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Rational design of hierarchically porous Fe-N-doped carbon as efficient electrocatalyst for oxygen reduction reaction and Zn-air batteries

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Nano Research 2021年第12期14卷 4768-4775页

作者： Zihan Meng Neng Chen Shichang Cai Jiawei Wu Rui Wang Tian Tian Haolin Tang Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan528200China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China School of Material Science and Engineering Henan University of TechnologyZhengzhou450001China

The rational design and construction of hierarchically porous nanostructure for oxygen reduction reaction (ORR) electrocatalysts is crucial to facilitate the exposure of accessible active sites and promote the mass/electron transfer under the gas-solid-liquid triple-phase condition. Herein, an ingenious method through the pyrolysis of creative polyvinylimidazole coordination with Zn/Fe salt precursors is developed to fabricate hierarchically porous Fe-N-doped carbon framework as efficient ORR electrocatalyst. The volatilization of Zn species combined with the nanoscale Kirkendall effect of Fe dopants during the pyrolysis build the hierarchical micro-, meso-, and macroporous nanostructure with a high specific surface area (1,586 m^(2)·g^(−1)), which provide sufficient exposed active sites and multiscale mass/charge transport channels. The optimized electrocatalyst exhibits superior ORR activity and robust stability in both alkaline and acidic electrolytes. The Zn-air battery fabricated by such attractive electrocatalyst as air cathode displays a higher peak power density than that of Pt/C-based Zn-air battery, suggesting the great potential of this electrocatalyst for Zn-air batteries.

关键词： hierarchically porous structure Fe-N-doped carbon electrocatalysts oxygen reduction reaction Zn-air batteries

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Trace of Atomically Dispersed Pd Enables Unprecedented Butadiene Semihydrogenation Performance Over Copper Catalyst

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ACS Catalysis 2025年第5期15卷 3810-3822页

作者： Zhao Wang Hao Yuan Jian Tao Shu-Lin Liu Ying Hong Zhi-Yi Hu Jian Zhang Bao-Lian Su The State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China State Key Laboratory of Solidification Processing School of Materials Science and Engineering Northwestern Polytechnical University Xi’an Shaanxi 710000 P. R. China The State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China；Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles Namur B-5000 Belgium

Semihydrogenation plays a key role in industrial hydrorefining of light alkenes, with a market above 400 billion by 2027. The high cost of commercial palladium-based catalysts strongly calls for innovation but with great challenges. Herein, copper nanoparticles decorated with a minimized ppm of Pd are developed through a chemical plating process to integrate the catalytic advantages of copper and palladium for achieving maximized catalysis in the semihydrogenation of a fatal impurity of butadiene in alkene feedstocks. The developed Pd–Cu catalyst (i.e., 114 ppm of Pd in Pd0.0033Cu1/TiO2) exhibits an unprecedented catalytic performance superior to commercial Pd/Al2O3, with 100% butene selectivity above 90% of butadiene conversion over 130 h on stream at 90 °C. Further exploration reveals that the atomically dispersed Pd on Cu nanoparticles, obtained at ultralow ppm levels of Pd loading, induces a hidden but critical H2trap, which concentrates H2on the Pd site for further H2dissociation that offers intermediate hydrogen atoms to the tandem butadiene semihydrogenation over the third layer of Cu atoms neighboring Pd through hydrogen spillover. Moreover, a threshold on Pd density was identified at Pd/Cu surficial atomic ratio of 1/138 (i.e., Pd0.0033Cu1/TiO2) for maximizing butadiene semihydrogenation performance, based on an extreme collaboration between Pd for H2dissociation and Cu for butadiene hydrogenation. This work provides important guidance for developing noble metal-saving catalysts in industrial applications.

