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Understanding the sluggish and highly variable transport kinetics of lithium ions in LiFePO_4

Science China Chemistry 2023年第11期66卷 3297-3306页

作者： Youcheng Hu Xiaoxiao Wang Peng Li Junxiang Chen Shengli Chen Hubei Electrochemical Power Sources Key Laboratory Department of ChemistryWuhan UniversityWuhan 430072China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

LiFePO_(4),one of the mainstream cathode materials of current EV batteries,exhibits experimental diffusion coefficients(D_(c))of Li^(+)which are not only several orders of magnitude lower than those predicted by the ionic hopping barriers obtained from theoretical calculations and spectroscopic measurements,but also span several orders from 10^(-14)to 10^(-18)cm^(2)s^(-1)under different states of charge(SOC)and the charging rates(C-rates).Atomic level understanding of such sluggishness and diversity of Li^(+)transport kinetics would be of significance in improving the rate performance of LiFePO_(4)through material and operation optimization but remain ***,we show that the high sensitivity of Li^(+)hopping barriers on the local Li–Li coordination environments(numbers and configurations)plays a key role in the ion transport *** is due a neural network-based deep potential(DP)which allows accurate and efficient calculation of hopping barriers of Li^(+)in LiFePO_(4)with various Li–Li coordination environments,with which the kinetic Monte-Carlo(KMC)method was employed to determine the D_(c)values at various C-rates and SOC across a broad ***,an accelerated KMC simulation strategy is proposed to obtain the D_(c)values under a wide range of SOC at low C-rates,which agree well with that obtained from the galvanostatic intermittent titration technique(GITT).The present study provides accurate descriptions of Li^(+)transport kinetics at both very high and low C-rates,which remains challenging to experiments and first-principles calculations,***,it is revealed that the gradient distributions of Li^(+)density along the diffusion path result in great asymmetry in the barriers of the forward and backward hopping,causing very slow diffusion of Li^(+)and the diverse variation of D_(c).

关键词： lithium iron phosphate diffusion coefficient machine-learning potential kinetic Monte Carlo simulations

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Efficient synthesis of nano high-entropy compounds for advanced oxygen evolution reaction

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Chinese Chemical Letters 2025年第4期36卷 216-220页

作者： Genxiang Wang Linfeng Fan Peng Wang Junfeng Wang Fen Qiao Zhenhai Wen School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Materials and Techniques Toward Hydrogen EnergyFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Developing efficient electrocatalysts for oxygen evolution reaction(OER)is imperative to enhance the overall efficiency of electrolysis systems and rechargeable metal-air batteries operating in aqueous ***-entropy materials,featured with their distinctive multi-component properties,have found extensive application as catalysts in electrochemical energy storage and conversion ***,synthesizing nanostructured high-entropy compounds under mild conditions poses a significant challenge due to the difficulty in overcoming the immiscibility of multiple metallic *** this context,the current study focuses on the synthesis of an array of nano-sized high entropy sulfides tailored for OER via a facile precursor pyrolysis method at low *** representative compound,Fe Co Ni Cu Mn Sx,demonstrates remarkable OER performance,achieving a current density of 10 m A/cm^(2) at an overpotential of merely 220 m V and excellent stability with constant electrolysis at 100 m A/cm^(2) for over 400 *** in-situ formed metal(oxy)hydroxide has been confirmed as the real active sites and its exceptional performance can be primarily attributed to the synergistic effects arising from its multiple ***,the synthetic methodology presented here is versatile and can be extended to the preparation of high entropy phosphides,which also present favorable OER *** research not only introduces promising non-noble electrocatalysts for OER but also offers a facile approach to expand the family of nano high-entropy materials,contributing significantly to the field of electrochemical energy conversion.

关键词： High-entropy sulfides High-entropy phosphides Oxygen evolution reaction Efficient synthesis Nano structure

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Engineered high-density carbon defects enable accelerated sulfur conversion for kinetics-boosted room-temperature sodium-sulfur batteries

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Journal of Energy Chemistry 2025年第5期104卷 442-451页

作者： Kejian Tang Yingxinjie Wang Xiangqi Peng Ziying Zhang Guohao Li Jie Wang Chi Chen Zhenjun Wu Xiuqiang Xie College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082HunanChina College of Materials Science and Engineering Hunan UniversityChangsha 410082HunanChina CAS Key Laboratory of Design and Assembly of Functional Nanostructures &Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina

