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Probing the fine structures of low atomic number catalysts by using electron energy loss spectroscopy

Particuology 2025年第3期98卷 154-171页

作者： Junnan Chen Ming Lu Qinhua Gu Bingsen Zhang Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang110016China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang110016China The Joint Laboratory of MXene Materials Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of EducationJilin Normal UniversityChangchun130103China

Low atomic number catalysts have gained widespread application in areas such as environmental management,catalytic reactions,and energy transformation,thanks to their cost-effectiveness and superior chemical *** in-depth exploration of the intricate structures of these catalysts,establishing their structure-activity relationships,and revealing their catalysis mechanisms are fundamental for developing novel and efficient *** energy loss spectroscopy(EELS),a pivotal electron microscopy technique,uniquely excels in dissecting the fine structures of low atomic number catalysts,since its high spatial resolution and acute sensitivity to elements with low atomic *** review summarizes the role of EELS in probing the fine structures of low-Z catalysts,encompassing the technological underpinnings,advantages,and specific use cases in catalyst *** can pinpoint the location,chemical surroundings,and electronic attributes of low-Z elements in catalysts,thus offering crucial insights for demystifying catalytic mechanisms and formulating innovative ***,this review delves into the potential advancements of EELS technology in the detailed structural study of low atomic number catalysts,hinting at a promising future for this research field.

关键词： Electron energy-loss spectroscopy Spectroscopic analysis Nanocarbon Transitional metal oxides

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engineering of geometrical configurations in dual-atom catalysts for electrocatalytic applications

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Journal of Energy Chemistry 2024年第7期94卷 273-287页

作者： Tao Zhang Yifan Liu Liang Xue Jingwen Sun Pan Xiong Junwu Zhu Key Laboratory for Soft Chemistry and Functional Materials of Ministry Education School of Chemistry and Chemical EngineeringNanjing University of Science and TechnologyNanjing210094JiangsuChina

Geometrical configurations play a crucial role in dual-atom catalysts(DACs)for electrocatalytic *** progress has been made to design DACs electrocatalysts with various geometri-cal configurations,but in-depth understanding the relationship between geometrical configurations and metal-metal interaction mechanisms for designing targeted DACs is still *** this review,the recent progress in engineering of geometrical configurations of DACs is systematically *** on the polarity of geometrical configuration,DACs can be classified into two different types that are homonuclear and heteronuclear ***,with regard to the geometrical configurations of the active sites,homonuclear DACs are identified into adjacent and bridged configurations,and heteronuclear DACs can be classified into adjacent,bridged,and separated ***,metal-metal interactions in DACs with different geometrical configurations are ***,the applications of DACs in different electrocatalytic reactions are discussed,including the oxygen reduction reaction(ORR),oxygen evolution reaction(OER),hydrogen evolution reaction(HER),and other ***,the future challenges and perspectives for advancements in DACs are *** review aims to provide inspiration for the design of highly effcient DACs towards energy relatedapplications.

关键词： Dual-atom catalysts Geometrical configurations Homonuclear Heteronuclear Electrocatalysis

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Modulating p-d orbital hybridization by CuO/Cu nanoparticles enables carbon nanofibers high cycling stability as anode for sodium storage

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Rare Metals 2023年第12期42卷 4039-4047页

作者： Zhi-Jia Zhang He-Yi Sun Yue-Fang Chen Yu-Wen Zhao Meng-Meng Zhang Chun-Sheng Li Yan Sun Zhong-Hui Gao Hui-Jun Li Yong Jiang School of Materials Science and Engineering Institute of Quantum Materials and DevicesState Key Laboratory of Separation Membrane and Membrane ProcessesTiangong UniversityTianjin 300387China School of Chemistry and Life Sciences School of Materials Science&Engineeringthe Key Laboratory of Advanced Ceramics and Machining Technology by the Ministry of Education of ChinaSuzhou University of Science and TechnologySuzhou 215009China School of Materials Science&Engineering The Key Laboratory of Advanced Ceramics and Machining Technology By the Ministry of Education of ChinaTianjin UniversityTianjin 300072China Faculty of Engineering and Information Sciences University of WollongongWollongongNSW 2522Australia

Carbon nanofibers(CNFs)have been extensively studied as anode materials for sodium-ion batteries due to their high conductivity,large aspect ratio and good electrochemical *** low specific capacity and low first cycle efficiency of CNFs,however,have hindered its practical ***,we present a facile strategy to synthesize a novel CNFs decorated with Cu/CuO nanoparticles(Cu-CNFs)using magnetron sputtering ***/CuO nanoparticles were uniformly distributed on the surface of *** to the density functional theory(DFT)calculation,Cu/CuO nanoparticles d-orbitals and CNFs p-orbitals present hybridization states,and the Na~+adsorption energy of the modified CNFs decreases from-2.14 to-2.97 *** Cu-CNFs composites exhibit excellent sodium storage properties,presenting a desirable initial Coulombic efficiency of 76%and a high specific reversible capacity of 300 mAh·g^(-1)at 0.1 A·g^(-1)after 400 ***-CNFs anode has excellent cycling stability under high current density,maintaining a high capacity of 150 mAh·g^(-1)at 1 A·g^(-1)after 6000 *** magnetron sputtering to regulate the electronic structure provides a new thought for improving the electrochemical performance of carbon materials.

