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1.
Article in English | MEDLINE | ID: mdl-38606549

ABSTRACT

PtRu alloys have been recognized as the state-of-the-art catalysts for the methanol oxidation reaction (MOR) in direct methanol fuel cells (DMFCs). However, their applications in DMFCs are still less efficient in terms of both catalytic activity and durability. Rare earth (RE) metals have been recognized as attractive elements to tune the catalytic activity, while it is still a world-class challenge to synthesize well-dispersed Pt-RE alloys. Herein, we developed a novel hydrogen-assisted magnesiothermic reduction strategy to prepare a highly dispersed carbon-supported lutetium-doped PtRu catalyst with ultrafine nanoclusters and atomically dispersed Ru sites. The PtRuLu catalyst shows an outstanding high electrochemical surface area (ECSA) of 239.0 m2 gPt-1 and delivers an optimized MOR mass activity and specific activity of 632.5 mA mgPt-1 and 26 A cmPt-2 at 0.4 V vs saturated calomel electrode (SCE), which are 3.6 and 3.5 times of commercial PtRu-JM and an order higher than PtLu, respectively. These novel catalysts have been demonstrated in a high-temperature direct methanol fuel cell running in a temperature range of 180-240 °C, achieving a maximum power density of 314.3 mW cm-2. The AC-STEM imaging, in situ ATR-IR spectroscopy, and DFT calculations disclose that the high performance is resulted from the highly dispersed PtRuLu nanoclusters and the synergistic effect of the atomically dispersed Ru sites with PtRuLu nanoclusters, which significantly reduces the CO* intermediates coverage due to the promoted water activation to form the OH* to facilitate the CO* removal.

2.
Angew Chem Int Ed Engl ; 61(52): e202215866, 2022 Dec 23.
Article in English | MEDLINE | ID: mdl-36333270

ABSTRACT

Concentration of electrolyte has significant effects on performances of rechargeable batteries. Previous studies mainly focused on concentrated electrolytes. So far, only several recipes on low-concentration electrolytes were studied, performing enhanced performance in advanced rechargeable batteries. Here, based on common electrolyte components, a low-concentration electrolyte composed of 0.2 M lithium hexafluorophosphate (LiPF6 ) solvated in fluoroethylene carbonate (FEC) and ethyl methyl carbonate (EMC) is employed for high-voltage Li metal battery. The synergistic working mechanisms of introducing fluorine-containing solvent in the solvated structure and low salt concentration effect are revealed, resulting in LiF-rich, uniform, and robust solid electrolyte interphase layer and fewer unfavorable decomposition products. As a result, this low-concentration electrolyte significantly enhances electrochemical performances of Li||Li symmetric cells and high-voltage LiCoO2 ||Li batteries.

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