Three-dimensional strain dynamics govern the hysteresis in heterogeneous catalysis

Passos, Aline Ribeiro; Rochet, Amélie; Manente, Luiza M.; Suzana, Ana F.; Harder, Ross; Cha, Wonsuk; Meneau, Florian

doi:10.1038/s41467-020-18622-2

Cited by 23 publications

(23 citation statements)

References 41 publications

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“…But note that the strain may propagate from the surface of the crystal into its interior during the reaction as demonstrated in Refs. [40,41] . The large penetration depth of X-rays allows more flexibility on the sample environment; as Bragg coherent X-ray imaging is non-destructive with proper calibration of the X-ray beam attenuation, it can be applied repeatedly during catalytic reaction on the same nanoparticle.…”

Section: Resultsmentioning

confidence: 99%

Facet‐Dependent Strain Determination in Electrochemically Synthetized Platinum Model Catalytic Nanoparticles

Carnis

Gao

Fernandez

et al. 2021

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Studying model nanoparticles is one approach to better understand the structural evolution of a catalyst during reactions. These nanoparticles feature well‐defined faceting, offering the possibility to extract structural information as a function of facet orientation and compare it to theoretical simulations. Using Bragg Coherent X‐ray Diffraction Imaging, the uniformity of electrochemically synthesized model catalysts is studied, here high‐index faceted tetrahexahedral (THH) platinum nanoparticles at ambient conditions. 3D images of an individual nanoparticle are obtained, assessing not only its shape but also the specific components of the displacement and strain fields both at the surface of the nanocrystal and inside. The study reveals structural diversity of shapes and defects, and shows that the THH platinum nanoparticles present strain build‐up close to facets and edges. A facet recognition algorithm is further applied to the imaged nanoparticles and provides facet‐dependent structural information for all measured nanoparticles. In the context of strain engineering for model catalysts, this study provides insight into the shape‐controlled synthesis of platinum nanoparticles with high‐index facets.

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Section: Resultsmentioning

confidence: 99%

Facet‐Dependent Strain Determination in Electrochemically Synthetized Platinum Model Catalytic Nanoparticles

Carnis

Gao

Fernandez

et al. 2021

Small

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“…Adjusting the reaction temperature can alter the catalytic performance in some cases. Passos et al 203 reported how heating versus cooling cycles influence the single nanoparticle elastic energy landscape. The highly compressive and tensile strain distribution was accordingly changed with temperature and so was the CO oxidation performance.…”

Section: Experimental Operando Applicationmentioning

confidence: 99%

Dynamics of Heterogeneous Catalytic Processes at Operando Conditions

Shi

Lin

Luo

et al. 2021

JACS Au

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The rational design of high-performance catalysts is hindered by the lack of knowledge of the structures of active sites and the reaction pathways under reaction conditions, which can be ideally addressed by an in situ / operando characterization. Besides the experimental insights, a theoretical investigation that simulates reaction conditions—so-called operando modeling—is necessary for a plausible understanding of a working catalyst system at the atomic scale. However, there is still a huge gap between the current widely used computational model and the concept of operando modeling, which should be achieved through multiscale computational modeling. This Perspective describes various modeling approaches and machine learning techniques that step toward operando modeling, followed by selected experimental examples that present an operando understanding in the thermo- and electrocatalytic processes. At last, the remaining challenges in this area are outlined.

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“…In situ Bragg coherent diffraction imaging (BCDI) recently demonstrated the possibility to acquire 3D strain maps of NPs and nanostructures 26 . In particular, the technique has been successfully used to reveal in situ bulk and surface strain dynamics as well as localisation of active sites during reaction 27 – 29 .…”

Section: Introductionmentioning

confidence: 99%

Imaging the facet surface strain state of supported multi-faceted Pt nanoparticles during reaction

Dupraz

Carnis

et al. 2022

Nat Commun

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Nanostructures with specific crystallographic planes display distinctive physico-chemical properties because of their unique atomic arrangements, resulting in widespread applications in catalysis, energy conversion or sensing. Understanding strain dynamics and their relationship with crystallographic facets have been largely unexplored. Here, we reveal in situ, in three-dimensions and at the nanoscale, the volume, surface and interface strain evolution of single supported platinum nanocrystals during reaction using coherent x-ray diffractive imaging. Interestingly, identical {hkl} facets show equivalent catalytic response during non-stoichiometric cycles. Periodic strain variations are rationalised in terms of O2 adsorption or desorption during O2 exposure or CO oxidation under reducing conditions, respectively. During stoichiometric CO oxidation, the strain evolution is, however, no longer facet dependent. Large strain variations are observed in localised areas, in particular in the vicinity of the substrate/particle interface, suggesting a significant influence of the substrate on the reactivity. These findings will improve the understanding of dynamic properties in catalysis and related fields.

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Three-dimensional strain dynamics govern the hysteresis in heterogeneous catalysis

Cited by 23 publications

References 41 publications

Facet‐Dependent Strain Determination in Electrochemically Synthetized Platinum Model Catalytic Nanoparticles

Facet‐Dependent Strain Determination in Electrochemically Synthetized Platinum Model Catalytic Nanoparticles

Dynamics of Heterogeneous Catalytic Processes at Operando Conditions

Imaging the facet surface strain state of supported multi-faceted Pt nanoparticles during reaction

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