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Electrolyte design for Li-conductive solid-electrolyte interphase enabling benchmark performance for all-solid-state lithium-metal batteries

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Nano Research 2024年第11期17卷 9640-9650页

作者： Cailing Fan Niaz Ahmad Tinglu Song Chaoyuan Zeng Xiaoxiao Liang Qinxi Dong Wen Yang School of Chemistry and Chemical Engineering Key Laboratory of Ministry of Education for Advanced Materials in Tropical Island Resources Collaborative Innovation Center of Ecological Civilization Hainan University Haikou 570228 China Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing 100081 China Experimental Center of Advanced Materials School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 China

Sulfide-based solid-state electrolytes (SSEs) with high Li+ conductivity (δLi^(+)) and trifling grain boundaries have great potential for all-solid-state lithium-metal batteries (ASSLMBs). Nonetheless, the in-situ development of mixed ionic-electronic conducting solid-electrolyte interphase (SEI) at sulfide electrolyte/Li-metal anode interface induces uneven Li electrodeposition, which causes Li-dendrites and void formation, significantly severely deteriorating ASSLMBs. Herein, we propose a dual anionic, e.g., F and N, doping strategy to Li7P3S11, tuning its composition in conjunction with the chemistry of SEI. Therefore, novel Li_(6.58)P_(2.76)N_(0.03)S_(10.12)F_(0.05) glass-ceramic electrolyte (Li_(7)P_(3)S_(11-5)LiF-3Li_(3)N-gce) achieved superior ionic (4.33 mS·cm^(−1)) and lowest electronic conductivity of 4.33 × 10^(−10) S·cm^(−1) and thus, offered superior critical current density of 0.90 mA·cm^(−2) (2.5 times >Li7P3S11) at room temperature (RT). Notably, Li//Li cell with Li6.58P2.76N0.03S10.12F0.05-gce cycled stably over 1000 and 600 h at 0.2 and 0.3 mA·cm^(−2) credited to robust and highly conductive SEI (in-situ) enriched with LiF and Li3N species. Li3N’s wettability renders SEI to be highly Li+ conductive, ensures an intimate interfacial contact, blocks reductive reactions, prevents Li-dendrites and facilitates fast Li+ kinetics. Consequently, LiNi0.8Co0.15Al0.05O_(2) (NCA)/Li_(6.58)P_(2.76)N_(0.03)S_(10.12)F_(0.05)-gce/Li cell exhibited an outstanding first reversible capacity of 200.8/240.1 mAh·g^(−1) with 83.67% Coulombic efficiency, retained 85.11% of its original reversible capacity at 0.3 mA·cm^(−2) over 165 cycles at RT.

关键词： Li_(6.58)P_(2.76)N_(0.03)S_(10.12)F_(0.05)-glass-ceramic electrolyte(gce) low electronic conductivity highly Li+conductive solid-electrolyte interphase(SEI) Li-dendrites and void suppression all-solid-state Li-metal batteries

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Interfacial interactions of Cu/MnOOH enhance ammonia synthesis from electrochemical nitrate reduction

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Chinese Chemical Letters 2025年第2期36卷 423-427页

作者： Hong-Rui Li Xia Kang Rui Gao Miao-Miao Shi Bo Bi Ze-Yu Chen Jun-Min Yan Key Laboratory of Automobile Materials Ministry of EducationSchool of Materials Science and EngineeringJilin UniversityChangchun 130022China

In this work,an effective catalyst of Cu/MnOOH has been successfully constructed for electrochemical nitrate reduction reaction(e NO_(3)RR)for synthesis of ammonia(NH_(3))under ambient *** substrate of MnOOH plays an important role on the size and electronic structure of Cu nanoparticles,where Cu has the ultrafine size of 2.2 nm and positive shift of its valence states,which in turn causes the increased number of Cu active sites and enhanced intrinsic activity of every active *** a result,this catalyst realizes an excellent catalytic performance on eNO_(3)RR with the maximal NH_(3)Faraday efficiency(FE)(96.8%)and the highest yield rate(55.51 mg h^(-1)cm^(-2))at a large NH_(3)partial current density of700 m A/cm^(2),which could help to promote the industrialization of NH_(3)production under ambient conditions.