关键词： Carbon nanofibers Cu/CuO nanoparticles Orbital hybridization Magnetron sputtering Density functional theory calculation

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Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature

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Nano Research 2024年第11期17卷 9651-9661页

作者： Jieshuangyang Chen Jie Lei Jinwei Zhou Xuanfeng Chen Rongyu Deng Mingzhi Qian Ya Chen Feixiang Wu School of Metallurgy and Environment Engineering Research Center of the Ministry of Education for Advanced Battery Materials Hunan Provincial Key Laboratory of Nonferrous Value-added Metallurgy Central South University Changsha 410083 China College of Materials Science and Engineering Institute of New Energy Materials and Engineering Fuzhou University Fuzhou 350108 China

The development of electrocatalysts with high catalytic activity is conducive to enhancing polysulfides adsorption and reducing activation energy of polysulfides conversion, which can effectively reduce polysulfide shuttling in Li-S batteries. Herein, a novel catalyst NiCo-MoO_(x)/rGO (rGO = reduced graphene oxides) with ultra-nanometer scale and high dispersity is derived from the Anderson-type polyoxometalate precursors, which are electrostatically assembled on the multilayer rGO. The catalyst material possesses dual active sites, in which Ni-doped MoO_(x) exhibits strong polysulfide anchoring ability, while Co-doped MoO_(x) facilitates the polysulfides conversion reaction kinetics, thus breaking the Sabatier effect in the conventional electrocatalytic process. In addition, the prepared NiCo-MoO_(x)/rGO modified PP separator (NiCo-MoO_(x)/rGO@PP) can serve as a physical barrier to further inhibit the polysulfide shuttling effect and realize the rapid Li+ migration. The results demonstrate that Li-S coin cell with NiCo-MoO_(x)/rGO@PP separator shows excellent cycling performance with the discharge capacity of 680 mAh·g^(−1) after 600 cycles at 1 C and the capacity fading of 0.064% per cycle. The rate performance is also impressive with the remained capacity of 640 mAh·g^(−1) after 200 cycles even at 4 C. When the sulfur loading is 4.0 mg·cm^(−2) and electrolyte volume/sulfur mass ratio (E/S) ratio is 6.0 μL·mg^(−1), a specific capacity of 830 mAh·g^(−1) is achieved after 200 cycles with a capacity decay of 0.049% per cycle. More importantly, the cell with NiCo-MoO_(x)/rGO@PP separator exhibits cycling performance under wide operating temperature with the reversible capacities of 518, 715, and 915 mAh·g^(−1) after 100 cycles at −20, 0, and 60 °C, respectively. This study provides a new design approach of highly efficient catalysts for sulfur conversion reaction in Li-S batteries.

关键词： lithium-sulfur batteries doped molybdenum oxide separator modification adsorption and catalysis dual-sites wide temperature

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Fluorine-Modulated MXene-Derived Catalysts for Multiphase Sulfur Conversion in Lithium-Sulfur Battery

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Nano-Micro Letters 2024年第12期16卷 201-216页

作者： Qinhua Gu Yiqi Cao Junnan Chen Yujie Qi Zhaofeng Zhai Ming Lu Nan Huang Bingsen Zhang Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016People’s Republic of China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016People’s Republic of China The Joint Laboratory of MXene Materials Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of EducationKey Laboratory of Preparation and Application of Environmental Friendly Materials of the Ministry of EducationJilin Normal UniversityChangchun 130103People’s Republic of China

Fluorine owing to its inherently high electronegativity exhibits charge delocalization and ion dissociation capabilities;as a result,there has been an influx of research studies focused on the utilization of fluorides to optimize solid electrolyte interfaces and provide dynamic protection of electrodes to regulate the reaction and function performance of ***,the shuttle effect and the sluggish redox reaction kinetics emphasize the potential bottlenecks of lithium-sulfur *** fluorine modulation regulate the reaction process of Li-S chemistry?Here,the TiOF/Ti_(3)C_(2)MXene nanoribbons with a tailored F distribution were constructed via an NH4F fluorinated *** on in situ characterizations and electrochemical analysis,the F activates the catalysis function of Ti metal atoms in the consecutive redox *** positive charge of Ti metal sites is increased due to the formation of O-Ti-F bonds based on the Lewis acid-base mechanism,which contributes to the adsorption of polysulfides,provides more nucleation sites and promotes the cleavage of S-S *** facilitates the deposition of Li_(2)S at lower ***,fluorine has the capacity to capture electrons originating from Li_(2)S dissolution due to charge compensation *** fluorine modulation strategy holds the promise of guiding the construction of fluorine-based catalysts and facilitating the seamless integration of multiple consecutive heterogeneous catalytic processes.

