Abstract

Nanoparticles are essential electrocatalysts in chemical production, water treatment and energy conversion, but engineering efficient and specific catalysts requires understanding complex structure-reactivity relations. Recent experiments have shown that Bragg coherent diffraction imaging might be a powerful tool in this regard. The technique provides three-dimensional lattice strain fields from which surface reactivity maps can be inferred. However, all experiments published so far have investigated particles an order of magnitude larger than those used in practical applications. Studying smaller particles quickly becomes demanding as the diffracted intensity falls. Here, in situ nanodiffraction data from 60 nm Au nanoparticles under electrochemical control collected at the hard X-ray nanoprobe beamline of MAX IV, NanoMAX, are presented. Two-dimensional image reconstructions of these particles are produced, and it is estimated that NanoMAX, which is now open for general users, has the requisites for three-dimensional imaging of particles of a size relevant for catalytic applications. This represents the first demonstration of coherent X-ray diffraction experiments performed at a diffraction-limited storage ring, and illustrates the importance of these new sources for experiments where coherence properties become crucial.

Highlights

  • Nanoparticles are used as catalysts for a range of electrochemical reactions (Kleijn et al, 2014)

  • We report results from two-dimensional Bragg coherent diffraction imaging (BCDI) studies performed on 60 nm gold particles inside an electrochemical cell

  • The particles were characterized by transmission electron microscopy (TEM) and found to be regular octahedra of side 64 nm, truncated by a cube of side 62 nm (Figure S1 of the supporting information), equivalent in volume to a sphere of diameter 59 nm

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Summary

Introduction

Nanoparticles are used as catalysts for a range of electrochemical reactions (Kleijn et al, 2014). 26, 1830–1834 short communications (Robinson & Harder, 2009; Favre-Nicolin et al, 2010) This information can, in turn, be used to map catalyst particle reactivity and to localize active sites, provided that the reaction induces some local strain in the lattice. While the resolution achievable in BCDI will not always allow distinguishing between such effects through direct imaging of surface structure, the technique is sensitive enough to localize, for example, specific adsorption of reactants. In this way, the catalytic decomposition of dissolved ascorbic acid on gold surfaces was recently mapped across the surfaces of submicrometre particles (Ulvestad et al, 2016). The measured intensity in the far field is proportional to the square modulus of the Fourier transform F of the exit wave,

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