuttle effect”by the LREHs,and a guide to design effective functional interlayers for high-performance Li-S batteries with excellent electrocatalytic activity.

关键词： Lithium-sulfur batteries Functional separator Layered rare-earth hydroxides Shuttle effect Adsorption Catalysis

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Synthesis and optical properties of highly efficient Na3KMg7（PO4）6:Eu2+ blue phosphor for full-spectrum white-light-emitting diodes:The role of Li2CO3 flux

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Journal of rare earths 2024年第7期42卷 1217-1223页

作者： Zihao Wang Sisi Liang Chenyang Zhan Kunyuan Xu Jie Hu Dejian Chen Liping Song Haomiao Zhu School of Physics and materials Science Nanchang University Ganjiang Innovation Academy Chinese Academy of Sciences CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of Sciences xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Research Center of Rare Earth MaterialsHaixi InstituteChinese Academy of Sciences

Full-spectrum phosphor-converted white-light-emitting diodes（pc-WLED） are emerging as a mainstream technology in semiconductor lighting.Nevertheless,high-performance blue phosphor which can be excited efficiently by a 400 nm NUV diode chip is still lacking.Herein,we present a blue-emitting Na3KMg7（PO4）6:Eu2+phosphor synthesized by the solid-reaction method.Particularly,we find that the using of Li2CO3as flux can significantly improve the crystal quality and thus the emission efficiency of the phosphor.Meanwhile,the excitation peak of the phosphor shifts from 365 to 400 nm,which is pivotal for efficient NUV（400 nm） diode chip excitation.The practical Eu2+concentration is also enhanced by using Li2CO3as flux,and the absorption efficiency is greatly increased.This phosphor exhibits superior PL the rmal stability,na mely retains 94% integrated photoluminescence intensity at 150℃of that at 25℃.As a result,the optimized phosphor shows an emission band peaked at 437 nm with a bandwidth of 40 nm and a high external photoluminescence quantum yield of 51.7%.Finally,a pc-WLED was fabricated by using NKMPO:Eu2+blue,Sr2SiO4:Eu2+green,CaAlSiN3:Eu2+red phosphors,and a400 nm NUV diode chip.It shows a high color rendering index of Ra=96.4 and a correlated color temperature of 4358 K.These results prove that NKMPO:Eu2+is a promising blue phosphor for fullspectrum WLED based on NUV diode chips.

关键词： Blue phosphor Eu2+ Full-spectrum white LEDs Na3KMg7(PO4)6 rare earths

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Investigation of Ce/BEA as a passive NOx adsorber:1.The occurrences of cerium and adsorption behavior

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Journal of rare earths 2024年第7期42卷 1265-1271页

作者： Minghui Yu Yiying Ding Xiaojie Yu Siwei Yan Meiqing Shen Jianqiang Wang Jun Wang Gurong Shen School of materials Science and Engineering Tianjin University School of Chemical Engineering and Technology Tianjin University National rare earth Catalysis Research institute

Ce/BEA has great potential as a passive NOxabsorber（PNA） to reduce the NOxemissions during the cold start phase especially in diesel engine for its high resistance to CO and suitable NOxdesorption temperature range.However,as a novel material,its physical and chemical properties still remain unknown.In this work,Ce/BEA was synthesized by ion-exchange method to identify the active species in NOxadsorption,compared with aggregated Ce species in Ce/SiAlOxprepared by impregnation method.X-ray diffraction（XRD）,high resolution-transmission electron microscopy（HR-TEM） and aberration-correctedscanning transmission electron microscopy（AC-STEM） were performed to confirm the isolated single atom formation of Ce species in Ce/BEA.UV-vis diffraction reflection spectra（DRS） and X-ray photoelectron spectroscopy（XPS） were conducted to find the difference of chemical environment between the isolated Ce species and aggregated ones.PNA performance evaluation and temperature programmed reduction of hydrogen（H2-TPR） results show the high NOxstorage capacity and active oxygen species quantity in Ce/BEA.It is also found that the main NOxadsorption species are Ce4+-O*rather than Ce3+.NOx-diffuse reflectance infrared Fourier transform spectroscopy（NOx-DRIFTS） confirms that the bidentate nitrite species are the critical NOxadsorption intermediates and the conception of NOxadsorption and desorption processes is proposed.

关键词： Ce/BEA Isolated Ce species Passive NOx absorber rare earths

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Effect of phase transition during roasting of Mountain Pass rare earth concentrate on leaching efficiency of rare earths

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Journal of rare earths 2024年第2期42卷 409-414,I0006页

作者： Yanyan Zhao Xu Sun Deliang Meng Xiangsheng Liu Qiang Zhong Zongyu Feng National Engineering Research Center for rare earth Grirem Advanced Materials Co.Ltd.Beijing0088China rare earth Functional materials(Xiong'an)Innovation Center Co. Ltd.Xiongan071700China General Research institute for Nonferrous Metals Beijing100088China

To find a greener and more economical approach for treating the Mountain Pass rare earth concentrate(MPREC),a novel "Combination Method",including the processes of oxidizing roasting,HCI leaching and sulfuric acid roasting,is proposed in this research.In this paper,the effect of phase transition behavior in hydrochloric acid leaching during oxidative roasting at 450-600℃ was studied.During roasting,the bastnasite in MPREC is decomposed into CeLa_(2)O_(3)F_(3) and(Ce_(0.33),La_(0.33),Ca_(0.33))O_(1.5).As the CeLa_(2)O_(3)F_(3) phase has the fluorine-fixation effect,the generated CeLa_(2)O_(3)F_(3) phase can not be dissolved by HCI after roasting at 500 and 550℃,but it can be decomposed by HCI after roasting at over 600℃,resulting in the improvement of the leaching rate of total F element.The maximum leaching efficiency of rare earth elements(REEs) can reach 70.32 wt% at the roasting temperature of 550℃.After roasting at over 600℃,some F^-ions in the solution combined with RE^(3+) to form REF_(3) precipitate and enter the leaching residue,and the others are in the form of [CeF_(3)]^+ in the leaching solution during leaching,therefore,the leaching efficiency of non-ce rium REEs decreases while that of cerium element increases.This work provides basic research for optimizing the actual production process of MPREC.

关键词： Mountain pass rare earth mine Roasting Phase change rare earths

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