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学者姓名：黄兴
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Developing active, stable, and cost-efficient electrocatalysts to replace platinum for the alkaline hydrogen evolution reaction (HER) is highly desirable yet represents a great challenge. Here, it is reported on a facile one-pot synthesis of RuxNi layered double hydroxides (RuxNi-LDHs) that exhibit remarkable HER activity and stability after an in-situ activation treatment, surpassing most state-of-the-art Ru-based catalysts as well as commercial Ru/C and Pt/C catalysts. The structural and chemical changes triggered by in-situ activation are systematically investigated, and the results clearly show that the pristine, less-active RuxNi-LDHs are transformed into a highly active catalyst characterized by raft-like, defect-rich Ru degrees particles decorated on the surface of RuxNi-LDHs. Density functional theory (DFT) calculations reveal that the defective Ru sites can effectively optimize the reaction pathway and lower the free energies of the elemental steps involved, leading to enhanced intrinsic activity. This work highlights the importance of the currently understudied strategy of defect engineering in boosting the HER activity of Ru-based catalysts and offers an effective approach involving in-situ electrochemical activation for the development of high-performance alkaline HER catalysts.
Keyword ：
alkaline HER alkaline HER defect engineering defect engineering defective Ru-degrees NPs defective Ru-degrees NPs first-principles calculations first-principles calculations RuxNi-LDHs RuxNi-LDHs
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| GB/T 7714 | Shi, Ningning , Ma, Ruijie , Lin, Linghui et al. In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution [J]. | SMALL , 2024 , 20 (27) . |
| MLA | Shi, Ningning et al. "In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution" . | SMALL 20 . 27 (2024) . |
| APA | Shi, Ningning , Ma, Ruijie , Lin, Linghui , Xie, Wangjing , Liu, Panpan , Li, Peng et al. In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution . | SMALL , 2024 , 20 (27) . |
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Alloying metals to form intermetallics has been proven effective in tuning the chemical properties of metal-based catalysts. However, intermetallic alloys can undergo structural and chemical transformations under reactive conditions, leading to changes in their catalytic function. Elucidating and understanding these transformations are crucial for establishing relevant structure-performance relationships and for the rational design of alloy-based catalysts. In this work, we used CuZn alloy nanoparticles (NPs) as a model material system and employed in situ transmission electron microscopy (TEM) to investigate the structural and chemical changes of CuZn NPs under H-2, O-2 and their mixture. Our results show how CuZn NPs undergo sequential transformations in the gas mixture at elevated temperatures, starting with gradual leaching and segregation of Zn, followed by oxidation at the NP surface. The remaining copper at the core of particles can then engage in dynamic behavior, eventually freeing itself from the zinc oxide shell. The structural dynamics arises from an oscillatory phase transition between Cu and Cu2O and is correlated with the catalytic water formation, as confirmed by in situ mass spectrometry (MS). Under pure H-2 or O-2 atmosphere, we observe different structural evolution pathways and final chemical states of CuZn NPs compared to those in the gas mixture. These results clearly demonstrate that the chemical state of alloy NPs can vary considerably under reactive redox atmospheres, particularly for those containing elements with distinct redox properties, necessitating the use of in situ or detailed ex situ characterizations to gain relevant insights into the states of intermetallic alloy-based catalysts and structure-activity relationships.
