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学者姓名:樊华
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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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Alloy catalysts often show superior effectiveness in the growth of carbon nanotubes/nanofibers (CNTs/CNFs) as compared to monometallic catalysts. However, due to the lack of an understanding of the active state and active structure, the origin of the superior performance of alloy catalysts is unknown. In this work, we report an in situ transmission electron microscopy (TEM) study of the CNF growth enabled by one of the most active known alloy catalysts, i.e., Ni-Co, providing insights into the active state and the interaction between Ni and Co in the working catalyst. We reveal that the functioning catalyst is highly dynamic, undergoing constant reshaping and periodic elongation/contraction. Atomic-scale imaging combined with in situ electron energy-loss spectroscopy further identifies the active structure as a Ni-Co metallic alloy (face-centered cubic, FCC). Aided by the molecular dynamics simulation and density functional theory calculations, we rationalize the dynamic behavior of the catalyst and the growth mechanism of CNFs and provide insight into the origin of the superior performance of the Ni-Co alloy catalyst.
Keyword :
active state active state bulk diffusion bulk diffusion DFT calculations DFT calculations fishbone CNF fishbone CNF in situ TEM in situ TEM MD simulation MD simulation Ni-Co metallic alloy Ni-Co metallic alloy
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GB/T 7714 | Fan, Hua , Qiu, Lu , Fedorov, Alexey et al. Dynamic State and Active Structure of Ni-Co Catalyst in Carbon Nanofiber Growth Revealed by in Situ Transmission Electron Microscopy [J]. | ACS NANO , 2021 , 15 (11) : 17895-17906 . |
MLA | Fan, Hua et al. "Dynamic State and Active Structure of Ni-Co Catalyst in Carbon Nanofiber Growth Revealed by in Situ Transmission Electron Microscopy" . | ACS NANO 15 . 11 (2021) : 17895-17906 . |
APA | Fan, Hua , Qiu, Lu , Fedorov, Alexey , Willinger, Marc-Georg , Ding, Feng , Huang, Xing . Dynamic State and Active Structure of Ni-Co Catalyst in Carbon Nanofiber Growth Revealed by in Situ Transmission Electron Microscopy . | ACS NANO , 2021 , 15 (11) , 17895-17906 . |
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Developing high-performance Fe-based ammonia catalysts through simple and cost-efficient methods has received an increased level of attention. Herein, we report for the first time, the synthesis of two-dimensional (2D) FeOOH nanoflakes encapsulated by mesoporous SiO2 (mSiO(2)) via a simple solution-based method for ammonia synthesis. Due to the sticking of the mSiO(2) coating layers and the limited spaces in between, the Fe after reduction retains the 2D morphology, showing high resistance against the sintering in the harsh Haber-Bosch process. Compared to supported Fe particles dispersed on mSiO(2) spheres, the coated catalyst shows a significantly improved catalytic activity by 50% at 425 degrees C. Thermal desorption spectroscopy (TDS) reveals the existence of a higher density of reactive sites for N-2 activation in the 2D Fe catalyst, which is possibly coupled to a larger density of surface defect sites (kinks, steps, point defects) that are generally considered as active centers in ammonia synthesis. Besides the structural impact of the coating on the 2D Fe, the electronic one is elucidated by partially substituting Si with Al in the coating, confirmed by Si-29 and Al-27 magic-angle spinning nuclear magnetic resonance (MAS NMR). An increased apparent activation energy (E-a) of the Al-containing catalyst evidences an influence on the nature of the active site. The herein-developed stable 2D Fe nanostructures can serve as an example of a 2D material applied in catalysis, offering the chance of a rational catalyst design based on a stepwise introduction of various promoters, in the coating and on the metal, maintaining the spatial control of the active centers.
Keyword :
2D Fe 2D Fe ammonia synthesis ammonia synthesis electron tomography electron tomography encapsulation encapsulation mesoporous SiO2 mesoporous SiO2 steps/kinks steps/kinks
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GB/T 7714 | Fan, Hua , Folke, Jan Markus , Liu, Zigeng et al. Ultrathin 2D Fe-Nanosheets Stabilized by 2D Mesoporous Silica: Synthesis and Application in Ammonia Synthesis [J]. | ACS APPLIED MATERIALS & INTERFACES , 2021 , 13 (25) : 30187-30197 . |
MLA | Fan, Hua et al. "Ultrathin 2D Fe-Nanosheets Stabilized by 2D Mesoporous Silica: Synthesis and Application in Ammonia Synthesis" . | ACS APPLIED MATERIALS & INTERFACES 13 . 25 (2021) : 30187-30197 . |
APA | Fan, Hua , Folke, Jan Markus , Liu, Zigeng , Girgsdies, Frank , Imlau, Robert , Ruland, Holger et al. Ultrathin 2D Fe-Nanosheets Stabilized by 2D Mesoporous Silica: Synthesis and Application in Ammonia Synthesis . | ACS APPLIED MATERIALS & INTERFACES , 2021 , 13 (25) , 30187-30197 . |
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该文从伦理、生态观、技术以及环境决策等方面探究生态文明建设,认为环境问题不仅是技术造成的,因此解决环境问题不能仅靠技术本身,应从哲学、伦理学等相关学科进行综合科学分析.
Keyword :
生态伦理观 生态伦理观 生态文明 生态文明 解决途径 解决途径
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GB/T 7714 | 樊华 . 试论生态文明建设的困境 [J]. | 海峡科学 , 2009 , (11) : 6-8 . |
MLA | 樊华 . "试论生态文明建设的困境" . | 海峡科学 11 (2009) : 6-8 . |
APA | 樊华 . 试论生态文明建设的困境 . | 海峡科学 , 2009 , (11) , 6-8 . |
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