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1.
Environ Res ; 229: 115950, 2023 07 15.
Artigo em Inglês | MEDLINE | ID: mdl-37084945

RESUMO

Engineering high-performance electrocatalysts to improve the kinetics of parallel electrochemical reactions in low-temperature fuel cells, water splitting, and metal-air battery applications is important and inevitable. In this study, by employing a chemical co-reduction method, we developed multifunctional Pt3Rh-Co3O4 alloy with uniformly distributed ultrafine nanoparticles (2-3 nm), supported on carbon. The presence of Co3O4 and the incorporation of Rh led to a strong electronic and ligand effect in the Pt lattice environment, which caused the d-band center of Pt to shift. This shift improved the electrocatalytic performance of Pt3Rh-Co3O4 alloy. When Pt3Rh-Co3O4/C was used to catalyze the oxygen reduction reaction (E1/2: 0.75 V), oxygen evolution reaction (η10: 290 mV), and hydrogen evolution reaction (η10: 55 mV), it showed greater endurance (mass activity loss of only 7%-17%) than Pt-Co3O4/C and Pt/C catalysts up to 5000 potential cycles in perchloric acid. Overall, the as-prepared Pt3Rh-Co3O4/C showed high multifunctional electrocatalytic potency, as demonstrated by typical electrochemical studies, and its physicochemical properties endorse their extended performance for a wide range of energy storage and conversion applications.


Assuntos
Ligas , Nanopartículas , Carbono , Oxigênio
2.
J Colloid Interface Sci ; 629(Pt B): 357-369, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36162393

RESUMO

A hybrid catalyst support anchoring a noble metal catalyst could be a promising material for building interfacial bonding between metallic nanostructures and polymer functionalized carbon supports to improve the kinetics of oxygen reduction reaction (ORR). This study successfully prepared a polyhedron nanostructured Pd and MoO2-embedded polyaniline-functionalized graphitized carbon nitride (PANI-g-C3N4) surface using a chemical reduction method. The Pd-Mo/PANI-g-C3N4 achieved an ORR activity of 0.27 mA µg-1 and 1.14 mA cm-2 at 0.85 V, which were 4.5 times higher than those of commercial 20% Pt/C catalyst (0.06 mA µg-1 and 0.14 mA cm-2). In addition, the Pd-Mo/PANI-g-C3N4 retained âˆ¼ 77.5% of its initial mass activity after 10,000 cycles, with only 30 mV half-wave potential reduction. Further, the engineered potential active sites in the catalyst material verified the significant improvement in the ORR activity of the catalyst with increased life-time, and theoretical calculations revealed that the synergistic effect of the catalytic components enhanced the ORR kinetics of the active sites.

3.
J Colloid Interface Sci ; 608(Pt 1): 207-218, 2022 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-34626967

RESUMO

An efficient oxygen bifunctional catalyst Pt-Ru-Ir with ordered mesoporous nanostructures (OMNs) was successfully synthesized by chemical reduction using KIT-6 mesoporous silica as a template. The crystallographic behavior, electronic effects, and microstructure of the catalysts were investigated by XRD, XPS, SEM, and TEM analysis. The influence of OMNs and the effect of Ir content in Pt-Ru-Ir catalyst on both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) were investigated. The synergistic and electronic effects play an important role in electrocatalytic performance through the electronic coupling between Pt, Ru and Ir followed by the alloy formation with different lattice strain percentages. Amongst, the OMNs Pt70Ru25Ir5 catalyst exhibits the highest mass activity of 0.21 mA µg-1 and specific activity of 0.33 mA cm-2 for ORR, which are nearly 5-fold greater than those for benchmark Pt/C catalyst. Furthermore, the Pt70Ru25Ir5 demonstrated enhanced OER activity with an overpotential of 470 mV at 10 mA cm-2, an onset potential of 1.70 V, and a Tafel slope of 118 mV dec-1, outperforming commercial IrO2. In addition, the durability of the Pt70Ru25Ir5 catalyst for ORR and OER are found to be extended in comparison with that of other catalysts reported in this work after 6000 cycles. These results demonstrate that the ordered OMNs Pt-Ru-Ir with low Ir content (∼5 wt%) could be a promising oxygen bifunctional catalyst for electrochemical energy conversion and storage applications.

4.
J Colloid Interface Sci ; 598: 126-135, 2021 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-33895534

RESUMO

Pt-based alloy nanomaterials with nanodendrites (NDs) structures are efficient electrocatalysts for methanol oxidation reaction (MOR), however their durability is greatly limited by the issue of transition metals dissolution. In this work, a facile trace Ir-doping strategy was proposed to fabricate Ir-PtZn and Ir-PtCu alloy NDs catalysts in aqueous medium, which significantly improved the electrocatalytic activity and durability for MOR. The as-prepared Ir-PtZn/Cu NDs catalysts showed distinct dendrites structures with the averaged diameter of 4.1 nm, and trace Ir doping subsequently improved the utilization of Pt atoms and promoted the oxidation efficiency of methanol. The electrochemical characterizations further demonstrated that the obtained Ir-PtZn/Cu NDs possessed enhanced mass activities of nearly 1.23 and 1.28-fold higher than those of undoped PtZn and PtCu, and approximately 2.35 and 2.67-fold higher than that of Pt/C in acid medium. More excitingly, after long-term durability test, the proposed Ir-PtZn and Ir-PtCu NDs still retained about 88.9% and 91.6% of its initial mass activities, which further highlights the key role of Ir-doping in determining catalyst performance. This work suggests that trace Ir-doping engineering could be a promising way to develop advanced electrocatalysts toward MOR for direct methanol fuel cell (DMFC) applications.

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