Keyword ：
CuZn alloy CuZn alloy In situ transmission electron microscopy (TEM) In situ transmission electron microscopy (TEM) redox atmosphere redox atmosphere structural and chemical transformations structural and chemical transformations
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| GB/T 7714 | Yue, Shengnan , Li, Qian , Zeng, Chaobin et al. Structural and chemical transformations of CuZn alloy nanoparticles under reactive redox atmospheres: An in situ TEM study [J]. | NANO RESEARCH , 2024 , 17 (7) : 6265-6273 . |
| MLA | Yue, Shengnan et al. "Structural and chemical transformations of CuZn alloy nanoparticles under reactive redox atmospheres: An in situ TEM study" . | NANO RESEARCH 17 . 7 (2024) : 6265-6273 . |
| APA | Yue, Shengnan , Li, Qian , Zeng, Chaobin , Klyushin, Alexander , Farra, Ramzi , Willinger, Marc-Georg et al. Structural and chemical transformations of CuZn alloy nanoparticles under reactive redox atmospheres: An in situ TEM study . | NANO RESEARCH , 2024 , 17 (7) , 6265-6273 . |
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Alkali-metal doped perovskite oxides have emerged as promising materials due to their unique properties and broad applications in various fields, including photovoltaics and catalysis. Understanding the complex interplay between alkali metal doping, structural modifications, and their impact on performance remains a crucial challenge. In this study, this challenge is addressed by investigating the synthesis and properties of Rb-doped perovskite oxides. These results reveal that the doping of Rb into perovskite oxides function as a structural modifier in the as-synthesized samples and during the oxygen evolution reaction (OER) as well. Electron microscopy and first-principles calculations confirm the enrichment of Rb on the surface of the as-synthesized sample. Further investigations into the electrocatalytic reaction revealed that the Rb-doped perovskite underwent drastic restructuring with Rb leaching and formation of strontium oxide. Rb-doped perovskite oxides are successfully fabricated in this study. However, an excessive introduction of Rb does not entirely mitigate Rb volatilization during synthesis at elevated temperatures. A surface enrichment of Rb is observed within the perovskite structure. During the oxygen evolution reaction, a significant structural evolution occurs, along with the detection of Rb leaching and the formation of strontium oxide. image
Keyword ：
alkali metal doping alkali metal doping oxygen evolution reaction oxygen evolution reaction perovskite oxide perovskite oxide surface enrichment surface enrichment surface reconstruction surface reconstruction
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| GB/T 7714 | Xie, Huachao , Zhang, Yuxuan , Liu, Panpan et al. Rb-Doped Perovskite Oxides: Surface Enrichment and Structural Reconstruction During the Oxygen Evolution Reaction [J]. | SMALL , 2024 . |
| MLA | Xie, Huachao et al. "Rb-Doped Perovskite Oxides: Surface Enrichment and Structural Reconstruction During the Oxygen Evolution Reaction" . | SMALL (2024) . |
| APA | Xie, Huachao , Zhang, Yuxuan , Liu, Panpan , Duo, Xuyao , Hu, Zhonghui , Yu, Jia et al. Rb-Doped Perovskite Oxides: Surface Enrichment and Structural Reconstruction During the Oxygen Evolution Reaction . | SMALL , 2024 . |
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Atomically precise low-nuclearity (n<10) silver nanoclusters (AgNCs) have garnered significant interest due to their size-dependent optical properties and diverse applications. However, their synthesis has remained challenging, primarily due to their inherent instability. The present study introduces a new feasible approach for clustering silver ions utilizing highly negative and redox-inert polyoxoniobates (PONbs) as all-inorganic ligands. This strategy not only enables the creation of novel Ag-PONb composite nanoclusters but also facilitates the synthesis of stable low-nuclearity AgNCs. Using this method, we have successfully synthesized a small octanuclear rhombic [Ag-8](6+) AgNC stabilized by six highly negative [LiNb27O75](14-) polyoxoanions. This marks the first PONb-protected superatomic AgNC, designated as {Ag-8@(LiNb27O75)(6)} (Ag-8@Nb-162), with an aesthetically spherical core-shell structure. The crystalline Ag-8@Nb-162 is stable under ambient conditions, What's more, it is water-soluble and able to maintain its molecular cluster structure intact in water. Further, the stable small [Ag-8](6+) AgNC has interesting temperature- and pH-dependent reversible fluorescence response, based on which a multiple optical encryption mode for anti-counterfeit technology was demonstrated. This work offers a promising avenue for the synthesis of fascinating and stable PONb-protected AgNCs and sheds light on the development of new-type optical functional materials.