关键词： Ammonia Nitrate reduction reaction Adsorption Electrocatalysis Interfacial interactions

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Multi-wavelength plasmonic optoelectronic memristor for reconfigurable logic operations and mixed-color pattern recognition

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science China(Information sciences) 2025年第2期68卷 5-14页

作者： Jiaqi HAN Zhuangzhuang LI Tao ZENG Xuanyu SHAN Riya SU Ya LIN Zhongqiang WANG Xiaoning ZHAO Shencheng FU Haiyang XU Yichun LIU Key Laboratory for UV Light-Emitting Materials and Technology (Northeast Normal University) Ministry of Education Department of Materials Science and Engineering National University of Singapore

Optoelectronic memristors have emerged as promising hardware platforms for highly efficient image perception owing to their low crosstalk, fast response, and low power consumption. However, the development of optoelectronic memristors with multi-wavelength recognition capabilities remains constrained by the limitations of their inherent bandgap. In this work, a multi-wavelength-modulated optoelectronic memristor that operates based on the localized surface plasmon resonance effect is developed using silver（Ag）-titanium dioxide（TiO2）/polymethyl methacrylate（PMMA） nanocomposites. The SET voltage can be gradually reduced by modulating the optical wavelength of visible irradiation. On this basis, reconfigurable IMP and False logic operations have been implemented in the memristive logic circuit. The neuromorphic visual preprocessing and recognition function for mixed-color patterns is demonstrated based on wavelength-dependent resistive switching behaviors. The proposed optoelectronic memristor enables high-density storage and in-memory computing.

关键词： optoelectronic memristor localized surface plasmon resonance multi-wavelength resistive switching color pattern recognition

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Carbon Energy 2025年第2期7卷 121-130页

作者： Tianyi Xu Dongxu Jiao Jinchang Fan Yilong Dong Zhaoyong Jin Lei Zhang Wei Zhang Jingxiang Zhao Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and Control Key Laboratory of Automobile MaterialsMinistry of EducationSchool of Materials Science and EngineeringJilin UniversityChangchunChina College of Chemistry Jilin UniversityChangchunChina Key Laboratory of Photonic and Electronic Bandgap Materials Ministry of EducationCollege of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbinChina

Strain effects have garnered significant attention in catalytic applications due to their ability to modulate the electronic structure and surface adsorption properties of *** this study,we propose a novel approach called“similar stacking”for stress modulation,achieved through the loading of Co_(2)P on Ni_(2)P(Ni_(2)P/Co_(2)P).Theoretical simulations reveal that the compressive strain induced by Co_(2)P influences orbital overlap and electron transfer with hydrogen ***,the number of stacked layers can be adjusted by varying the precursor soaking time,which further modulates the strain range and hydrogen *** a 2-h soaking condition,the strain effect proves favorable for efficient hydrogen *** characterizations using X-ray diffraction,high-angel annular dark-field scanning transmission election microscope(HAADF-STEM),and X-ray absorption near-edge structure spectroscopy successfully demonstrate lattice contraction of Co_(2)P and bond length shortening of ***,our catalyst shows an ultrahigh current density of 1 A cm^(-2) at an overpotential of only 388 mV,surpassing that of commercial Pt/C,while maintaining long-term *** material design strategy of similar stacking opens up new avenues of strain modulation and the deeper development of electrocatalysts.

关键词： compressive strain heterogeneous phosphide hydrogen evolution reaction similar stacking

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Designing interstitial boron-doped tunnel-type vanadium dioxide cathode for enhancing zinc ion storage capability

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Carbon Energy 2023年第8期5卷 78-86页

作者： Shiwen Wang Hang Zhang Kang Zhao Wenqing Liu Nairui Luo Jianan Zhao Shide Wu Junwei Ding Shaoming Fang Fangyi Cheng Henan Provincial Key Laboratory of Surface&Interface Science College of Materials and Chemical EngineeringZhengzhou University of Light IndustryZhengzhouChina Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjinChina

Chemical doping is a powerful method to intrinsically tailor the electrochemical properties of electrode ***,an interstitial boron-doped tunnel-type VO_(2)(B)is constructed via a facile hydrothermal *** analysis techniques demonstrate that boron resides in the interstitial site of VO_(2)(B)and such interstitial doping can boost the zinc storage kinetics and structural stability of VO_(2)(B)cathode during ***,we found that the boron doping level has a saturation limit peculiarity as proved by the quantitative ***,the 2 at.%boron-doped VO_(2)(B)shows enhanced zinc ion storage performance with a high storage capacity of 281.7 mAh g^(-1) at 0.1 A g^(-1),excellent rate performance of 142.2 mAh g^(-1) at 20 A g^(-1),and long cycle stability up to 1000 cycles with the capacity retention of 133.3 mAh g^(-1) at 5 A g^(-1).Additionally,the successful preparation of the boron-doped tunneltype α-MnO_(2) further indicates that the interstitial boron doping approach is a general strategy,which supplies a new chance to design other types of functional electrode materials for multivalence batteries.

