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1.
Inorg Chem ; 61(31): 12466-12472, 2022 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-35894934

RESUMO

Pd-based catalysts are attractive anodic electrocatalysts for direct methanol fuel cells owing to their low cost and natural abundance. However, they suffer from sluggish reaction kinetic and insufficient electroactivity in methanol oxidation reaction (MOR). In this work, we developed a facile one-pot approach to fabricate low Pt-doped Pd12P3.2 nanowires with crystalline/amorphous heterophase (termed Pt-Pd12P3.2 NWs) for MOR. The unique crystalline/amorphous heterophase structures promote the catalytic activity by the plentiful active sites at the phase boundaries and/or interfaces and the synergistic effect between different phases. Moreover, the incorporation of trace Pt into Pd lattices modifies the electronic structure and improves the electron transfer ability. Therefore, the obtained Pt-Pd12P3.2 NWs display significantly enhanced electrocatalytic performance toward MOR with the mass activity of 2.35 A mgPd+Pt-1, which is 9.0, 2.9, and 2.0 times higher than those of the commercial Pd/C (0.26 A mgPd-1), Pd12P3.2 NWs (0.82 A mgPd-1), and commercial Pt/C (1.19 A mgPt-1). The high mass activity enables the Pt-Pd12P3.2 NWs to be the promising Pd-based catalysts for MOR.

2.
Inorg Chem ; 61(5): 2612-2618, 2022 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-35060700

RESUMO

A key challenge for direct methanol fuel cells is the sluggish reaction kinetics, poor anti-CO poisoning ability, and insufficient Pt utilization of platinum-based catalysts during methanol oxidation reaction (MOR). Herein, we report a facile approach for PtCuNi electrocatalysts with adjustable inner and surface configurations. By judiciously controlling the nucleation/growth kinetics, PtCuNi core-shell alloy nanoparticles (PtCuNi-CS NPs) fortified with a Cu-rich core and a Pt-rich shell are obtained. Especially, PtCuNi-CS NPs show the highest mass activity and specific activity toward MOR, 5.7 and 5.1 times higher than those of commercial Pt/C. Density functional theory calculations reveal that the PtCuNi-CS NPs with a suitable d-band center possess excellent electro-oxidation activity. Additionally, the doping of Cu and Ni atoms endows the PtCuNi-CS NPs with enhanced OH* adsorption. This work provides an effective design strategy to develop Pt-based trimetallic electrocatalysts as efficient anode materials for fuel cell applications.

3.
Soft Matter ; 16(7): 1840-1849, 2020 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-31971198

RESUMO

Combining a hydrophobic interaction crosslinked curdlan as the first network and hydrophobic interaction crosslinked polyacrylamide as the second network, we have fabricated a curdlan/HPAAm double network (DN) hydrogel using a one-pot method. The resulting DN hydrogel exhibited good mechanical properties, i.e. an elastic modulus of 103 kPa, a tensile fracture strength of 0.81 MPa, a tensile stretch of 25.3 and a compressive stress of 62.5 MPa when the compressive strain increased up to 99%. The DN gel could withstand ten compression tests under 90% compressive strain without observable damage. The DN gel demonstrated 84% stiffness recovery and 97% toughness recovery after the deformed samples were relaxed and stored at 95 °C for 4 h. The stiffness and fracture stress of the DN gel were enhanced after sterilization treatment at 120 °C. Furthermore, the gels exhibited 52% self-healing of fracture stretch after the samples were cut and brought into contact at 95 °C for 4 h. The self-recovery and self-healing properties of the DN gel both originated from the first curdlan network via the reformation of hydrophobic interactions and the second HPAAm network via reformation of the broken hydrophobic associations.

4.
Chem Commun (Camb) ; 58(74): 10376-10379, 2022 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-36017783

RESUMO

PdCoP nanoparticles (PdCoP NPs) with nanopore structures were synthesized by a facile one-pot solvothermal approach. Due to their unique geometric structures and the electronic and synergistic effects among multiple components, the optimized PdCoP NPs (PdCoP-NPs-1) show superior mass activity (5.97 A mgPd-1) for the ethanol oxidation reaction under alkaline conditions.


Assuntos
Nanopartículas , Nanoporos , Catálise , Etanol/química , Oxirredução
5.
Dalton Trans ; 50(32): 11099-11105, 2021 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-34318845

RESUMO

Hydrogen is a promising substitute for non-renewable fossil fuels. Producing hydrogen fuel by electrolyzing water is an effective strategy to address the growing environmental problems. Platinum (Pt) is still the most active electrocatalyst to catalyze the hydrogen evolution reaction (HER) in alkaline media. Herein, we demonstrate that ultrafine candied haws-shaped PtWNi nanoalloys modified with the Ni species (Nin+) could be formed in the alkaline electroactivation process of PtWNi alloys. Notably, the Ni species (Nin+) promoted the decomposition of water and produced hydrogen intermediates, which were then immediately adsorbed on the surface of Pt and recombined into molecular hydrogen. Moreover, these hydrogen intermediates also enhanced the instability of the HO-H bond, leading to an increase in the total activity.

6.
Chem Asian J ; 15(11): 1736-1742, 2020 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-32338434

RESUMO

Surfactants or capping agents are usually employed to control the shapes and sizes of metal nanowires (NWs). Polyvinylpyrrolidone (PVP) and oleylamine (OAm) are the most common capping agents used in the synthesis of metal nanowires. However, these capping agents bind strongly onto the surface of the nanowires and severely prevent the reactant molecules from entering the active sites. In the present research, a facile acetic acid/NaBH4 treatment technology is reported to effectively remove PVP and OAm from the surface of the co-doped Pt NWs. Interestingly, the morphology of poor crystalline platinum nanowires treated with NaBH4 solution is transformed into nanowire networks (NWNs) with higher crystallinity. Furthermore, in comparison with the commercial Pt/C catalyst, the catalytic activity of co-doped Pt NWNs with clean surfaces shows improvements of up to 4.1 times for mass activity and 5.1 times for specific activity, respectively.

7.
Nanoscale ; 7(43): 18278-83, 2015 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-26486194

RESUMO

We report the X-ray crystallographic structure of an 18-metal atom Au-Ag bimetallic nanocluster (NC) formulated as [Au15Ag3(SC6H11)14]. This NC consists of a Au6Ag3 bi-octahedral kernel, which is built up by two octahedral Au3Ag3 units through sharing one Ag3 triangular face. The [Au15Ag3(SC6H11)14] can be viewed as a core-shell structure with the doped Ag atoms as the core and Au atoms as the shell. Detailed analyses by UV-vis spectroscopy, X-ray photoelectron spectroscopy (XPS), and electrochemical measurements clearly show distinct differences in the electronic structure between [Au15Ag3(SC6H11)14] and the homometal [Au18(SC6H11)14] NC. This study contributes to the deep understanding on bimetallic nanoclusters.

8.
J Am Chem Soc ; 126(19): 5976-7, 2004 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-15137757

RESUMO

Eu2O3 nanotubes have been successfully fabricated by an improved sol-gel template method within the nanochannels of porous anodic alumina templates. The morphology, structure, and composition of the nanotubes were characterized by means of X-ray diffraction techniques, scanning electron microscope, transmission electron microscopy, and selected-area electron diffraction. The results show that the Eu2O3 nanotubes are polycrystalline with a cubic structure. The outer diameter of nanotubes is 50-80 nm, and the thickness of the tube wall is about 5 nm. The mechanism of nanotube formation was discussed.

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