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1.
Adv Sci (Weinh) ; : e2406659, 2024 Sep 24.
Artículo en Inglés | MEDLINE | ID: mdl-39316367

RESUMEN

Hydrogen production from the decomposition of ammonia is considered an effective approach for addressing challenges associated with hydrogen storage and transportation. However, their relatively high energy consumption and low efficiency hinder practical multi-scenario applications. In this study, Y2O3-stabilized catalysts with Co-loaded onto porous nitrogen-doped carbon (Y2O3-Co/NC) are synthesized by pyrolysis of Y(NO3)3-modified ZIF-67 under an inert atmosphere, followed by annealing in a reducing environment. The introduction of Y2O3 enhanced the recombination and desorption of N atoms and facilitated the gradual dehydrogenation of NHx on the catalyst surface, resulting in improved catalytic activity for the thermal decomposition of ammonia. Benefitting from the electron-donating properties of Y2O3 and N-doped carbon, the optimized catalyst achieved a remarkable NH3 conversion efficiency of 92.3% at a high gas hourly space velocity of 20 000 cm3· g cat - 1 ${\mathrm{g}}_{{\mathrm{cat}}}^{ - {\mathrm{1}}}$ ·h-1 with an encouraging H2 production rate of 20.6 mmol· g cat - 1 ${\mathrm{g}}_{{\mathrm{cat}}}^{ - {\mathrm{1}}}$ ·min-1 at 550 °C. Moreover, the synthesized catalyst undergoes a fast-dynamic reconstruction process, resulting in exceptionally stable catalytic activity during the thermal decomposition of ammonia, rendering it a promising candidate for carbon-free energy thermocatalytic conversion technology.

2.
Artículo en Inglés | MEDLINE | ID: mdl-38598686

RESUMEN

Clathrates are potential "phonon-glass, electron-crystal" thermoelectric semiconductors, whose structure of polyhedron stacks is very attractive. However, their mechanical properties have not yet met the requirements of industrial applications. Here, we report the ideal strength of element-substituted type-I and type-VIII clathrates and the shear deformation mechanism by using density functional theory. The results show that the framework element is the determinant of the intrinsic mechanical properties of the clathrates and is affected by sequential weakening of Si-Ge-Sn. The highest ideal shear strength is 8.71 GPa for I-Ba8Au6Si40 along the (110)/[001] slip system, which is attributed to the formation of higher-energy Si-Si covalent bonds. Meanwhile, the ideal shear strength of Ba-filled I/VIII clathrates (4.51/2.65 GPa) is higher than that of Sr-filled clathrates (3.64 GPa/1.91 GPa). In addition, the strength and ultimate strain of VIII-Ba8Ga16Sn30 can be significantly increased by the structural coordination accommodating with the stiffness of the Ga-Ge bond to achieve simultaneous bond breaking. Our findings demonstrate that the element substitution strategy is an effective approach for designing highly robust clathrates.

3.
Small ; 20(27): e2310692, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38243875

RESUMEN

Multiscale defects engineering offers a promising strategy for synergistically enhancing the thermoelectric and mechanical properties of thermoelectric semiconductors. However, the specific impact of individual defects, in particular precipitation, on mechanical properties remains ambiguous. In this work, the mechanical and thermoelectric properties of Sn1.03- xMnxTe (x = 0-0.30) semiconductors are systematically studied. Mn-alloying induces dense dislocations and Mn nano-precipitates, resulting in an enhanced compressive strength with x increased to 0.15. Quantitative calculations are performed to assess the strengthening contributions including grain boundary, solid solution, dislocation, and precipitation strengthening. Due to the dominant contribution of precipitation strengthening, the yield strength of the x = 0.10 sample is improved by ≈74.5% in comparison to the Mn-free Sn1.03Te. For x ≥ 0.15, numerous MnTe precipitates lead to a synergistic enhancement of strength-ductility. In addition, multiscale defects induced by Mn alloying can scatter phonons over a wide frequency spectrum. The peak figure of merit ZT of ≈1.3 and an ultralow lattice thermal conductivity of ≈0.35 Wm-1 K-1 are obtained at 873 K for x = 0.10 and x = 0.30 samples respectively. This work reveals tha precipitation evolution optimizes the mechanical and thermoelectric properties of Sn1.03- xMnxTe semiconductors, which may hold potential implications for other thermoelectric systems.