Keyword ：
fluorescence fluorescence macromolecules macromolecules nanoclusters nanoclusters polyoxoniobate polyoxoniobate silver silver
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| GB/T 7714 | Hong, Li-Hao , Yue, Sheng-Nan , Huang, Xing et al. Development of Stable Water-Soluble Supratomic Silver Clusters Utilizing A Polyoxoniobate-Protected Strategy: Giant Core-Shell-Type Ag8@Nb162 Fluorescent Nanocluster [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (29) . |
| MLA | Hong, Li-Hao et al. "Development of Stable Water-Soluble Supratomic Silver Clusters Utilizing A Polyoxoniobate-Protected Strategy: Giant Core-Shell-Type Ag8@Nb162 Fluorescent Nanocluster" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 29 (2024) . |
| APA | Hong, Li-Hao , Yue, Sheng-Nan , Huang, Xing , Sun, Cai , Cai, Ping-Wei , Sun, Yan-Qiong et al. Development of Stable Water-Soluble Supratomic Silver Clusters Utilizing A Polyoxoniobate-Protected Strategy: Giant Core-Shell-Type Ag8@Nb162 Fluorescent Nanocluster . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (29) . |
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Catalysts based on palladium are among the most effective in the complete oxidation of methane. Despite extensive studies and notable advances, the nature of their catalytically active species and conceivable structural dynamics remains only partially understood. Here, we combine operando transmission electron microscopy (TEM) with near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and density functional theory (DFT) calculations to investigate the active state and catalytic function of Pd nanoparticles (NPs) under methane oxidation conditions. We show that the particle size, phase composition and dynamics respond appreciably to changes in the gas-phase chemical potential. In combination with mass spectrometry (MS) conducted simultaneously with in situ observations, we uncover that the catalytically active state exhibits phase coexistence and oscillatory phase transitions between Pd and PdO. Aided by DFT calculations, we provide a rationale for the observed redox dynamics and demonstrate that the emergence of catalytic activity is related to the dynamic interplay between coexisting phases, with the resulting strained PdO having more favorable energetics for methane oxidation. Palladium-based catalysts are highly effective for the complete oxidation of methane. Here, the authors employ operando transmission electron microscopy, near-ambient pressure X-ray photoelectron spectroscopy, and density functional theory calculations to investigate the active state and catalytic function of Pd nanoparticles in methane oxidation.
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| GB/T 7714 | Yue, Shengnan , Praveen, C. S. , Klyushin, Alexander et al. Redox dynamics and surface structures of an active palladium catalyst during methane oxidation [J]. | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
| MLA | Yue, Shengnan et al. "Redox dynamics and surface structures of an active palladium catalyst during methane oxidation" . | NATURE COMMUNICATIONS 15 . 1 (2024) . |
| APA | Yue, Shengnan , Praveen, C. S. , Klyushin, Alexander , Fedorov, Alexey , Hashimoto, Masahiro , Li, Qian et al. Redox dynamics and surface structures of an active palladium catalyst during methane oxidation . | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
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Platinum nanoparticles (NPs) supported by titania exhibit a strong metal-support interaction (SMSI)([1]) that can induce overlayer formation and encapsulation of the NP's with a thin layer of support material. This encapsulation modifies the catalyst's properties, such as increasing its chemoselectivity([2]) and stabilizing it against sintering.([3]) Encapsulation is typically induced during high-temperature reductive activation and can be reversed through oxidative treatments.([1]) However, recent findings indicate that the overlayer can be stable in oxygen.([4, 5]) Using in situ transmission electron microscopy, we investigated how the overlayer changes with varying conditions. We found that exposure to oxygen below 400 degrees C caused disorder and removal of the overlayer upon subsequent hydrogen treatment. In contrast, elevating the temperature to 900 degrees C while maintaining the oxygen atmosphere preserved the overlayer, preventing platinum evaporation when exposed to oxygen. Our findings demonstrate how different treatments can influence the stability of nanoparticles with or without titania overlayers. expanding the concept of SMSI and enabling noble metal catalysts to operate in harsh environments without evaporation associated losses during burn-off cycling.
Keyword ：
Electron Microscopy Electron Microscopy Heterogeneous Catalysis Heterogeneous Catalysis Metal-Support Interaction Metal-Support Interaction Platinum Platinum
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| GB/T 7714 | Beck, Arik , Frey, Hannes , Huang, Xing et al. Controlling the Strong Metal-Support Interaction Overlayer Structure in Pt/TiO2 Catalysts Prevents Particle Evaporation [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 . |
| MLA | Beck, Arik et al. "Controlling the Strong Metal-Support Interaction Overlayer Structure in Pt/TiO2 Catalysts Prevents Particle Evaporation" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2023) . |
| APA | Beck, Arik , Frey, Hannes , Huang, Xing , Clark, Adam H. , Goodman, Emmett D. , Cargnello, Matteo et al. Controlling the Strong Metal-Support Interaction Overlayer Structure in Pt/TiO2 Catalysts Prevents Particle Evaporation . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 . |
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Carbon-supported metal nanoparticles (NPs) comprise an important class of heterogeneous catalysts. The interaction between the metal and carbon support influences the overall material properties, viz., the catalytic performance. Herein we use in situ and ex situ transmission electron microscopy (TEM) in combination with in situ X-ray spectroscopy (XPS) to investigate the encapsulation of metallic iridium NPs by carbon in an Ir/C catalyst. Real-time atomic-scale imaging visualizes particle reshaping and increased graphitization of the carbon support upon heating of Ir/C in vacuum. According to in situ TEM results, carbon overcoating grows over Ir NPs during the heating process, starting from ca. 550 degrees C. With the carbon overlayers formed, no sintering and migration of Ir NPs is observed at 800 degrees C, yet the initial Ir NPs sinter at or below 550 degrees C, i.e., at a temperature associated with an incomplete particle encapsulation. The carbon overlayer corrugates when the temperature is decreased from 800 to 200 degrees C and this process is associated with the particle surface reconstruction and is reversible, such that the corrugated carbon overlayer can be smoothed out by increasing the temperature back to 800 degrees C. The catalytic performance (activity and stability) of the encapsulated Ir NPs in the hydrogen evolution reaction (HER) is higher than that of the initial (nonencapsulated) state of Ir/C. Overall, this work highlights microscopic details of the currently understudied phenomenon of the carbon encapsulation of supported noble metal NPs and demonstrates additionally that the encapsulation by carbon is an effective measure for tuning the catalytic performance.
