Measuring and directing charge transfer in heterogenous catalysts

Zachman, Michael J.; Fung, Victor; Polo‐Garzon, Felipe; Cao, Shaohong; Moon, Jisue; Huang, Zhennan; Jiang, De‐en; Wu, Zili; Chi, Miaofang

doi:10.1038/s41467-022-30923-2

Cited by 41 publications

(28 citation statements)

References 70 publications

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“…For instance, the charge transfer from the SrTiO 3 (STO) support to Au nanoparticle is directly visualized, which is supported by DFT calculations. 167 This technique can be extended to the characterization of bimetallic nanoparticles supported on solid carriers, which may provide insights on the charge redistribution in these materials.…”

Section: Characterization Of Morphologymentioning

confidence: 99%

Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

2023

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Heterogeneous bimetallic catalysts have broad applications in industrial processes, but achieving a fundamental understanding on the nature of the active sites in bimetallic catalysts at the atomic and molecular level is very challenging due to the structural complexity of the bimetallic catalysts. Comparing the structural features and the catalytic performances of different bimetallic entities will favor the formation of a unified understanding of the structure−reactivity relationships in heterogeneous bimetallic catalysts and thereby facilitate the upgrading of the current bimetallic catalysts. In this review, we will discuss the geometric and electronic structures of three representative types of bimetallic catalysts (bimetallic binuclear sites, bimetallic nanoclusters, and nanoparticles) and then summarize the synthesis methodologies and characterization techniques for different bimetallic entities, with emphasis on the recent progress made in the past decade. The catalytic applications of supported bimetallic binuclear sites, bimetallic nanoclusters, and nanoparticles for a series of important reactions are discussed. Finally, we will discuss the future research directions of catalysis based on supported bimetallic catalysts and, more generally, the prospective developments of heterogeneous catalysis in both fundamental research and practical applications.

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Section: Characterization Of Morphologymentioning

confidence: 99%

Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

2023

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“…Moreover, the 4D-STEM technique can even be used to image light elements such as lithium atoms. 307 With 4D-STEM, 306 one can capture ADF, BF, and CoM in tandem to uncover both structural and chemical information. In particular, the CoM of the electron beam intensity in the detector plane retains information on internal fields as it measures the momentum transfer from the specimen to the electron probe.…”

Section: Measuring Charge Transfer In Heterogeneous Catalysts Using 4...mentioning

confidence: 99%

In Situ and Emerging Transmission Electron Microscopy for Catalysis Research

et al. 2023

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Catalysts are the primary facilitator in many dynamic processes. Therefore, a thorough understanding of these processes has vast implications for a myriad of energy systems. The scanning/transmission electron microscope (S/TEM) is a powerful tool not only for atomic-scale characterization but also in situ catalytic experimentation. Techniques such as liquid and gas phase electron microscopy allow the observation of catalysts in an environment conducive to catalytic reactions. Correlated algorithms can greatly improve microscopy data processing and expand multidimensional data handling. Furthermore, new techniques including 4D-STEM, atomic electron tomography, cryogenic electron microscopy, and monochromated electron energy loss spectroscopy (EELS) push the boundaries of our comprehension of catalyst behavior. In this review, we discuss the existing and emergent techniques for observing catalysts using S/TEM. Challenges and opportunities highlighted aim to inspire and accelerate the use of electron microscopy to further investigate the complex interplay of catalytic systems.

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“…The mapping results offer direct evidence for the discussion of the spatial charge transfer and redistribution upon the SMSI occurrence. The subnanometer charge transfer behavior can be further correlated to the atomically resolved interfacial structures when combined with computational studies . In a recent study, an unsupervised machine learning method has been developed to interrogate the weak and thus mostly overlooked STEM-EELS signals contributed by the ultrathin SMSI overlayer .…”

Section: Characterization and Identification Of Smsimentioning

confidence: 99%

“…The subnanometer charge transfer behavior can be further correlated to the atomically resolved interfacial structures when combined with computational studies. 35 In a recent study, an unsupervised machine learning method has been developed to interrogate the weak and thus mostly overlooked STEM-EELS signals contributed by the ultrathin SMSI overlayer. 36 Near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and operando X-ray absorption spectroscopy (XAS) containing X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) results are powerful tools to gain macroscopic structural and electronic information complementary to the microscopic data.…”

Section: Smsimentioning

confidence: 99%

Nonclassical Strong Metal–Support Interactions for Enhanced Catalysis

Sun

Yang

Dai

2023

J. Phys. Chem. Lett.

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Figure 1. (a) Schematic summarizing the characterization techniques for identifying the occurrence of SMSI. (b) In situ DRIFT spectra monitoring evolution of the adsorbed CO species on the Ru nanoparticles with partial TiO x encapsulation under H 2 flow at 160 °C. The inset shows the emergence of CH 4 species with the characteristic frequency at 3015 cm −1 upon introducing H 2 . Reproduced with permission from ref 26. Copyright 2020 Springer Nature. (c) In situ XRD result of the Pt-TiO 2 catalyst treated with H 2 at 200 and 600 °C, respectively, as well as the corresponding Pawley fitting result for the Pt unit cell after H 2 reduction at different temperatures. The diffraction shift toward higher angles and lattice contraction of the Pt unit cell indicates the alloying pathway along with the suboxide overlayer formation. Reproduced with permission from ref 27. Copyright 2020 Springer Nature. Annular bright field (ABF) image of the Pd(111) surface interfaced with the TiO x overlayer composed of a bilayer structure with the lattice spacing being ∼2.9 and ∼3.0 Å, respectively. The Pd/TiO x interface is highlighted using the dashed yellow line. Adapted with permission from ref 31.

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Measuring and directing charge transfer in heterogenous catalysts

Cited by 41 publications

References 70 publications

Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

In Situ and Emerging Transmission Electron Microscopy for Catalysis Research

Nonclassical Strong Metal–Support Interactions for Enhanced Catalysis

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