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Energy Storage Mechanism of Vanadium Nitride via Intercalating Different Atomic Radius for Expanding Interplanar Spacing

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Energy & Environmental materials 2022年第2期5卷 565-571页

作者： Ying Liu Lingyang Liu Long Kang Fen Ran State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals School of Material Science and EngineeringLanzhou University of TechnologyLanzhou 730050China Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical EngineeringLiaocheng UniversityLiaocheng 252059China

As a promising anode material in supercapacitors,vanadium nitride has been widely concerned due to its ultra-high theoretical specific ***,its routine test capacitance value is still far from the theoretical value and its energy storage mechanism is *** order to solve these two key problems,here we prepare interplanar spacing expanded vanadium nitride materials with different impurity atoms intercalation from two anionic precursors of vanadium-based metal organic frameworks with different functional *** obtained vanadium nitride reaches a higher specific capacitance;and further,through ex situ X-Ray diffraction and in situ Raman,the charge storage of vanadium nitride is contributed by two processes:the first benefit is from the K^(+) de/intercalation in the interplanar spacing,and the other one is derived from the redox reaction with OH−by adsorption on ***,both of the first principle calculation and extended experiments support this *** believe that such detailed research on the energy storage mechanism can provide a clear idea for the application of metal nitrides in supercapacitors and other energy storage devices.

关键词： electrode materials energy storage mechanism supercapacitors vanadium nitride V-MOFs

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Structural features and thermoelectric performance of Sb- and Bi-doped Cu_(2)SnSe_(3) compounds

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Rare Metals 2021年第9期40卷 2474-2485页

作者： Shu-Ping Deng Xian-Yan Jiang Li-Li Chen Zi-Ye Zhang Ning Qi Yi-Chu Wu Xin-Feng Tang Zhi-Quan Chen School of Physics and Technology Hubei Key Laboratory of Nuclear Solid State PhysicsWuhan UniversityWuhan 430072China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

In this paper, a series of Sb-doped and Bi-doped Cu_(2)Sn_(1-x)M_(x)Se_(3) samples(M = Sb, Bi) are prepared by vacuum melting combined with the spark plasma sintering process. The effects of different atomic doping amounts on their properties are discussed. Structural studies indicate that all obtained samples comprise a single Cu_(2)SnSe_(3) phase. Sb and Bi atoms are experimentally demonstrated to be efficient cation dopants for increasing the transport performance. Compared with that doping on the cation site,Bi doping is much more efficient in increasing the electron concentration of the Cu_(2)SnSe_(3) system. Ultimately, a high figure of merit of 0.36 is achieved in the Cu_(2)Sn_(0.94)Sb_(0.06) Se_(3) sample at 773 K due to the enhanced power factor and lowered lattice thermal conductivity,which are 1.73 times higher than those of the pure *** results provide an efficient approach to enhance thermoelectric performance via other doping atoms, which could also be applied to copper-based chalcogenide materials.

关键词： Thermoelectric properties Positron annihilation spectroscopy Ternary copper chalcogenide Structure features Doping Polycrystalline

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Recent progress in C-N coupling for electrochemical CO_(2) reduction with inorganic nitrogenous species in aqueous solution

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materials Reports(Energy) 2023年第1期3卷 65-77,I0003页

作者： Shuxia Liu Tanyuan Wang Lior Elbaz Qing Li State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanHubei430074China Department of Chemistry and the Institute of Nanotechnology and Advanced Materials Bar-Ilan UniversityRamat-Gan5290002Israel

The electrocatalytic CO_(2) reduction in aqueous solution mainly involves bond cleavage and formation between C,H and O,and it is highly desirable to expand the bond formation reaction of C with other atoms to obtain novel and valuable *** electrochemical synthesis of N-containing organic chemicals in electrocatalytic CO_(2) reduction via introducing N sources is an effective strategy to expand the product scope,since chemicals con-taining C–N bonds(*** and amines)are important reactants/products for medicine,agriculture and *** article focuses on the research progress of C–N coupling from CO_(2) and inorganic nitrogenous species in aqueous ***,the reaction pathways related to the reaction intermediates for urea,formamide,acetamide,methylamine and ethylamine are ***,the electrocatalytic performance of different catalysts for these several N-containing products are summarized and ***,the challenges and op-portunities are analyzed,aiming to provide general insights into future research directions for electrocatalytic C–N coupling.

