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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 ***,this paper aims to address the issue by introducing MXene through a simple and scalable method for assembling graphene and realizing ultrahigh P doping *** 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 *** addition,N/P co-doping introduces abundant defects,providing more active sites for K^(+) storage and facilitating K^(+) *** 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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Grain growth behavior and properties of high-entropy pseudobrookite(Mg,Co,Ni,Zn)Ti_(2)O_(5) ceramics

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Journal of Advanced Ceramics 2024年第6期13卷 757-768页

作者： Xiaohui Ma Jinyu Wu Lingyi Meng Jinfeng Zhang Heng Chen Liwen Yan Anran Guo Jiachen Liu Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and EngineeringTianjin UniversityTianjin 300072China xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China

It is well known that the grain size of high-entropy ceramics is quite small owing to the sluggish diffusion effect. However, abnormal grain growth often occurs in high-entropy pseudobrookite ceramics, ultimately resulting in the formation of many abnormally grown grains with a grain size as large as 50 μm. To study this phenomenon, the grain growth behavior of high-entropy pseudobrookite ceramics was systematically investigated in this paper. The results demonstrate that the starting material powders first react with each other to form a high-entropy intermediate phase and calcined TiO_(2) powders (TiO_(2)-1100 ℃), and then as the sintering temperature increases, the formed high-entropy intermediate phase further reacts with TiO_(2)-1100 ℃ to form high-entropy pseudobrookite ceramics. Thus, in this system, in addition to the sluggish diffusion effect, the grain sizes of the high-entropy intermediate phase and TiO_(2)-1100 ℃ also affect the morphology of high-entropy pseudobrookite. Compared to nanosized TiO_(2), micron-sized TiO_(2) has a lower sintering activity. Therefore, the high-entropy intermediate phases (Mg,Co,Ni,Zn)TiO_(3) and TiO_(2)-1100 ℃ prepared with micron-sized starting materials exhibit lower grain sizes, finally resulting in the formation of high-entropy (Mg,Co,Ni,Zn)Ti_(2)O_(5) with small grain sizes. Moreover, nano-indentation and thermal conductivity tests were carried out on high-entropy (Mg,Co,Ni,Zn)Ti_(2)O_(5) with different morphologies. The results show that the hardness of high-entropy (Mg,Co,Ni,Zn)Ti_(2)O_(5) increases from 6.05 to 9.95 GPa as the grain size increases, whereas the thermal conductivity decreases from 2.091±0.006 to 1.583±0.006 W·m^(−1)·K^(−1). All these results indicate that high-entropy (Mg,Co,Ni,Zn)Ti_(2)O_(5) with a small grain size is a potential material for thermal protection.

关键词： grain size sluggish diffusion effect two-step solid phase process high-entropy intermediate phase high-entropy pseudobrookite ceramic

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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 *** 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 ***,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 *** material can be re peatedly excited by X-ray and emits similar lumine scence intensity every time,which shows good PersL *** 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 *** 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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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 *** 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 *** distortion is accomplished by introducing rare earth elements with different cation radii and *** 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 *** 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 *** 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 ***,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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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 ***,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 *** 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 *** 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,*** 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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Oxygen self-doping pyrolyzed polyacrylic acid as sulfur host with physical/chemical adsorption dual function for lithium-sulfur batteries

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Chinese Chemical Letters 2024年第7期35卷 473-479页

作者： Yan Wang Huixin Chen Fuda Yu Shanyue Wei Jinhui Song Qianfeng He Yiming Xie Miaoliang Huang Canzhong Lu Engineering Research Center of Environment-Friendly Functional materials Ministry of EducationInstitute of Materials Physical ChemistryHuaqiao UniversityXiamen 361021China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China

Lithium-sulfur(Li-S)batteries with high theoretical capacity and energy density need to solve problems such as the high decomposition energy barrier of Li_(2)S and large volume change of sulfur in the charging process caused by the shuttle effect before practical ***,a green synthesis method is used to prepare polyacrylic acid(PAA)superabsorbent material,and then the pyrolyzed PAA(P/PAA)material is obtained as the positive electrode of Li-S *** functional calculation reveals that the oxygen self-doping pyrolyzed polyacrylic acid(P/PAA)delivered stronger binding energy toward Li2S species in carbonyl C=O than that of graphite powder(GP)which are-1.58 eV and-1.02 eV,*** with the distribution of relaxation time analysis and the in-situ electrochemical impedance approach,it is further demonstrated that the designed P/PAA as sulfur host plays a physical/chemical adsorption dual function in maintaining the stability and rate performance of *** an initial discharge capacity of 1258 mAh/g at 0.1 C and a minimal capacity decline of 0.05%per cycle even after 800 cycles at 0.5 C,the produced cathode demonstrated outstanding electrochemical *** average Coulombic efficiency is nearly 100%.The P/PAA electrodes may typically retain 96%of their capacity while declining on average only 0.033%per cycle after 130 cycles at 3 *** effort provides a new method for the future development of heteroatomic self-doping superabsorbent with promising adsorption properties for polysulfides as cathode materials of Li-S batteries.

关键词： Polyacrylic acid Oxygen self-doping Green synthetic Pore mesh polymer cathodes Lithium-sulfur batteries

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Synthesis and optical properties of highly efficient Na_(3)KMg_(7)(PO_(4))_(6):Eu^(2+)blue phosphor for full-spectrum white-light-emitting diodes:The role of Li_(2)CO_(3)flux

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Journal of rare earths 2024年第7期42卷 1217-1223,I0001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 UniversityNanchang330000China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou341000China 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 SciencesFuzhou350002China xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Research Center of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen361021China

Full-spectrum phosphor-converted white-light-emitting diodes(pc-WLED)are emerging as a mainstream technology in semiconductor ***,high-performance blue phosphor which can be excited efficiently by a 400 nm NUV diode chip is still ***,we present a blue-emitting Na_(3)KMg_(7)(PO_(4))6:Eu^(2+)phosphor synthesized by the solid-reaction ***,we find that the using of Li_(2)CO_(3)as flux can significantly improve the crystal quality and thus the emission efficiency of the ***,the excitation peak of the phosphor shifts from 365 to 400 nm,which is pivotal for efficient NUV(400 nm)diode chip *** practical Eu^(2+)concentration is also enhanced by using Li_(2)CO_(3)as flux,and the absorption efficiency is greatly *** phosphor exhibits superior PL thermal stability,namely 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:Eu^(2+)blue,Sr_(2)SiO_(4):Eu^(2+)green,CaAlSiN_(3):Eu^(2+)red phosphors,and a 400 nm NUV diode *** shows a high color rendering index of R_(a)=96.4 and a correlated color temperature of 4358 *** results prove that NKMPO:Eu^(2+)is a promising blue phosphor for full-spectrum WLED based on NUV diode chips.

关键词： Eu^(2+) Blue phosphor Na_(3)KMg_(7)(PO_(4))_(6) Full-spectrum white LEDs rare earths

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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 ***,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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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 ***,we first propose the implementability of layered rare-earth hydroxides(LREHs)in Li-S batteries to optimize electrochemical *** 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 *** 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 *** 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 *** 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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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 *** the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction ***,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 *** 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 *** 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 *** 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 ***,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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