This corrosion: Octahedral Pt-Ni alloy nanoparticles (NPs) are converted into concave Pt(3)Ni NPs by a coordination-assisted chemical-etching process. The corroded concave Pt-Ni NPs have a higher density of low-coordinate atoms in steps sites, a decisive property in heterogeneous catalysis.
Resistive switching effect in conductor/insulator/conductor thin-film stacks is promising for resistance random access memory with high-density, fast speed, low power dissipation and high endurance, as well as novel computer logic architectures. NiO is a model system for the resistive switching effect and the formation/rupture of Ni nanofilaments is considered to be essential. However, it is not clear how the nanofilaments evolve in the switching process. Moreover, since Ni nanofilaments should be ferromagnetic, it provides an opportunity to explore the electromagnetic coupling in this system. Here, we report a direct observation of Ni nanofilaments and their specific evolution process for the first time by a combination of various measurements and theoretical calculations. We found that multi-nanofilaments are involved in the low resistance state and the nanofilaments become thin and rupture separately in the RESET process with subsequent increase of the rupture gaps. Theoretical calculations reveal the role of oxygen vacancy amount in the evolution of Ni nanofilaments. We also demonstrate electromagnetic coupling in this system, which opens a new avenue for multifunctional devices.
Silver−copper (AgCu) bimetallic catalysts hold great potential for electrochemical carbon dioxide reduction reaction (CO 2 RR), which is a promising way to realize the goal of carbon neutrality. Although a wide variety of AgCu catalysts have been developed so far, it is relatively less explored how these AgCu catalysts evolve during CO 2 RR. The absence of insights into their stability makes the dynamic catalytic sites elusive and hampers the design of AgCu catalysts in a rational manner. Here, we synthesized intermixed and phase-separated AgCu nanoparticles on carbon paper electrodes and investigated their evolution behavior in CO 2 RR. Our time-sequential electron microscopy and elemental mapping studies show that Cu possesses high mobility in AgCu under CO 2 RR conditions, which can leach out from the catalysts by migrating to the bimetallic catalyst surface, detaching from the catalysts, and agglomerating as new particles. Besides, Ag and Cu manifest a trend to phase-separate into Cu-rich and Ag-rich grains, regardless of the starting catalyst structure. The composition of the Cu-rich and Ag-rich grains diverges during the reaction and eventually approaches thermodynamic values, i.e., Ag 0.88 Cu 0.12 and Ag 0.05 Cu 0.95 . The separation between Ag and Cu has been observed in the bulk and on the surface of the catalysts, highlighting the importance of AgCu phase boundaries for CO 2 RR. In addition, an operando high-energy-resolution X-ray absorption spectroscopy study confirms the metallic state of Cu in AgCu as the catalytically active sites during CO 2 RR. Taken together, this work provides a comprehensive understanding of the chemical and structural evolution behavior of AgCu catalysts in CO 2 RR.
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