关键词： Catalysis Fluorination MXene Lithium-sulfur battery Shuttle effect

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A Radiative-Cooling Hierarchical Aligned Porous Poly(vinylidene fluoride)Film by Freeze-Thaw-Promoted Nonsolvent-Induced Phase Separation

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Chinese Journal of Polymer science 2024年第7期42卷 976-983,I0009页

作者： Yiting Zhang Jiahui Sun Yufeng Wang Yunchen Wu Chun Huang Chao Zhang Tianxi Liu Key Laboratory of Synthetic and Biological Colloids Ministry of Education School of Chemical and Material EngineeringJiangnan UniversityWuxi214122China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai201620China

Passive daytime radiative cooling(PDRC)is an innovative and sustainable cooling technology that holds immense potential for addressing the energy *** the numerous reports on radiative coolers,the design of a straightforward,efficient,and readily producible system remains a ***,we present the development of a hierarchical aligned porous poly(vinylidene fluoride)(HAP-PVDF)film through a freeze-thaw-promoted nonsolvent-induced phase separation *** film features oriented microporous arrays in conjunction with random nanopores,enabling efficient radiative cooling performance under direct sunlight *** incorporation of both micro-and nano-pores in the HAP-PVDF film results in a remarkable solar reflectance of 97%and a sufficiently high infrared thermal emissivity of 96%,facilitating sub-environmental cooling at 18.3℃ on sunny days and 13.1℃ on cloudy ***,the HAP-PVDF film also exhibits exceptional flexibility and *** calculations further confirm a radiative cooling power of 94.8 W·m^(-2)under a solar intensity of 1000W·m^(-2),demonstrating a performance comparable to the majority of reported radiative coolers.

关键词： Daytime radiative cooling Hierarchical porosity PVDF porous film Thermal insulation Nonsolvent-induced phase separation

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Bamboo-like MnO_(2)·Co_(3)O_(4):High-performance catalysts for the oxidative removal of toluene

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Journal of Environmental sciences 2025年第1期147卷 617-629页

作者： Ali Rastegarpanah Jiguang Deng Yuxi Liu Lin Jing Wenbo Pei Jia Wang Hongxing Dai Beijing Key Laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

Themanganese-cobalt mixed oxide nanorodswere fabricated using a hydrothermalmethod with different metal precursors(KMnO_(4)and MnSO_(4)·H_(2)O for MnOx and Co(NO3)2>6H_(2)O and CoCl_(2)>6H_(2)O for Co_(3)O_(4)).Bamboo-like MnO_(2)>Co_(3)O_(4)(B-MnO_(2)>Co_(3)O_(4)(S))was derived from repeated hydrothermal treatments with Co_(3)O_(4)@MnO_(2)and MnSO_(4)>H_(2)O,whereas Co_(3)O_(4)@MnO_(2)nanorods were derived from hydrothermal treatment with Co_(3)O_(4)nanorods and KMnO_(4).The study shows that manganese oxide was tetragonal,while the cobalt oxide was found to be cubic in the crystalline *** surface ions were present in multiple oxidation states(e.g.,Mn^(4+)and Mn^(3+))and surface oxygen *** content of adsorbed oxygen species and reducibility at low temperature declined in the sequence of BMnO_(2)>Co_(3)O_(4)(S)>Co_(3)O_(4)@MnO_(2)>MnO_(2)>Co_(3)O_(4),matching the changing trend in *** all the samples,B-MnO_(2)>Co_(3)O_(4)(S)showed the preeminent catalytic performance for the oxidation of toluene(T10%=187℃,T50%=276℃,and T90%=339℃).In addition,the B-MnO_(2)>Co_(3)O_(4)(S)sample also exhibited good H_(2)O^(-),CO_(2)^(-),and SO_(2)^(-)resistant *** good catalytic performance of B-MnO_(2)>Co_(3)O_(4)(S)is due to the high concentration of adsorbed oxygen species and good reducibility at low *** oxidation over B-MnO_(2)>Co_(3)O_(4)(S)proceeds through the adsorption of O_(2)and toluene to form O∗,OH∗,and H_(2)C(C6H5)∗species,which then react to produce benzyl alcohol,benzoic acid,and benzaldehyde,ultimately converting to CO_(2)and H_(2)*** findings suggest that B-MnO_(2)>Co_(3)O_(4)(S)has promising potential for use as an effective catalyst in practical applications.