Keyword ：
carbonsupported metal NPs carbonsupported metal NPs DFT calculations DFT calculations encapsulation encapsulation HER HER in situ TEM in situ TEM SMSI SMSI
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| GB/T 7714 | Liu, Panpan , Klyushin, Alexander , Chandramathy Surendran, Praveen et al. Carbon Encapsulation of Supported Metallic Iridium Nanoparticles: An in Situ Transmission Electron Microscopy Study and Implications for Hydrogen Evolution Reaction [J]. | ACS NANO , 2023 , 17 (23) : 24395-24403 . |
| MLA | Liu, Panpan et al. "Carbon Encapsulation of Supported Metallic Iridium Nanoparticles: An in Situ Transmission Electron Microscopy Study and Implications for Hydrogen Evolution Reaction" . | ACS NANO 17 . 23 (2023) : 24395-24403 . |
| APA | Liu, Panpan , Klyushin, Alexander , Chandramathy Surendran, Praveen , Fedorov, Alexey , Xie, Wangjing , Zeng, Chaobin et al. Carbon Encapsulation of Supported Metallic Iridium Nanoparticles: An in Situ Transmission Electron Microscopy Study and Implications for Hydrogen Evolution Reaction . | ACS NANO , 2023 , 17 (23) , 24395-24403 . |
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本发明公开了一种镍基过渡金属配合物及其制备方法和应用。所述配合物的化学式为Ni2(pko)4(ppoa)2，其中，Hpko=二(2‑吡啶)酮肟，ppoa=苯基膦酸；属于单斜晶系，C21/c空间群，晶胞参数为a=20.3165(17)Å，b=15.4122(17)Å，c=20.1208(18)Å，α=90°，β=108.827(3)°，γ=90°，Z=4。所述配合物通过扩散法生成，制备方法简单，操作简便；其作为均相催化剂溶解于电解质溶液中，可以作为电催化剂用于将CO2电化学还原为CO。
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| GB/T 7714 | 黄兴 , 史宁宁 , 杨顺航 et al. 一种镍基过渡金属配合物及其制备方法和应用 : CN202210619002.3[P]. | 2022-06-01 00:00:00 . |
| MLA | 黄兴 et al. "一种镍基过渡金属配合物及其制备方法和应用" : CN202210619002.3. | 2022-06-01 00:00:00 . |
| APA | 黄兴 , 史宁宁 , 杨顺航 , 刘盼盼 . 一种镍基过渡金属配合物及其制备方法和应用 : CN202210619002.3. | 2022-06-01 00:00:00 . |
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Oxidative dehydrogenation of propane with carbon dioxide (CO2-ODP) characterizes the tandem dehy-drogenation of propane to propylene with the reduction of the greenhouse gas of CO2 to valuable CO. However, the existing catalyst is limited due to the poor activity and stability, which hinders its indus-trialization. Herein, we design the finned Zn-MFI zeolite encapsulated noble metal nanoparticles (NPs) as bifunctional catalysts (NPs@Zn-MFI) for CO2-ODP. Characterization results reveal that the Zn2+ species are coordinated with the MFI zeolite matrix as isolated cations and the NPs of Pt, Rh, or RhPt are highly dispersed in the zeolite crystals. The isolated Zn2+ cations are very effective for activating the propane and the small NPs are favorable for activating the CO2, which synergistically promote the selective transfor-mation of propane and CO2 to propylene and CO. As a result, the optimal 0.25%Rh0.50%Pt@Zn-MFI cata-lyst shows the best propylene yield, satisfactory CO2 conversion, and long-term stability. Moreover, considering the tunable synergetic effects between the isolated cations and NPs, the developed approach offers a general guideline to design more efficient CO2-ODP catalysts, which is validated by the improved performance of the bifunctional catalysts via simply substituting Sn4+cations for Zn2+ cations in the MFI zeolite matrix.(c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences Published by Elsevier B.V. All rights reserved.