The practical application of room-temperature sodium-sulfur(RT Na-S)batteries is hindered by sluggish reaction kinetics and deleterious side *** address these challenges,a defective carbon is designed as a sulfur host through a simple temperature-controlled *** abundant porosity and surface roughness enhance sulfur encapsulation and mitigate side ***,highly disordered structure facilitates the chemical adsorption towards NaPSs and accelerates sulfur ***,electrochemical characterizations reveal that concentration polarization during the formation of long-chain NaPSs emerges as the key polarization and activation polarization dominates the nucleation of Na_(2)S during discharge,while they both significantly affect the formation of S_(8)/long-chain NaPSs during *** to the improved adsorption capability and electrocalatytic sites,S/CZ-900presents lower concentration polarization and activation polarization during both discharge and ***,S/CZ-900 cathode achieves 1031,914,and 671 mAh g^(-1)at 1,2,and 5 *** cathode with a high sulfur loading of 6.4 mg cm^(-2)delivers an impressive areal capacity of 14.3 mAh cm^(-2).Moreover,the S/CZ-900||Na/CZ-900(Al)full cell exhibits robust cycling stability,maintaining 1094 mAh g^(-1)after 40 cycles at 0.1 *** insights provide a workable solution of metal-free carbonaceous host materials for the evolution of RT Na-S batteries.

关键词： Metal-free carbonaceous sulfur host Highly disordered structure Porous and rough carbon RT Na-S batteries

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High-brightness near-infrared luminescent bioprobes based on lanthanide-doped Na3CrF6 nanoparticles

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Science China Materials 2024年第12期67卷 4113-4114页

作者： Yun Xing Shiqi Yu Datao Tu Xueyuan Chen State Key Laboratory of Structural Chemistry Fujian Key Laboratory of Nanomaterialsand CAS Key Laboratory of Design and Assembly of Functional NanostructuresFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China University of Chinese Academy of Sciences Beijing 100049China

Over the past decade,near-infrared(NIR)luminescent materials have emerged as a frontier in photonics and material science,finding diverse applications in bioimaging,encryption,and photodetection[1].Particularly,NIR nanoprobes are widely utilized in life science and clinical medicine because of their high spatial resolution,deep tissue penetration,low optical absorption and scattering,and minimal autofluorescence[2,3].

关键词： nanoparticles frontier utilized

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3D printing technology for rechargeable Li/Na-ion batteries

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Journal of Energy Chemistry 2025年第4期103卷 237-263页

作者： Ziting Chen Yihao Yang Songheng Xie Yangjie Liu Puwu Liang Xiang Hu Zhenhai Wen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen EnergyFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350000FujianChina College of Chemistry Fuzhou UniversityFuzhou 350108FujianChina

The rapid advancement of energy storage technologies highlights the urgent need for innovative electrochemical energy storage(EES)systems featuring complex ***-dimensional(3D)printing has emerged as a groundbreaking solution,enabling the fabrication of customized,high-performance electrodes with precise structural *** approach enhances accuracy,convenience,and facilitates improved ion and electron *** this review,we systematically summarize recent advancements in leveraging 3D printing techniques for lithium-ion and sodium-ion *** begin by comparing the unique capabilities of various 3D printing methods against traditional fabrication techniques for producing tailored *** then address critical challenges across different battery module architectures-cathodes,anodes,electrolytes,and integrated systems-highlighting breakthroughs in material selection,ink formulation,and ***,we explore the future potential of 3Dprinted batteries in next-generation EES devices,emphasizing their role in advancing customizable,high-efficiency *** insights provided herein illuminate how 3D printing can significantly accelerate the development of advanced battery materials,fostering innovation in energy storage technology.

关键词： 3D printing Li/Na-ion batteries Electrode Electrolyte Integrated batteries

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Boosting characteristic emissions of lanthanide in Cs_(2)Ag_(0.6)Na_(0.4)InCl_(6-x)Br_(x) double perovskites via mixing halide

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Journal of Rare Earths 2025年第1期43卷 39-46,I0002页

作者： Shujian Wang Dejian Chen Jie Hu Sisi Liang Kunyuan Xu Maochun Hong Haomiao Zhu University of Science and Technology of China Hefei230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou341000China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian 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 InstitutesChinese Academy of SciencesXiamen361021China