关键词： CO_(2) reduction C-N coupling Heterogeneous electrocatalysis Amide Amine

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Two-Dimensional materials for Highly Efficient and Stable Perovskite Solar Cells

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Nano-Micro Letters 2024年第10期16卷 176-212页

作者： Xiangqian Shen Xuesong Lin Yong Peng Yiqiang Zhang Fei Long Qifeng Han Yanbo Wang Liyuan Han State Key Laboratory of Metal Matrix Composites Shanghai Jiao Tong UniversityShanghai 200240People's Republic of China Xinjiang Key Laboratory of Solid State Physics and Devices School of Physical Science and TechnologyXinjiang UniversityUrumqi 830046People's Republic of China Special Division of Environmental and Energy Science College of Arts and SciencesKomaba Organization for Educational ExcellenceUniversity of TokyoTokyo 153-8902Japan State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070People's Republic of China College of Chemistry Henan Institute of Advanced TechnologyZhengzhou UniversityZhengzhou 450001People's Republic of China Guangxi Key Laboratory of Optical and Electronic Materials and Devices Collaborative Innovation Center for Exploration of Nonferrous Metal Deposits and Efficient Utilization of ResourcesSchool of Materials Science and EngineeringGuilin University of TechnologyGuilin 541004People's Republic of China

Perovskite solar cells(PSCs)offer low costs and high power conversion ***,the lack of long-term stability,primarily stemming from the interfacial defects and the sus-ceptible metal electrodes,hinders their practical *** the past few years,two-dimensional(2D)materials(e.g.,graphene and its derivatives,transitional metal dichalcogenides,MXenes,and black phosphorus)have been identified as a promising solution to solving these problems because of their dangling bond-free surfaces,layer-dependent electronic band structures,tunable functional groups,and inherent ***,recent progress of 2D material toward efficient and stable PSCs is summarized,including its role as both interface materials and *** discuss their beneficial effects on perovskite growth,energy level alignment,defect passivation,as well as blocking external *** particular,the unique properties of 2D materials to form van der Waals heterojunction at the bottom interface are ***,perspectives on the further development of PSCs using 2D materials are provided,such as designing high-quality van der Waals heterojunction,enhancing the uniformity and coverage of 2D nanosheets,and developing new 2D materials-based electrodes.

关键词： Perovskite solar cells Two-dimensional materials Interface engineering Van der Waals heterojunction Electrodes

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The Effect of Nd^(3+) Concentration on Upconversion Luminescence in Yb^(3+)/Tm^(3+)/Nd^(3+) Tripledoped b-NaGdF_(4) Nanocrystals

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Journal of Wuhan University of technology(materials Science) 2022年第3期37卷 393-398页

作者： HOU Huayu GAN Lin WANG Youfa WANG Wei State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China School of Automotive Engineering Wuhan University of TechnologyWuhan 430070China Hubei Key Laboratory of Advanced Technology for Automotive Components Wuhan University of TechnologyWuhan 430070China Hubei Collaborative Innovation Center for Automotive Components Technology Wuhan University of TechnologyWuhan 430070China

Nd^(3+)-doped NaGdF_(4):Yb,Tm nanocrystals were synthesized by an improved high-temperature thermal decomposition method,and the effects of doping concentrations on the crystal structure,phase composition,and upconverted fluorescence intensity were also *** results reveal that the introduction of Nd^(3+) ions does not cause the transformation of the crystal phase,but induce the change of the unit cell ***,the fluorescence intensity of the synthesized nanocrystals when co-doped with 3 mol%Nd^(3+) is the strongest under the excitation of 980 nm laser,which is 3.9 times that of the Nd^(3+)-free doped nanoparticles,and the average size is 62.9 *** it is located in the blue area of the CIE coordinate diagram,and the corresponding color purity is 91.81%under the same experimental *** resulting nanocrystals show the potential as excellent fluorescence labeling and in vivo imaging probes.

关键词： upconversion Nd^(3+)doped fluorescence intensity β-NaGdF4

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Three-dimensional ordered hierarchically porous carbon materials for high performance Li-Se battery

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Journal of Energy Chemistry 2022年第5期31卷 624-636页

作者： Hongyan Li Wenda Dong Chao Li Tarek Barakat Minghui Sun Yingying Wang Liang Wu Lang Wang Lei Xia Zhi-Yi Hu Yu Li Bao-Lian Su Laboratory of Inorganic Materials Chemistry(CMI) University of NamurB-5000 NamurBelgium Namur Institute of Structured Matter(NISM) University of NamurB-5000 NamurBelgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430074HubeiChina

Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport *** optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.