关键词： cathode interstitial boron doping tunnel-type VO_(2)(B) zinc ion battery

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Design and Synthesis of Bis-β-ketoimine Binuclear Titanium Complex Isomers to Probe Bimetallic Synergistic Effect for Ethylene Polymerization

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Chinese Journal of Polymer science 2025年第5期43卷 756-768页

作者： Ming Zhou Meng-Yuan Xue Ping-Zhou Huang Ting-Cheng Li Qing-Liang You Guang-Yong Xie Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education&Hubei Key Laboratory of Catalysis and Materials Science South-Central Minzu UniversityWuhan430074China Key Laboratory of Optoelectronic Chemical Materials and Devices Ministry of EducationSchool of Chemical and Environmental EngineeringJianghan UniversityWuhan430056China

Binuclear complexes have attracted extensive attention in fields such as catalysis because of their likely bimetallic synergistic effect;however,the mechanism and factors influencing this synergism remain *** this work,six bis-β-ketoimine binuclear titanium complexes4a-4f containing different alkylthio sidearms and configurations were synthesized and characterized by nuclear magnetic resonance hydrogen spectrum(~1H-NMR),nuclear magnetic resonance carbon spectrum(^(13)C-NMR),Fourier transform infrared spectrum(FTIR),and elemental *** intermetallic distances of isomeric complexes 4a,4d,4e and 4f determined through density functional theory(DFT)optimization were in the order 4a<4d<4e<4f and were found to significantly influence the catalytic performance for ethylene(co)*** complexes could efficiently catalyze ethylene polymerization and ethylene/1-hexene or ethylene/1-octene copolymerization with high activity to produce highmolecular-weight ethylene homo-and *** the three binuclear titanium complexes 4a-4c with similar structures but different lengths of alkylthio sidearms,complex 4a,which contained the shortest methylthio sidearm,exhibited the highest activity for ethylene polymerization and copolymerization with 1-hexene or ***,for ethylene/1-hexene or ethylene/1-octene copolymerization,it showed the highest comonomer incorporation compared with propylthio(4b)and octylthio(4c)derivatives because of the smaller steric hindrance of the methyl group in 4a and the more open coordination space for vinyl ***,among the isomeric complexes 4a,4d,4e and4f,complex 4a with the shortest bimetallic distance also exhibited the highest activity towards ethylene(co)polymerization,and the highest 1-hexene or 1-octene incorporation in comparison with its regioisomeric counterparts 4d,4e and p-phenyl-bridged analog 4f,owing to a more appropriate bimetallic distance that is conducive to a synergistic effec

关键词： Binuclear titanium complex Isomer Ethylene polymerization Copolymerization Synergistic effect

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Electrosynthesis of H_(2)O_(2)via two-electron oxygen reduction over carbon-based catalysts:From microenvironment control to electrode/reactor design

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Energy Reviews 2024年第2期3卷 117-135页

作者： Jingjing Jia Zhenxin Li Yunrui Tian Xia Li Rui Chen Jiachen Liu Ji Liang Key Laboratory of Advanced Ceramics and Machining Technology Ministry of EducationSchool of Materials Science and EngineeringTianjin UniversityTianjinChina

The electrochemical production of hydrogen peroxide(H_(2)O_(2))by the two-electron oxygen reduction(2e^(-)-ORR)process has the advantages of high safety,low energy consumption,and environmental *** 2e^(-)-ORR,the catalyst/electrode is the key component as it strongly affects catalytic performance and *** materials have the advantages of high electronic conductivity,good structural stability,easy control of nanostructures,and low ***,it has been regarded as a promising catalyst/electrode material for the electrosynthesis of H_(2)O_(2)via 2e^(-)-*** addition,studies have also considered the optimization of the liquid/gas interface by tuning the electrode surface,electrolyte pH,and reactor configurations for further improving the activity and selectivity of *** this review,we provide an in-depth discussion of the recent research on the carbon-based electrocatalysts for 2e^(-)ORR,especially in terms of microenvironment tuning,catalyst/electrode interface engineering,and reactor design for achieving stable and efficient production of H_(2)O_(2).The challenges that we are still facing and the future development prospects will then be concluded,which we believe should help the future development in this field.

