Theoretical Perspective on <i>Operando</i> Spectroscopy of Fluxional Nanocatalysts

Poths, Patricia; Alexandrova, Anastassia N.

doi:10.1021/acs.jpclett.2c00628

Cited by 11 publications

(12 citation statements)

References 68 publications

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“…Note that transition metal sub-nanoclusters can exhibit structural flexibility and rich isomerism not accessible to bulk materials, see ref. 67–69 and references therein.…”

Section: Resultsmentioning

confidence: 99%

Towards determining molecular structure with ESI-MS backed by computational methods: structures of subnanoclusters of Pd and Cu chlorides, ion dynamics in vacuum, and challenges to the methodology

Bondarenko

Vlasova

Polynski

et al. 2022

Inorg. Chem. Front.

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“…Note that transition metal sub-nanoclusters can exhibit structural flexibility and rich isomerism not accessible to bulk materials, see ref. 67–69 and references therein.…”

Section: Resultsmentioning

confidence: 99%

Towards determining molecular structure with ESI-MS backed by computational methods: structures of subnanoclusters of Pd and Cu chlorides, ion dynamics in vacuum, and challenges to the methodology

Bondarenko

Vlasova

Polynski

et al. 2022

Inorg. Chem. Front.

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“…(Photo)electrochemical processes may lead to the destabilization of thermodynamically stable materials and facilitate the formation of metastable phases. Depending on working conditions, these metastable phases may be short- or long-lived and even define the overall interfacial activity and stability. ,− Thus, in some cases, material interfaces can be in constant state of dynamic metastability making it challenging to analyze their properties based solely on equilibrium Pourbaix diagrams. Metastable phases may exhibit catalytic activity much higher than that of their thermodynamically stable parent structures, albeit often at the expense of their stability.…”

Section: Discussionmentioning

confidence: 99%

Corrosion of Electrochemical Energy Materials: Stability Analyses Beyond Pourbaix Diagrams

2023

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Since their first appearance, electrode potential/solution pH charts (Pourbaix diagrams) have served as a general framework for the analysis of material corrosion in aqueous solutions. Their utility in describing electrochemical stability of materials is rooted in the equilibrium thermodynamics based formalism. Electrochemical energy systems, however, do not always operate under thermodynamic equilibrium conditions, and corrosion itself is an inherently irreversible interfacial process. In this Perspective, we highlight a number of representative studies drawn primarily from (photo)electrocatalysis research and aimed to account for the effects of potentiodynamic polarization and transient dissolution, interfacial electrochemical reactions, formation and stability of metastable phases, strain-induced corrosion, as well as the kinetics of dissolution and phase transformations. Some theoretical approaches that can help disentangle corrosion mechanisms under conditions relevant to electrochemical energy conversion applications are briefly discussed. We also advocate for more research efforts directed at the basic science of electrochemical corrosion that has long been deemed as a not “fancy” topic.

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“…More importantly, as we mentioned earlier, it is very difficult to determine the catalytic impact of the structural changes we observe simply from the image, and we expect a significant role of theory to rationalize the underlying processes and the complicated convolution of the different parameters. 57,274 Image-free representations of EM data are thus required to feed computers and to allow for improved causal correlations. The conversion of 2D TEM image stacks into meaningful observables and their representation as multidimensional plots also offer opportunities for novel denoising and reconstruction algorithms, 275 data management, and visualization strategies.…”

Section: Instrumentation Improvements and Methods Developmentmentioning

confidence: 99%

“…In this aspect, we expect that the following data acquisition and analysis approaches will become increasingly integrated into the workflow of future operando experiments: (i) automated sample acquisition routines for large area imaging, (ii) on-the-fly image analysis enabled by machine learning enhanced image segmentation, , and (iii) special software that enables better tracking of metadata such as the imaging conditions, electron dose, and catalysis parameters. More importantly, as we mentioned earlier, it is very difficult to determine the catalytic impact of the structural changes we observe simply from the image, and we expect a significant role of theory to rationalize the underlying processes and the complicated convolution of the different parameters. , Image-free representations of EM data are thus required to feed computers and to allow for improved causal correlations. The conversion of 2D TEM image stacks into meaningful observables and their representation as multidimensional plots also offer opportunities for novel denoising and reconstruction algorithms, data management, and visualization strategies.…”

Section: Perspectives On the Further Directions Of The Fieldmentioning

confidence: 96%

Operando Electron Microscopy of Catalysts: The Missing Cornerstone in Heterogeneous Catalysis Research?

Chee,

Lunkenbein,

Schlögl

et al. 2023

Chem. Rev.

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Heterogeneous catalysis in thermal gas-phase and electrochemical liquid-phase chemical conversion plays an important role in our modern energy landscape. However, many of the structural features that drive efficient chemical energy conversion are still unknown. These features are, in general, highly distinct on the local scale and lack translational symmetry, and thus, they are difficult to capture without the required spatial and temporal resolution. Correlating these structures to their function will, conversely, allow us to disentangle irrelevant and relevant features, explore the entanglement of different local structures, and provide us with the necessary understanding to tailor novel catalyst systems with improved productivity. This critical review provides a summary of the still immature field of operando electron microscopy for thermal gas-phase and electrochemical liquid-phase reactions. It focuses on the complexity of investigating catalytic reactions and catalysts, progress in the field, and analysis. The forthcoming advances are discussed in view of correlative techniques, artificial intelligence in analysis, and novel reactor designs.

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Theoretical Perspective on Operando Spectroscopy of Fluxional Nanocatalysts

Cited by 11 publications

References 68 publications

Towards determining molecular structure with ESI-MS backed by computational methods: structures of subnanoclusters of Pd and Cu chlorides, ion dynamics in vacuum, and challenges to the methodology

Towards determining molecular structure with ESI-MS backed by computational methods: structures of subnanoclusters of Pd and Cu chlorides, ion dynamics in vacuum, and challenges to the methodology

Corrosion of Electrochemical Energy Materials: Stability Analyses Beyond Pourbaix Diagrams

Operando Electron Microscopy of Catalysts: The Missing Cornerstone in Heterogeneous Catalysis Research?

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