Lanthanide ions(Ln^(3+))doping provides a potential strategy to control over the luminescent properties of lead-free halide double perovskite nanocrystals(DP NCs).However,due to the low energy transfer efficiency between self-trapped exciton(STE)and Ln^(3+)ions,the characteristic emissions of Ln^(3+)ions are not ***,the energy transfer mechanism between STE and Ln^(3+)ions is also elusive and requires in-depth *** chose trace Bi^(3+)-doped Cs_(2)Ag_(0.6)Na_(0.4)InCl_(6-x)Br_(x) as a representative DP matrix to demonstrate that by tuning the bromide concentration,the Ln^(3+)emission can be greatly *** enhanced STE and Ln^(3+)ions energy transfer originates from the high covalency of Ln-Br bond,which contributes to improve ment of the characteristic emission of Ln^(3+)*** re,optical spectroscopy reveals that the energy transfer mechanism from DP to Eu^(3+)ions is different from all the other doped Ln^(3+)*** energy transfer from DP to Eu^(3+)ions is mostly through Eu-Br charge transfer while the other Ln^(3+)ions are excited by energy transfer from *** distinct energy transfer mechanism has resulted from the energy separation between the excited energy level of Ln^(3+)ions and the bottom of conduction band of *** increasing the energy separation,the energy transfer from STE to Ln^(3+)ions is less efficient because of the generation of a larger number of phonons and finally becomes impossible for Eu^(3+)*** results provide new insight into tuning the energy transfer of Ln^(3+)-doped DP NCs.

关键词： Double perovskitenanocrystal Lead free Lanthanideions Energytransfer Rare earths

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The marriage of perovskite nanocrystals with lanthanide-doped upconversion nanoparticles for advanced optoelectronic applications

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Aggregate 2024年第5期5卷 9-22页

作者： Wen Zhang Wei Zheng Ping Huang Dengfeng Yang Zhiqing Shao Xueyuan Chen Fujian Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistryand CAS Key Laboratory of Design and Assembly of Functional NanostructuresFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouChina Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China FuzhouChina University of Chinese Academy of Sciences BeijingChina

The exceptional optoelectronic properties of lead halide perovskite nanocrystals(PeNCs)in the ultraviolet and visible spectral regions have positioned them as a promising class of semiconductor materials for diverse optoelectronic and photo-voltaic ***,their limited response to near-infrared(NIR)light due to the intrinsic bandgap(>1.5 eV)has hindered their applications in many advanced *** circumvent this limitation,it is of fundamental significance to inte-grate PeNCs with lanthanide-doped upconversion nanoparticles(UCNPs)that are capable of efficiently converting low-energy NIR photons into high-energy ultravi-olet and visible *** leveraging the energy transfer from UCNPs to PeNCs,this synergistic combination can not only expand the NIR responsivity range of PeNCs but also introduce novel emission profiles to upconversion luminescence with multi-dimensional tunability(e.g.,wavelength,lifetime,and polarization)under low-to-medium power NIR irradiation,which breaks through the inherent restric-tions of individual PeNCs and UCNPs and thereby opens up new opportunities for materials and device *** this review,we focus on the latest advance-ments in the development of PeNCs-UCNPs nanocomposites,with an emphasis on the controlled synthesis and optical properties design for advanced optoelectronic applications such as full-spectrum solar cells,NIR photodetectors,and multilevel *** future efforts and prospects toward this active research field are also envisioned.

关键词： energy transfer heterostructure lanthanide luminescence perovskite nanocrystals upconversion nanoparticles

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Insight into bay-/end-substituted perylene diimide and its S-scheme heterojunction for enhanced photocatalytic H2O2 production under visible-light irradiation

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材料科学技术（英文版） 2025年第3期206卷 257-268页

作者： Bo Zhang Kang Li Renfu Li Shoufeng Wang Longtian Kang 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 Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China College of Chemistry Fuzhou UniversityFuzhou 350116China University Chinese Academy of Science Fujian CollegeFuzhou 350002China 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 Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China University Chinese Academy of Science Fujian CollegeFuzhou 350002China

Here,1D bis(N-carboxymethyl)peryleneimide(H2PDI),0D 1,6,7,12-tetrachloro-bis(N-carboxymethyl)peryleneimide(4Cl-H2PDI),and 2D 4Cl-H2PDI/graphene quantum dot(4Cl-H2PDI/GQD)nanostructures are synthesized and carefully *** effect of bay-/end-substitution and S-scheme heterojunction of PDI-based materials as main catalysts on the photocatalytic H2O2 evolution is first studied through the oxygen reduction reaction(ORR).Under the visible-light irradiation(＞420 nm),4Cl-H2PDI and 4Cl-H2PDI/GQD as photocatalysts exhibit the～7 and～16 times H2O2 evolution rate than H2PDI(1059.6 vs.2484.0 vs.160.0 μM g-1 h-1),*** systematical experiments reveal that 4C1-H2PDI and 4Cl-H2PDI/GQD should prefer a two-step single-electron ORR process,while H2PDI may involve a 4e-water oxidation and one-step 2e-ORR *** experiments confirm that the bay-substitution and GQD doping of H2PDI can promote the generation,transportation,and separation of photogenerated electrons and holes,and prolong the carrier *** work provides insight into PDI-based photocatalytic H2O2 production.

