Determination of the 3D Atomic Structures of Nanoparticles

Kim, Byung Hyo; Heo, Jun-Young

doi:10.1002/smsc.202000045

Cited by 16 publications

(23 citation statements)

References 78 publications

(91 reference statements)

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“…The recent development of advanced characterization techniques, including aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM), scanning tunneling microscopy images, extended X-ray absorption fine structure (EXAFS) curve fitting, and DFT modeling, provide crucial tools for identifying the atomic structure. [31][32][33][34][35][36][37] Meanwhile, tremendous efforts have been devoted to exploring SMSIs in SACs and their relationship with catalytic properties. [38][39][40][41] However, a systematic understanding of SMSIs Recognizing and controlling the structure-activity relationships of singleatom catalysts (SACs) is vital for manipulating their catalytic properties for various practical applications.…”

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confidence: 99%

Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species

et al. 2022

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atoms in SACs are chemically bonded to elements on the supports. This unique structural characteristic endows SACs with strong metal support interactions (SMSIs) [6][7][8][9][10] and tailorable homogenized active metal sites. [11][12][13][14] SACs have been found to be very favorable in many fields, including electrocatalysis, [15][16][17][18] organocatalysis, [19][20][21] industrial catalysis, [22][23][24] and others. [25][26][27][28][29][30] Consequently, revealing the atomic structure of the central metal atoms and the SMSI in SACs has become an important subject of research because it provides possibilities for rational design of novel SACs for specific reactions. The recent development of advanced characterization techniques, including aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM), scanning tunneling microscopy images, extended X-ray absorption fine structure (EXAFS) curve fitting, and DFT modeling, provide crucial tools for identifying the atomic structure. [31][32][33][34][35][36][37] Meanwhile, tremendous efforts have been devoted to exploring SMSIs in SACs and their relationship with catalytic properties. [38][39][40][41] However, a systematic understanding of SMSIs Recognizing and controlling the structure-activity relationships of singleatom catalysts (SACs) is vital for manipulating their catalytic properties for various practical applications. Herein, Fe SACs supported on nitrogen-doped carbon (SA-Fe/CN) are reported, which show high catalytic reactivity (97% degradation of bisphenol A in only 5 min), high stability (80% of reactivity maintained after five runs), and wide pH suitability (working pH range 3-11) toward Fenton-like reactions. The roles of different N species in these reactions are further explored, both experimentally and theoretically. It is discovered that graphitic N is an adsorptive site for the target molecule, pyrrolic N coordinates with Fe(III) and plays a dominant role in the reaction, and pyridinic N, coordinated with Fe(II), is only a minor contributor to the reactivity of SA-Fe/CN. Density functional theory (DFT) calculations reveal that a lower d-band center location of pyrrolic-type Fe sites leads to the easy generation of Fe-oxo intermediates, and thus, excellent catalytic properties.

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confidence: 99%

Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species

et al. 2022

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“…First, it overcomes the stage rotation limitation and, therefore, removes the missing-wedge artifacts. Second, it allows data acquisition in a period of seconds (compared to minutes and hours for cryoET) . Brownian tomography has many challenges including the development of sample preparation methods where particle rotation is controlled and also quantifying electron-sample interactions.…”

Section: Tem Methodsmentioning

confidence: 99%

“…Second, it allows data acquisition in a period of seconds (compared to minutes and hours for cryoET). 193 Brownian tomography has many challenges including the development of sample preparation methods where particle rotation is controlled and also quantifying electron-sample interactions. However, continued development of this method could enable self-assembly mechanisms of unique 3D objects to be studied with nanometer or even atomic resolution.…”

Section: Electron Tomography and Single Particle Analysismentioning

confidence: 99%

A Close Look at Molecular Self-Assembly with the Transmission Electron Microscope

et al. 2021

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Molecular self-assembly is pervasive in the formation of living and synthetic materials. Knowledge gained from research into the principles of molecular self-assembly drives innovation in the biological, chemical, and materials sciences. Self-assembly processes span a wide range of temporal and spatial domains and are often unintuitive and complex. Studying such complex processes requires an arsenal of analytical and computational tools. Within this arsenal, the transmission electron microscope stands out for its unique ability to visualize and quantify self-assembly structures and processes. This review describes the contribution that the transmission electron microscope has made to the field of molecular self-assembly. An emphasis is placed on which TEM methods are applicable to different structures and processes and how TEM can be used in combination with other experimental or computational methods. Finally, we provide an outlook on the current challenges to, and opportunities for, increasing the impact that the transmission electron microscope can have on molecular self-assembly.

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“…Although the first application of tomography was in astronomy, and ET has been well developed as an advanced technology with angstrom-level resolution using modern TEM systems, 15 this technique is largely overlooked by the earth and planetary science community. Only a few recent studies have employed ET for research in the field of earth and planetary science (e.g., Refs.…”

Section: Introductionmentioning

confidence: 99%

Three-Dimensional Analyses Of Geological Materials On Nanoscale By Electron Tomography

Zhu¹

2022

At.Spectrosc.

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Electron tomography (ET), an electron-microscopy-based technique that provides three-dimensional (3D) structural information from a tilt series of two-dimensional (2D) projections, has promoted the in-depth investigation of biological molecules in structural biology and the analysis of material structures on the atomic scale in physical sciences. Although ET has developed rapidly as an effective technique wherein atomic-scale resolution has been achieved by using advanced transmission electron microscopy systems, it has not been widely used by the earth and planetary science community. Herein, we verify the applicability of ET in research related to earth and planetary science. The data demonstrate that ET can be used to observe the 3D morphology of mineral grains and 3D distributions of the chemical components of earth and planetary materials. Notably, ET coupled with spectroscopy, including electron energy loss spectroscopy and energy dispersive spectroscopy, is an effective technique for studying the 3D distribution of elements and their various oxidation states in geological materials. Atomic ET is also a promising technique for detecting trace elements in host minerals. The use of ET can advance the study of earth and planetary materials because it provides additional 3D information about geological objects.

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Determination of the 3D Atomic Structures of Nanoparticles

Cited by 16 publications

References 78 publications

Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species

Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species

A Close Look at Molecular Self-Assembly with the Transmission Electron Microscope

Three-Dimensional Analyses Of Geological Materials On Nanoscale By Electron Tomography

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