Compositional distribution, strain, and defects in alloy nanoparticles significantly affect the catalytic properties for a wide range of applications such as gas reforming, fuel cells, electrolysis, etc. while various alloy compositions of nanoparticles have been investigated to improve performance and reduce the amount of precious metals used. It was reported that the composition distribution of the alloy particles, expectedly homogeneous in the whole particle, changed dynamically depending on the operating environment, resulting in altering the catalytic activity [1]. Furthermore, defects such as dislocations, grain boundaries, and elastic strain of the crystalline lattice also significantly affect catalytic properties. Since these factors dynamically change and evolve under operating environments, in situ measurements are essential to reveal these factors and ultimately to exploit them to enhance the catalytic properties. Bragg coherent diffraction imaging (BCDI) is a lens-less imaging method that measures speckle patterns near Bragg diffraction from a crystalline sample and reconstructs the 3D particle images. Since Bragg diffraction is inherently sensitive to displacements of the crystal lattice, BCDI yields the displacement field within the sample as well as the electron density, i.e., the “shape” of the particle. This displacement field information further allows us to evaluate strain distribution, dislocations, and composition distribution in the particle. BCDI is also advantageous for in situ measurements because the 3D image can be obtained by rotating the sample by only a few degrees, which eases the geometrical constraint of an electrochemical cell for the measurement. This is in contrast to conventional 3D imaging techniques such as X-ray CT, which usually requires 180 degrees of sample rotation.Furthermore, it is expected that the measurement capabilities of BCDI will be rapidly advanced by upgrading synchrotron radiation facilities such as APS-U, which delivers high-flux coherent X-rays. This should expand the applications of BCDI to wider electrochemical materials. In this presentation, we will briefly overview the principle of BCDI followed by specific examples of in situ measurements of catalytic alloy particles [2-4] conducted at 34-ID-C at Advanced Photon Source.[1] F. Tao et al., Science 322, 932 (2008).[2] T. Kawaguchi et al., Phys. Rev. Lett. 123, 246001 (2019).[3] T. Kawaguchi et al., Nano Lett. 21, 5945 (2021).[4] D. Sheyfer, R. G. Mariano, T. Kawaguchi, et al., Nano Lett. 23, 1 (2023).
Read full abstract