Keyword ：
Carbon dioxide Carbon dioxide Encapsulated noble metal nanoparticles Encapsulated noble metal nanoparticles Finned Zn-MFI zeolite Finned Zn-MFI zeolite Oxidative dehydrogenation Oxidative dehydrogenation Propane Propane
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| GB/T 7714 | Yuan, En-Hui , Niu, Yiming , Huang, Xing et al. Finned Zn-MFI zeolite encapsulated noble metal nanoparticle catalysts for the oxidative dehydrogenation of propane with carbon dioxide [J]. | JOURNAL OF ENERGY CHEMISTRY , 2023 , 80 : 479-491 . |
| MLA | Yuan, En-Hui et al. "Finned Zn-MFI zeolite encapsulated noble metal nanoparticle catalysts for the oxidative dehydrogenation of propane with carbon dioxide" . | JOURNAL OF ENERGY CHEMISTRY 80 (2023) : 479-491 . |
| APA | Yuan, En-Hui , Niu, Yiming , Huang, Xing , Li, Meng , Bao, Jun , Song, Yong-Hong et al. Finned Zn-MFI zeolite encapsulated noble metal nanoparticle catalysts for the oxidative dehydrogenation of propane with carbon dioxide . | JOURNAL OF ENERGY CHEMISTRY , 2023 , 80 , 479-491 . |
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The commercial application of lithium-sulfur batteries is severely hampered by polysulfide shuttle effects, sluggish redox kinetics, and uncontrollable lithium dendrite growth. Herein, a unique Ni-doped CoSe2 nanoparticle decorated bilayer carbon (Ni-CoSe2/BC) structure is synthesized for both the sulfur cathode and lithium anode, which introduces bi-functionalities including I) the internal carbon conductive network skeleton of carbon nanotubes is capable of physically confining, storing, and alleviating volume expansion of sulfur; and II) Ni-CoSe2 nanoparticles decorated on the external carbon nanoarrays contribute to efficient chemical anchoring and accelerated polysulfide conversion for the cathode, and serve as lithiophilic sites to induce homogeneous lithium deposition for the anode. As a result, Ni-CoSe2/BC effectively inhibits the shuttle effect and induces dendrite-free lithium deposition. The Ni-CoSe2/BC-S delivers a high discharge specific capacity of 806 mAh g- 1 after 400 cycles at 1 C, with a low capacity decay rate of 0.07% per cycle. Moreover, the Ni-CoSe2/BC-Li exhibits an impressively long cycle life of 2000 h at 10 mA cm-2/10 mAh cm-2. Notably, the lithium-sulfur full cell assembled with Ni-CoSe2/BC as universal hosts for both anode and cathode possesses an average discharge capacity of 6.07 mAh cm-2 in 50 cycles (Sulfur loading=12.8 mg cm-2, Electrolyte/Sulfur=7.8 & mu;L mg-1, and Negative/Positive=1.56). This work provides novel structural design and mechanism insights for the practical application of lithium-sulfur batteries.
Keyword ：
Carbon nanostructure Carbon nanostructure Catalysis Catalysis Li -S batteries Li -S batteries Lithium metal anode Lithium metal anode Lithium polysulfides Lithium polysulfides Metal-organic frameworks Metal-organic frameworks Metal selenide Metal selenide
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| GB/T 7714 | Xie, Yonghui , Zheng, Wenrui , Ao, Juan et al. Multifunctional Ni-doped CoSe2 nanoparticles decorated bilayer carbon structures for polysulfide conversion and dendrite-free lithium toward high-performance Li-S full cell [J]. | ENERGY STORAGE MATERIALS , 2023 , 62 . |
| MLA | Xie, Yonghui et al. "Multifunctional Ni-doped CoSe2 nanoparticles decorated bilayer carbon structures for polysulfide conversion and dendrite-free lithium toward high-performance Li-S full cell" . | ENERGY STORAGE MATERIALS 62 (2023) . |
| APA | Xie, Yonghui , Zheng, Wenrui , Ao, Juan , Shao, Yeqing , Huang, Xing , Li, Hong et al. Multifunctional Ni-doped CoSe2 nanoparticles decorated bilayer carbon structures for polysulfide conversion and dendrite-free lithium toward high-performance Li-S full cell . | ENERGY STORAGE MATERIALS , 2023 , 62 . |
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