关键词： Manganese-cobalt mixed oxide Nanorod Bamboo-like morphology Hydrothermal method Toluene oxidation

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Fluorine-containing polyimide nanofiber membranes for durable and anti-aging daytime radiative cooling

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Journal of materials science & Technology 2024年第12期179卷 166-173页

作者： Qiaoran Zhang Tiantian Xue Yang Lu Lei Ma Dingyi Yu Tianxi Liu Wei Fan Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China

Personal daytime radiative cooling(PDRC)materials have high sunlight reflection and high selective emis-sivity to outer space in the main atmospheric window,demonstrating huge potential in energy-saving for sustainable ***,polymer-based membranes for radiative cooling have been widely re-ported,due to their easy processing,low cost,and unique optical ***,the desired high sunlight reflectance of PDRC materials is easily dampened by environmental aging,high temperature,and ultraviolet(UV)irradiation,resulting in reduced cooling performance for most polymers,adverse to large-scale practical *** this work,we demonstrate a novel polyimide nanofiber(PINF)membrane with a fluorine-containing structure via typical electrospinning *** resultant PINF membrane exhibits high sunlight reflectance,UV resistance,and excellent thermal stability,rendering anti-aging day-time radiative *** sunlight reflectance of PINF membranes could maintain constant in the aging test for continuous 720 h under outdoor solar irradiation,exhibiting durable and long-term personal day-time radiative cooling performance.

关键词： Polyimide Nanofiber UV resistance Daytime radiative cooling

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Amide-functionalized MOG for effective adsorption of U(Ⅵ)and Pb(Ⅱ)from nuclear wastewater

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Rare Metals 2024年第12期43卷 6781-6790页

作者： Qi Zhou Dong-Ling Peng Guo-Jian Ren Chao-Wei Zhang Ling-Long Yi Qin-He Pan Key Laboratory of Advanced Materials of Tropical Island Resources Ministry of EducationSchool of Chemistry and Chemical EngineeringHainan UniversityHaikou570228China College of Food Science and Engineering Hainan UniversityHaikou570228China

Nuclear energy,recognized as one of the most environmentally friendly energy sources available,has undergone extensive *** the utilization of nuclear energy,the generation of nuclear wastewater containing significant ... 详细信息

关键词： energy Pb(Ⅱ) adsorption

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The aging behavior,microstructure and mechanical properties of AlN/AZ91 composite

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Journal of Magnesium and Alloys 2023年第7期11卷 2458-2468页

作者： Yunxia Sun Changlin Yang Bin Zhang Jianfeng Fan Hongxiang Li Tianhao Zhao Jing Li State Key Laboratory of Solidification Processing Northwestern Polytechnical UniversityXi’anShaanxi 710072PR China Yangtze River Delta Research Institute of NPU TaicangJiangsu 215400PR China Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of EducationTaiyuan University of TechnologyTaiyuan 030024PR China State Key Laboratory for Advanced Metals and Materials University of Science and Technology BeijingBeijing 100083PR China

Microstructure evolution and mechanical properties of the aging treated AlN/AZ91 composites were systematically investigated by optical microscopy(OM),high resolution scanning electron microscopy(HRSEM)with an energy dispersive spectrum(EDS),and high-angle annular dark field scanning transmission electron microscopy(HAADF-STEM).The results show that the higher fracture elongation(14±1%)and ultimate tensile strength(275±6 MPa)were simultaneously obtained in the peak-aged AlN/AZ91 *** with AZ91 matrix alloy,the strength was increased by about 44%and the elongation was approximately five times higher,which mainly attributed to the precipitation of nano-sizedγ-Mg_(17)Al_(12)phase and the activation of non-basal slip systems induced by in-situ AlN particles at room ***,the in-situ formation of AlN reinforcements consumed part of Al element in the matrix alloy,which resulted into the volume fraction decreasing ofγ-Mg_(17)Al_(12)precipitates,and then the age hardening and strengthening efficiency were reduced in the AlN/AZ91 *** the other hand,the mismatch of thermal expansion coefficient between AlN particles and AZ91 matrix generated high density dislocations around AlN particles,which promoted the precipitation ofγ-Mg_(17)Al_(12)phase,and then the peak aging time and temperature were decreased.

关键词： Magnesium matrix composites In-situ AlN particles Aging behavior Microstructure Mechanical properties

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