4.
J Colloid Interface Sci ; 657: 870-879, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38091910

RESUMEN

The development of efficient and stable electrocatalysts for hydrogen evolution reaction (HER) is impending for the advancement of water-splitting. In this study, we developed a novel electrocatalyst consisting of highly dispersed Ru nanoclusters ameliorated by cobalt single atoms and N, S co-doped reduced graphene oxide (CoSARuNC@NSG). Benefitted from the optimized electronic structure of the Ru nanoclusters induced by the adjacent single atomic Co and N, S co-doped RGO support, the electrocatalyst exhibits exceptional HER performance with overpotentials of 15 mV and 74 mV for achieving a current density of 10 mA cm-2 in alkaline and acidic water. The catalyst outperforms most noble metal-based HER electrocatalysts. Furthermore, the electrolyzer assembled with CoSARuNC@NSG and RuO2 demonstrated an overall voltage of 1.56 V at 10 mA cm-2 and an excellent operational stability for over 25 h with almost no attenuation. Theoretical calculations also deduce its high HER activity demonstrated by the smaller reaction energy barrier due to the optimized electronic structure of Ru nanoclusters. This strategy involving the regulation of metal nanoparticles activity through flexible single atom and GO support could provide valuable insights into the design of high-performance and low-cost HER catalysts.

5.
Nat Nanotechnol ; 18(11): 1281-1288, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37500776

RESUMEN

Room-temperature bismuth telluride (Bi2Te3) thermoelectrics are promising candidates for low-grade heat harvesting. However, the brittleness and inflexibility of Bi2Te3 are far reaching and bring about lifelong drawbacks. Here we demonstrate good pliability over 1,000 bending cycles and high power factors of 4.2 (p type) and 4.6 (n type) mW m-1 K-2 in Bi2Te3-based films that were exfoliated from corresponding single crystals. This unprecedented bendability was ascribed to the in situ observed staggered-layer structure that was spontaneously formed during the fabrication to promote stress propagation whilst maintaining good electrical conductivity. Unexpectedly, the donor-like staggered layer rarely affected the carrier transport of the films, thus maintaining its superior thermoelectric performance. Our flexible generator showed a high normalized power density of 321 W m-2 with a temperature difference of 60 K. These high performances in supple thermoelectric films not only offer useful paradigms for wearable electronics, but also provide key insights into structure-property manipulation in inorganic semiconductors.

6.
Nanomaterials (Basel) ; 12(12)2022 Jun 20.
Artículo en Inglés | MEDLINE | ID: mdl-35745452

RESUMEN

Emerging high-entropy alloy (HEA) films achieve high strength but generally show ineludible brittle fractures, strongly restricting their micro/nano-mechanical and functional applications. Nanolayered (NL) CoCrFeNi/graphene composites are elaborately fabricated via magnetron sputtering and the transfer process. It is uncovered that NL CoCrFeNi/graphene composite pillars exhibit a simultaneous ultra-high strength of 4.73 GPa and considerable compressive plasticity of over 20%. Detailed electron microscope observations and simulations reveal that the monolayer graphene interface can effectively block the crack propagation and stimulate dislocations to accommodate further deformation. Our findings open avenues for the fabrication of high-performance, HEA-based composites, thereby addressing the challenges and unmet needs in flexible electronics and mechanical metamaterials.

7.
ACS Appl Mater Interfaces ; 14(3): 4326-4334, 2022 Jan 26.
Artículo en Inglés | MEDLINE | ID: mdl-35018776

RESUMEN

Type-I clathrate Ba8Au6Ge40, possessing an interesting structure stacked by polyhedrons, is a potential "phonon-glass, electron-crystal" thermoelectric material. However, the mechanical properties of Ba8Au6Ge40 vital for industrial applications have not been clarified. Here, we report the first density functional theory calculations of the intrinsic mechanical properties of thermoelectric clathrate Ba8Au6Ge40. Among the different loading directions, the {110}/⟨001⟩ shearing and ⟨110⟩ tension are the weakest, with strengths of 4.51 and 6.64 GPa, respectively. Under {110}/⟨001⟩ shearing, the Ge-Ge bonds undergo significant stretching and twisting, leading to a severe distortion of the tetrakaidecahedral cage, giving rise to the fast softening of the flank Au-Ge bonds. At a strain of 0.2655, the Au-Ge bonds suddenly break, resulting in the collapse of the cage and the failure of the material. Under a ⟨110⟩ tension, the stretching of the Ge-Ge bonds keeps accelerating the softening of the Au-Ge bonds in the top/bottom hexagons, which releases the stress and disables the structure. The Au-Ge bonds are more rigid, contributing two-thirds of the structural deformation resistance. This work provides a new insight to understand the failure mechanisms of type-I clathrates with varied framework constitutions, which should help inform the design of robust thermoelectric clathrate materials.

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