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Facile Synthesis of Quaternary Structurally Ordered L12-Pt(Fe, Co, Ni)3 Nanoparticles with Low Content of Platinum as Efficient Oxygen Reduction Reaction Electrocatalysts.

ABSTRACT: Synthesis of electrocatalysts for oxygen reduction reaction (ORR) with not only prominent electrocatalytic performance but also a low amount of Pt is the urgent challenge in the popularization of fuel cells. In this work, through a facile synthetic strategy of spray dehydration on a solid surface and annealing process, we demonstrate the first manufacture of quaternary structurally ordered PtM3 (M = transition metal) intermetallic nanoparticles (NPs), Pt(Fe, Co, Ni)3, in order to lower the content of Pt. The atomic contents of Pt, Fe, Co, and Ni are equal and the chemical structure of Pt(Fe, Co, Ni)3 is a cubic L12-ordered structure. L12-Pt(Fe, Co, Ni)3/C electrocatalysts exhibit enhanced electrocatalytic performance toward ORR with mass activity (MA) 6.6 times higher than the commercial Pt/C and a minimal loss of 17% in MA and 1.5% loss in specific activity (SA) after 10?000 potential cycles at 0.9 V. Furthermore, the stability behavior is confirmed to be attributed to the coaction of particle sizes and the ordering effect. Compared with traditional Pt-based electrocatalysts in the stoichiometric forms of Pt3M and PtM, L12-Pt(Fe, Co, Ni)3 intermetallic NPs exhibit excellent performance and higher cost effectiveness. Moreover, this work also proposes a facile and effective synthetic strategy for manufacturing multicomponent Pt-based electrocatalysts for ORR.

SUBMITTER: Wang S

PROVIDER: S-EPMC6822218 | biostudies-literature | 2019 Oct

REPOSITORIES: biostudies-literature

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Facile Synthesis of Quaternary Structurally Ordered L12-Pt(Fe, Co, Ni)3 Nanoparticles with Low Content of Platinum as Efficient Oxygen Reduction Reaction Electrocatalysts.

Wang Sihao S Luo Qingyu Q Zhu Yingfang Y Tang Shaolong S Du Youwei Y

ACS omega 20191016 18

Synthesis of electrocatalysts for oxygen reduction reaction (ORR) with not only prominent electrocatalytic performance but also a low amount of Pt is the urgent challenge in the popularization of fuel cells. In this work, through a facile synthetic strategy of spray dehydration on a solid surface and annealing process, we demonstrate the first manufacture of quaternary structurally ordered PtM3 (M = transition metal) intermetallic nanoparticles (NPs), Pt(Fe, Co, Ni)3, in or ...[more]

PMID: 31681899

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Project description:Metal-organic frameworks (MOFs) have been investigated with regard to the oxygen evolution reaction (OER) due to their structure diversity, high specific surface area, adjustable pore size, and abundant active sites. However, the poor conductivity of most MOFs restricts this application. Herein, through a facile one-step solvothermal method, the Ni-based pillared metal-organic framework [Ni2(BDC)2DABCO] (BDC = 1,4-benzenedicarboxylate, DABCO = 1,4-diazabicyclo[2.2.2]octane), its bimetallic nickel-iron form [Ni(Fe)(BDC)2DABCO], and their modified Ketjenblack (mKB) composites were synthesized and tested toward OER in an alkaline medium (KOH 1 mol L-1). A synergistic effect of the bimetallic nickel-iron MOF and the conductive mKB additive enhanced the catalytic activity of the MOF/mKB composites. All MOF/mKB composite samples (7, 14, 22, and 34 wt.% mKB) indicated much higher OER performances than the MOFs and mKB alone. The Ni-MOF/mKB14 composite (14 wt.% of mKB) demonstrated an overpotential of 294 mV at a current density of 10 mA cm-2 and a Tafel slope of 32 mV dec-1, which is comparable with commercial RuO2, commonly used as a benchmark material for OER. The catalytic performance of Ni(Fe)MOF/mKB14 (0.57 wt.% Fe) was further improved to an overpotential of 279 mV at a current density of 10 mA cm-2. The low Tafel slope of 25 mV dec-1 as well as a low reaction resistance due to the electrochemical impedance spectroscopy (EIS) measurement confirmed the excellent OER performance of the Ni(Fe)MOF/mKB14 composite. For practical applications, the Ni(Fe)MOF/mKB14 electrocatalyst was impregnated into commercial nickel foam (NF), where overpotentials of 247 and 291 mV at current densities of 10 and 50 mA cm-2, respectively, were realized. The activity was maintained for 30 h at the applied current density of 50 mA cm-2. More importantly, this work adds to the fundamental understanding of the in situ transformation of Ni(Fe)DMOF into OER-active α/β-Ni(OH)2, β/γ-NiOOH, and FeOOH with residual porosity inherited from the MOF structure, as seen by powder X-ray diffractometry and N2 sorption analysis. Benefitting from the porosity structure of the MOF precursor, the nickel-iron catalysts outperformed the solely Ni-based catalysts due to their synergistic effects and exhibited superior catalytic activity and long-term stability in OER. In addition, by introducing mKB as a conductive carbon additive in the MOF structure, a homogeneous conductive network was constructed to improve the electronic conductivity of the MOF/mKB composites. The electrocatalytic system consisting of earth-abundant Ni and Fe metals only is attractive for the development of efficient, practical, and economical energy conversion materials for efficient OER activity.

Dataset Information

Facile Synthesis of Quaternary Structurally Ordered L12-Pt(Fe, Co, Ni)3 Nanoparticles with Low Content of Platinum as Efficient Oxygen Reduction Reaction Electrocatalysts.

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Facile Synthesis of Quaternary Structurally Ordered L1<sub>2</sub>-Pt(Fe, Co, Ni)<sub>3</sub> Nanoparticles with Low Content of Platinum as Efficient Oxygen Reduction Reaction Electrocatalysts.

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