关键词： 3D ordered hierarchically porous carbon(OHPC) Shuttle effect Cyclability High rate capability The generalized Murray’s law Li-Se batteries

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Deep learning-enhanced NIR-II fluorescence volumetric microscopy for dynamic 3D vascular imaging

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Journal of Innovative Optical Health Sciences 2025年第3期18卷 154-164页

作者： Shiyi Peng Yuhuang Zhang Xuanjie Mou Tianxiang Wu Mingxi Zhang Jun Qian State Key Laboratory of Extreme Photonics and Instrumentation International Research Center for Advanced PhotonicsCentre for Optical and Electromagnetic ResearchCollege of Optical Science and EngineeringZhejiang UniversityHangzhou 310058P.R.China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070P.R.China

Three-dimensional (3D) visualization of dynamic biological processes in deep tissue remains challenging due to the trade-off between temporal resolution and imaging depth. Here, we present a novel near-infrared-II (NIR-II, 900–1880nm) fluorescence volumetric microscopic imaging method that combines an electrically tunable lens (ETL) with deep learning approaches for rapid 3D imaging. The technology achieves volumetric imaging at 4.2 frames per second (fps) across a 200 μm depth range in live mouse brain vasculature. Two specialized neural networks are utilized: a scale-recurrent network (SRN) for image enhancement and a cerebral vessel interpolation (CVI) network that enables 16-fold axial upsampling. The SRN, trained on two-photon fluorescence microscopic data, improves both lateral and axial resolution of NIR-II fluorescence wide-field microscopic images. The CVI network, adapted from video interpolation techniques, generates intermediate frames between acquired axial planes, resulting in smooth and continuous 3D vessel reconstructions. Using this integrated system, we visualize and quantify blood flow dynamics in individual vessels and are capable of measuring blood velocity at different depths. This approach maintains high lateral resolution while achieving rapid volumetric imaging, and is particularly suitable for studying dynamic vascular processes in deep tissue. Our method demonstrates the potential of combining optical engineering with artificial intelligence to advance biological imaging capabilities.

关键词： NIR-II fluorescence bioimaging volumetric microscopy deep learning reconstruction dynamic vascular imaging

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Iron oxide nanoparticles with photothermal performance and enhanced nanozyme activity for bacteria-infected wound therapy

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Regenerative Biomaterials 2022年第1期9卷 548-559页

作者： Jiaxin Guo Wenying Wei Yanan Zhao Honglian Dai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Biomedical Materials and Engineering Research Center of Hubei ProvinceWuhan University of TechnologyWuhan 430070China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200China Shenzhen Research Institute of Wuhan University of Technology Shenzhen 518000China

Metal-based nanomaterials usually have broad-spectrum antibacterial properties,low biological toxicity and no drug resistance due to their intrinsic enzyme-like catalytic properties and external field(magnetic,thermal,acoustic,optical and electrical)***,iron oxide(Fe_(3)O_(4))nanoparticles(IONPs)synthesized by us have good biosafety,excellent photothermal conversion ability and peroxidase-like catalytic activity,which can be used to construct a photothermal-enzymes combined antibacterial treatment *** with peroxide-like catalytic activity can induce H_(2)O_(2)to catalyze the production of·OH in a slightly acidic environment,thus achieving certain bactericidal effects and increasing the sensitivity of bacteria to *** stimulated by near-infrared light,the photothermal effect could destroy bacterial cell membranes,resulting in cleavage and inactivation of bacterial protein,DNA or ***,it can also improve the catalytic activity of peroxidase-like and promote IONPs to catalyze the production of more·OH for killing *** IONPs synergistic treatment,the antibacterial rate of Escherichia coli and Staphylococcus aureus reached nearly 100%.It also has an obvious killing effect on bacteria in infected wounds of mice and can effectively promote the healing of *** wounds,which has great application potential in clinical anti-infection treatment.

关键词： antibacterial photothermal therapy peroxidase-like catalytic therapy

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