Abstract

Direct formation of ultra-small nanoparticles on carbon supports by rapid high temperature synthesis method offers new opportunities for scalable nanomanufacturing and the synthesis of stable multi-elemental nanoparticles. However, the underlying mechanisms affecting the dispersion and stability of nanoparticles on the supports during high temperature processing remain enigmatic. In this work, we report the observation of metallic nanoparticles formation and stabilization on carbon supports through in situ Joule heating method. We find that the formation of metallic nanoparticles is associated with the simultaneous phase transition of amorphous carbon to a highly defective turbostratic graphite (T-graphite). Molecular dynamic (MD) simulations suggest that the defective T-graphite provide numerous nucleation sites for the nanoparticles to form. Furthermore, the nanoparticles partially intercalate and take root on edge planes, leading to high binding energy on support. This interaction between nanoparticles and T-graphite substrate strengthens the anchoring and provides excellent thermal stability to the nanoparticles. These findings provide mechanistic understanding of rapid high temperature synthesis of metal nanoparticles on carbon supports and the origin of their stability.

Highlights

  • Direct formation of ultra-small nanoparticles on carbon supports by rapid high temperature synthesis method offers new opportunities for scalable nanomanufacturing and the synthesis of stable multi-elemental nanoparticles

  • Through high resolution transmission electron microscopy (TEM) (HRTEM) and atomistic simulations, we find that the defective edge planes are the preferred sites for the formation and stabilization of metal nanoparticles

  • The morphological changes in the S-carbon nanofibers (CNFs) due to Joule heating is visualized in the form of a series of bright field TEM images and Movie S1

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Summary

Introduction

Direct formation of ultra-small nanoparticles on carbon supports by rapid high temperature synthesis method offers new opportunities for scalable nanomanufacturing and the synthesis of stable multi-elemental nanoparticles. The nanoparticles partially intercalate and take root on edge planes, leading to high binding energy on support This interaction between nanoparticles and T-graphite substrate strengthens the anchoring and provides excellent thermal stability to the nanoparticles. We reported a fast, high temperature, and dry synthesis method based on rapid Joule heating of a carbon matrix loaded with metal salt precursors (carbothermal shock)[20]. This process generates extremely high temperature (>1500 K) to thermally decompose the loaded salt precursors to metallic nanoparticles[20,21,22]. We believe the mechanistic details reported in this work would guide the nanoparticles synthesis through Joule heatingbased methods, and pave the way on understanding other rapid high temperature synthesis approaches

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