关键词： Photocatalysis Oxygen reduction reaction H2O2 evolution Perylenediimide S-scheme heterojunction

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Alternative lead-free mixed-valence double perovskites for high-efficiency photovoltaic applications

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Journal of Energy Chemistry 2023年第9期84卷 347-353页

作者： Wenbo Li Yuheng Li Zilong Zhang Peng Gao 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 350002FujianChina Laboratory for Advanced Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021FujianChina University of Chinese Academy of Sciences Beijing 100049China

Lead-based organic-inorganic hybrid perovskites have exhibited great potential in photovoltaics,achieving power conversion efficiencies(PCEs) exceeding 25%.However,the toxicity of lead and the instability of these materials under moist conditions pose significant barriers to large-scale *** overcome these limitations,researchers have proposed mixed-valence double perovskites,where Cs_(2)Au~ⅠAu~ⅢI_6 is a particularly effective absorber due to its suitable band gap and high absorptance *** further extend the scope of these lead-free materials,we varied the trivalent gold ion and halogen anion in Cs_(2)Au~ⅠAu~ⅢI_6,resulting in 18 new structures with unique ***,using first-principles calculations and elimination criteria,we identified four materials with ideal band gaps,small effective carrier mass,and strong anisotropic optical *** to theoretical modeling,Cs_(2)AuSbCl_6,Cs_(2)AuInCl_6,and Cs_(2)AuBiCl_6 are potential candidates for solar cell absorbers,with a spectroscopic limited maximum efficiency(SLME) of approximately 30% in a 0.25 μm-thick *** three compounds have not been previously reported,and therefore,our work provides new insights into potential materials for solar energy *** aim for this theoretical exploration of novel perovskites to guide future experiments and accelerate the development of high-performance photovoltaic devices.

关键词： Mixed valence double perovskite Theoretical calculation Electronic configuration Photovoltaic performance

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Influence of different Fe doping strategies on modulating active sites and oxygen reduction reaction performance of Fe, N-doped carbonaceous catalysts

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Journal of Energy Chemistry 2022年第7期31卷 511-520,I0013页

作者： Yang Liu Suqiong He Bing Huang Ziyan Kong Lunhui Guan CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina University of Chinese Academy of Sciences Beijing 100049China

Fe/N/C catalysts,synthesized through the pyrolysis of Fe-doped metal–organic framework (MOF) precursors,have attracted extensive attention owing to their promising oxygen reduction reaction (ORR) catalytic activity in fuel cells and/or metal-air ***,post-treatments (acid washing,second pyrolysis,and so on) are unavoidable to improve ORR catalytic activity and *** method for introducing Fe^(3+) sources (anhydrous Fe Cl_(3)) into the MOF structure,in particular,is a critical step that can avoid time-consuming post-treatments and result in more exposed Fe-N_(x) active ***,three different Fe doping strategies were systematically investigated to explore their influence on the types of active sites formed and ORR ***-NC(Zn^(2+)),synthesized by one-step pyrolysis of Fe doped ZIF-8 (Zn^(2+)) precursor which was obtained by adding the anhydrous Fe Cl_(3)source into the Zn(NO_(3))_(2)·6H_(2)O/methanol solution before mixing,possessed the highest Fe-N_(x)active sites due to the high-efficiency substitution of Zn^(2+)ions with Fe^(3+) ions during ZIF-8 growth,the strong interaction between Fe^(3+) ions and N atoms of 2-Methylimidazole (2-MIm),and ZIF-8’s micropore confinement *** a result,Fe-NC(Zn^(2+)) presented high ORR activity in the entire p H range (p H=1,7,and 13).At p H=13,Fe-NC(Zn^(2+)) exhibited a half-wave potential (E1/2) of 0.95 V (*** hydrogen electrode),which was 70 m V higher than that of commercial Pt/*** importantly,Fe-NC(Zn^(2+)) showed superior ORR stability in neutral media without performance loss after 5,000 cycles.A record-high open-circuit voltage(1.9 V) was obtained when Fe-NC(Zn^(2+)) was used as a cathodic catalyst in assembled Mg-air batteries in neutral *** assembled liquid and all-solid Mg-air batteries with high performance indicated that Fe-NC(Zn^(2+)) has enormous potential for use in flexible and wearable Mg-air batteries.

关键词： Mg-air battery Oxygen reduction reaction Single-atom Fe/N/C catalysts Fe doping strategies Zeolitic imidazole frameworks

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