This paper reveals the ordered structure and composition effect to electrochemical catalytic activity towards oxygen reduction reaction (ORR) of ternary metallic Pt-Co-Cu/C catalysts. Bimetallic Pt-Co alloy nanoparticles (NPs) represent an emerging class of electrocatalysts for ORR, but practical applications, e.g. in fuel cells, have been hindered by low catalytic performances owning to crystal phase and atomic composition. Cu is introduced into Pt-Co/C lattices to form PtCoxCu1−x/C (x=0.25, 0.5 and 0.75) ternary-face-centered tetragonal (fct) ordered ternary metallic NPs. The chemically ordered Pt-Co-Cu/C catalysts exhibit excellent performance of 1.31 A mg-1 Pt in mass activity and 0.59 A cm-2 Pt in specific activity which are significantly higher than Pt-Co/C and commercial Johnson Matthey (JM) Pt/C catalysts, because of the ordered crystal phase and composition control modified the Pt-Pt atoms distance and the surface electronic properties. The presence of Cu improves the surface electronic structure, as well as enhances the stability of catalysts.
The phase state of nanoparticles plays a pivotal role in regulating the electronic structure of Pd to enhance the catalytic performance and durability for the oxygen reduction reaction (ORR). To elucidate the correlation of the electronic structure with activity, a series of body‐centered cubic (bcc) PdCu/C, PdCuFe/C, and PdCuCo/C intermetallic compounds were fabricated by using an impregnation reduction method followed by annealing. The results of rotating disk electrode studies show that the structurally ordered PdCuFe/C nanoparticles exhibit a much larger increase in mass activity (0.08 A mgPd−1), about 2.1 and 5 times higher than ordered PdCuCo/C and PdCu/C, respectively. More importantly, the maximum power density of the ordered PdCuFe/C was 267 mW cm−2 in proton exchange membrane fuel cells. The X‐ray photoelectron spectroscopy results revealed that that the addition of Fe into PdCu/C can efficiently regulate the electronic structure of Pd in optimizing the oxygen binding energy for the ORR. Our work provides a general approach to enhance Pd‐based ternary alloy catalysts with Pt‐like catalytic activity for fuel cell applications.
A tandem
Michael addition–cyclization of nitroalkenes with 1,3-dicarbonyl
compounds was developed using phase transfer catalyst (PTC), allowing
for the synthesis of polysubstituted-[4,5]-dihydrofuran in high yields.
A wide range of substrates were demonstrated by this one-step process.
Meanwhile, nitro group was substituted to form corresponding nitrite
ion detected in the aqueous phase providing a reasonable pathway for
denitrating poisonous and explosive nitro-containing compounds. The
proposed mechanism was also supported by our DFT calculations.
A highly efficient melamine/BH 3 H 2 evolution system, which can spontaneously release 6 equiv of H 2 from 1 equiv of melamine at room temperature and is capable of releasing further 3 equiv of H 2 at higher temperatures, has been developed. The dehydrogenation reaction was verified and studied by 1 H and 11 B NMR, MALDI-TOF MS analyses, as well as H 2 evolution experiments, under different conditions. The reaction products were characterized by elemental analyses, IR, and solid 11 B NMR spectroscopic techniques. Studies on the dehydrogenation reaction of BH 3 with a model compound oaminopyridine provide solid experimental evidence for further confirming the spontaneous NH/BH dehydrocoupling reaction.
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