Unveiling the nucleation and evolution of twinned intermetallic nanocrystals for CO-tolerant selective hydrogenation

Wang, Kun; Liu, Haojie; Zhang, Luyao; Yu, Boyuan; Hu, Yang; Yang, Feng

doi:10.1039/d2qi02262a

Cited by 3 publications

(3 citation statements)

References 66 publications

(90 reference statements)

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“…Most of heterogeneous reactions occurred in microenvironments, such as on solid surface, interface [22, 49,93,97,98], or in confined pore [99]. Therefore, it is essential to investigate the dynamics of clusters in such a realistic environment.…”

Section: Dynamics Of Metal Nanoclusters In Confined Spacementioning

confidence: 99%

Dynamic evolution of metal nanoclusters revealed by in-situ electron microscopy

Zhang

et al. 2023

J. Phys. D: Appl. Phys.

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Nanoclusters involve finite metal atoms are of great importance in chemical synthesis and catalysis due to their unique structure-dependent properties. Knowing how nanoclusters work in reaction conditions is no doubt one of the most important challenges, which requires deep insight into atomic-scale dynamics during the process. State-of-the-art in-situ transmission electron microscope (TEM) can realize the real-time study, which is expected to reveal insights into the underlying mechanisms of catalysis and design efficient catalysts. In this minireview, we aim to give a critical review and recent progress on nanocluster dynamics unveiled by in-situ and environmental TEM from two aspects: evolutions of metal single atoms and nanoclusters in high-temperature reaction conditions and the well-defined molecular clusters in confined space. We emphasize the cluster-environment interaction and the cluster structure-property relationships. In the end, we also summarize the present achievements and propose future challenges. We expect this review will fuel the excitement and stimulate research in the fields of cluster and catalysis.

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Section: Dynamics Of Metal Nanoclusters In Confined Spacementioning

confidence: 99%

Dynamic evolution of metal nanoclusters revealed by in-situ electron microscopy

Zhang

et al. 2023

J. Phys. D: Appl. Phys.

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“…Limited by the 2D projection of transmission electron microscopy (TEM) images, the surface atomic structures of HEI nanocrystals are still unreachable. Second, the disorder-to-order (i.e., solid-solution-to-intermetallic) phase transition at high temperatures, − which is generally necessary to prepare HEI is rather complicated. Third, interactions among multimetals of HEI are more complicated than in binary intermetallic.…”

Section: Introductionmentioning

confidence: 99%

Unveiling Atomic-Scaled Local Chemical Order of High-Entropy Intermetallic Catalyst for Alkyl-Substitution-Dependent Alkyne Semihydrogenation

Liu,

Zhang,

Zhang

et al. 2024

J. Am. Chem. Soc.

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High-entropy intermetallic (HEI) nanocrystals, composed of multiple elements with an ordered structure, are of immense interest in heterogeneous catalysis due to their unique geometric and electronic structures and the cocktail effect. Despite tremendous efforts dedicated to regulating the metal composition and structures with advanced synthetic methodologies to improve the performance, the surface structure, and local chemical order of HEI and their correlation with activity at the atomic level remain obscure yet challenging. Herein, by determining the three-dimensional (3D) atomic structure of quinary PdFeCoNiCu (PdM) HEI using atomic-resolution electron tomography, we reveal that the local chemical order of HEI regulates the surface electronic structures, which further mediates the alkyl-substitutiondependent alkyne semihydrogenation. The 3D structures of HEI PdM nanocrystals feature an ordered (intermetallic) core enclosed by a disordered (solid-solution) shell rather than an ordered surface. The lattice mismatch between the core and shell results in apparent near-surface distortion. The chemical order of the intermetallic core increases with annealing temperature, driving the electron redistribution between Pd and M at the surface, but the surface geometrical (chemically disordered) configurations and compositions are essentially unchanged. We investigate the catalytic performance of HEI PdM with different local chemical orders toward semihydrogenation across a broad range of alkynes, finding that the electron density of surface Pd and the hindrance effect of alkyl substitutions on alkynes are two key factors regulating selective semihydrogenation. We anticipate that these findings on surface atomic structure will clarify the controversy regarding the geometric and/or electronic effects of HEI catalysts and inspire future studies on tuning local chemical order and surface engineering toward enhanced catalysts.

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“…In situ characterization techniques with atomically resolved spatial resolution is desired. In recent years, in situ scanning transmission electron microscopy (S/TEM) has gained prominence as a technique for investigating transient catalyst phenomena due to its exceptional subnanometer spatial resolution, enabling direct observation of dynamic catalyst changes, including size, morphology, facets, and migration behavior. − By replicating the atmospheric composition and temperature of catalyst reaction conditions, researchers have revealed structural and chemical evolutions in various catalysts with the necessary spatial and temporal resolutions. These observations have provided direct insights into our understanding of reaction mechanisms and catalyst degradation processes.…”

mentioning

confidence: 99%

Sintering Mechanism of Pt/Al₂O₃ in Complex Emission Gases Elucidated via In Situ Environmental STEM

Smith,

Liccardo,

Cendejas

et al. 2024

ACS Materials Lett.

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Unveiling the nucleation and evolution of twinned intermetallic nanocrystals for CO-tolerant selective hydrogenation

Abstract: Revealing the nucleation and evolution processes of nanocrystals is of great importance for their application as catalytic materials, the performance of which is closely related to their surface and interface...

Cited by 3 publications

References 66 publications

Dynamic evolution of metal nanoclusters revealed by in-situ electron microscopy

Dynamic evolution of metal nanoclusters revealed by in-situ electron microscopy

Unveiling Atomic-Scaled Local Chemical Order of High-Entropy Intermetallic Catalyst for Alkyl-Substitution-Dependent Alkyne Semihydrogenation

Sintering Mechanism of Pt/Al₂O₃ in Complex Emission Gases Elucidated via In Situ Environmental STEM

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Unveiling the nucleation and evolution of twinned intermetallic nanocrystals for CO-tolerant selective hydrogenation

Abstract: Revealing the nucleation and evolution processes of nanocrystals is of great importance for their application as catalytic materials, the performance of which is closely related to their surface and interface...

Cited by 3 publications

References 66 publications

Dynamic evolution of metal nanoclusters revealed by in-situ electron microscopy

Dynamic evolution of metal nanoclusters revealed by in-situ electron microscopy

Unveiling Atomic-Scaled Local Chemical Order of High-Entropy Intermetallic Catalyst for Alkyl-Substitution-Dependent Alkyne Semihydrogenation

Sintering Mechanism of Pt/Al2O3 in Complex Emission Gases Elucidated via In Situ Environmental STEM

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Sintering Mechanism of Pt/Al₂O₃ in Complex Emission Gases Elucidated via In Situ Environmental STEM