关键词： Oxygen reduction Hydrogen peroxide Carbon-based catalyst Electrode surface Reactor design

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Incommensurate modulated structure and its influence on the martensitic transformation temperature span of single phase multielement Ni-Cu-Co-Mn-Ga two-way shape memory single crystals

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材料科学技术（英文版） 2025年第5期208卷 230-240页

作者： Qijjia Yu Yang Liu Chen Si Wenjia Wang Jiaxi Meng Jingmin Wang Jinghua Liu Chengbao Jiang Key Laboratory of Advanced Aerospace Materials and Performance(Ministry of Education) School of Materials Science and EngineeringBeihang UniversityBeijing 100191PR China Center of Microstructure Science Frontier Institute of Science and TechnologyState Key Laboratory for Mechanical Behavior of MaterialsXi'an Jiaotong UniversityXi'an 710049PR China

Significant two-way shape memory effect(TWSME)was achieved in single crystals of single-phase mul-tielement Ni42-xCu8CoxMn37Ga13(8 ≤ x ≤ 12)alloys by performing thermomechanical ***,anomalous dependence of the martensitic transformation temperature span on Co content was *** training,quite a narrow temperature span of the martensitic transformation,nearly independent of the Co content,was observed in all single *** training the temperature span was still narrow for 8 ≤ x ≤ 10.9 but was obviously expanded for 10.9＜x ≤ ***-resolution transmission electron microscopy revealed that at the atomic scale,there exists incommensurate modulated structure in the single phase single crystals,as evidenced by nonperiodic satellite spots in the selected area electronic diffraction ***,the modulated wave vector of the satellite spots was increased by higher Co *** first principal calculations it was considered that the incommensurate modulated structure originates from the formation of Co-Co *** training arrays of ordered dislocations with the same Burgers vector were introduced for 8 ≤ x ≤ 10.9 but the network of dislocations was formed for 10.9＜x ≤ *** on analysis of transmission electron microscopy,geometric phase,thermody-namics,and Landau theory,it was considered that the austenite/martensite phase interface was pinned by the network of dislocations,expanding the temperature span of the martensitic *** work supplies new insights for understanding the microstructure and martensitic transformation of Ni-Mn-Ga-based alloys.

关键词： Martensitic transformation Incommensurate modulated structure Temperature span Dislocation Two-way shape memory effect

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Preparation of squeezed light with low average photon number based on dynamic Casimir effect

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Chinese Physics B 2023年第12期32卷 212-220页

作者：李娜林资鉴韦梅松廖明杰许静平柯三黄羊亚平 Key Laboratory of Advanced Micro-Structured Materials of Ministry of Education School of Physics Science and EngineeringTongji UniversityShanghai 200092China

It is well known that squeezed states can be produced by nonlinear optical processes,such as parametric amplification and four wave mixing,in which two photons are created or annihilated *** the Hamiltonian of the dynamic Casimir effect contains a~2 and a~(+2),photons in such a process are also generated or annihilated in *** we propose to get squeezed light through the dynamic Casimir ***,we demonstrate it from the full quantum perspective and the semiclassical perspective *** from previous work,we focus on generating squeezed states with the lowest average photon number,because such squeezed states have better quantum *** the full quantum picture,that is,phonons also have quantum properties,when the system is initially in the excited state of phonons,squeezed light cannot be generated during the evolution,but the light field can collapse to the squeezed state by measuring the state of *** the phonon is treated as a classical quantity,that is,the cavity wall is continuously driven,squeezed light with the minimum average photon number will be generated in the case of *** will play a positive role in better regulating the photon state generated by the dynamic Casimir system in the future.

关键词： cavity quantum electrodynamics quantum optics squeezed light

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Redox Couple Modulation in NASICON Phosphates toward High-Performance Cathodes for Na-Ion Batteries

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Energy Material Advances 2024年第1期5卷 570-586页

作者： Dashan Fan Qiuyu Shen Han Li Xuanhui Qu Lifang Jiao Yongchang Liu Beijing Advanced Innovation Center for Materials Genome Engineering Institute for Advanced Materials and TechnologyState Key Laboratory for Advanced Metals and MaterialsUniversity of Science and Technology BeijingBeijing 100083China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

Natrium superionic conductor(NASICON)-type phosphates have aroused a great interest as cathode materials for sodium-ion batteries(SIBs)by virtue of their stable 3-dimensional frameworks,flexible molecular formula tunability,and superior ionic ***,the intrinsic low electronic conductivity and relatively low theoretical specific capacity place obstacles in their way toward achieving higher electrochemical *** addition,only 2-electron reactions in most NASICON cathodes and poor reversibility of high-voltage redox couples severely limit their energy *** address the above tough issues,an in-depth understanding of transition metal selection,elements ratio optimization,and Na-storage mechanism is of paramount ***,this mini review summarizes the latest progresses on the NASICON-type phosphate cathodes for SIBs from the perspective of redox couple *** cathodes featuring high operating voltage and multielectron reactions are discussed in ***,the remaining challenges and personal outlooks based on redox couple regulation are put forward,shedding light on the designing rules for high-energy and long-durability NASICON-type phosphate cathodes for SIBs in the future.

关键词： theoretical specific capacity ionic conductivityneverthelessthe cathode materials electronic conductivity high performance cathodes redox couple modulation sodium ion batteries electrochemical performance

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