Abstract
Despite being studied for nearly 50 years, smallest chemically stable moieties in the metallic glass (MG) could not be found experimentally. Herein, we demonstrate a novel experimental approach based on electrochemical etching of amorphous alloys in inert solvent (acetonitrile) in the presence of a high voltage (1 kV) followed by detection of the ions using electrolytic spray ionization mass spectrometry (ESI MS). The experiment shows stable signals corresponding to Pd, PdSi and PdSi2 ions, which emerges due to the electrochemical etching of the Pd80Si20 metallic glass electrode. These fragments are observed from the controlled dissolution of the Pd80Si20 melt-spun ribbon (MSR) electrode. Annealed electrode releases different fragments in the same experimental condition. These specific species are expected to be the smallest and most stable chemical units from the metallic glass which survived the chemical dissolution and complexation (with acetonitrile) process. Theoretically, these units can be produced from the cluster based models for the MG. Similar treatment on Pd40Ni40P20 MSR resulted several complex peaks consisting of Pd, Ni and P in various combinations suggesting this can be adopted for any metal-metalloid glass.
Highlights
Despite being studied for nearly 50 years, smallest chemically stable moieties in the metallic glass (MG) could not be found experimentally
In search of the most stable configuration in metal-metalloid type metallic glasses, we introduce a novel method to visualize the chemical building blocks of single phase complex amorphous materials using a combination of accessible mass spectrometry (MS) supported by Raman spectroscopy
In electrolytic spray ionization mass spectrometry, metals are electrochemically etched with acetonitrile (ACN) in the presence of a high voltage
Summary
Despite being studied for nearly 50 years, smallest chemically stable moieties in the metallic glass (MG) could not be found experimentally. The amorphous structure of metallic glasses with similar compositions that exhibit only short- and medium range order results in maze-like pattern in high resolution transmission electron microscopy (TEM) without any discernible microstructural information[1,2,3] In view of their distinct physical and chemical properties, metallic glasses have gained popularity in several scientific disciplines. In a process known as “Electrolytic Spray”, which is a fairly recent technique, introduced and described by Cooks and co-workers, electrospray ionization is employed to form ions for further characterization[23,24] We have adopted this technique to determine the immediate local chemical bonds among the constituents of a metallic glass. The combination of two techniques (mass spectrometry and Raman spectroscopy) can be employed to determine the bonding and the active constituents, which are responsible for the stabilization of the amorphous phase in the model systems Pd80Si20 and Pd40Ni40P20
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