A perspective on oxide-supported single-atom catalysts

Zhou, Junyi; Xu, Zhen; Xu, Mingzhi; Zhou, Xiong; Wu, Kai

doi:10.1039/d0na00393j

Cited by 18 publications

(14 citation statements)

References 87 publications

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“…The atomically dispersed nature of SACs allows the utilization of almost 100% of its activity, which bodes well for newer opportunities in several applications. Apart from carbon as a support material, several other porous metal oxides including 2D nanomaterials have been successfully utilized for the preparation of SACs. ,− …”

Section: Synthesis Of Fe-sacsmentioning

confidence: 99%

Single-Atom (Iron-Based) Catalysts: Synthesis and Applications

et al. 2021

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Supported single-metal atom catalysts (SACs) are constituted of isolated active metal centers, which are heterogenized on inert supports such as graphene, porous carbon, and metal oxides. Their thermal stability, electronic properties, and catalytic activities can be controlled via interactions between the single-metal atom center and neighboring heteroatoms such as nitrogen, oxygen, and sulfur. Due to the atomic dispersion of the active catalytic centers, the amount of metal required for catalysis can be decreased, thus offering new possibilities to control the selectivity of a given transformation as well as to improve catalyst turnover frequencies and turnover numbers. This review aims to comprehensively summarize the synthesis of Fe-SACs with a focus on anchoring single atoms (SA) on carbon/graphene supports. The characterization of these advanced materials using various spectroscopic techniques and their applications in diverse research areas are described. When applicable, mechanistic investigations conducted to understand the specific behavior of Fe-SACs-based catalysts are highlighted, including the use of theoretical models. CONTENTS 1. Introduction 13620 2. Scope of This Review 13623 3. Synthesis of Fe-SACs 13623 3.1. N-Doped Graphene-Based Fe-SACs 13623 3.2. Nitrogen-Doped Porous Carbon-Based Fe-SACs 13626 3.3. C 3 N 4 -Based Fe-SACs 13634 4.

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Section: Synthesis Of Fe-sacsmentioning

confidence: 99%

Single-Atom (Iron-Based) Catalysts: Synthesis and Applications

et al. 2021

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“…In their pioneering article, Zhang and coworkers reported on an investigation of Pt/FeOx SAC for CO oxidation [25]. Though the current SAC literature is dominated by carbon-based materials (especially for electrocatalytic applications), most of the works on SAC in the early 2010s and before, used transition metal oxides as the support, and this field is still very active [36,37]. In addition to recent SAC studies on late transition metals, it has been known for decades that various selective (mild) oxidation reactions are well catalyzed by oxide-supported molecular structures consisting of early transition metals coordinated to oxygen atoms, i.e.…”

Section: Oxide-supported Single-atom Catalystsmentioning

confidence: 99%

Supported Metal Single‐Atom Thermocatalysts for Oxidation Reactions

Piccolo

Loridant

Christopher

2022

Supported Metal Single Atom Catalysis

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The interest in single-metal-atom dispersion in heterogeneous catalysis has existed since the 1950s with spectroscopic investigations of rhodium "single-site" catalysts supported on alumina, and more recently with oxometallate monomers for selective oxidation reactions. A decade ago, advances in electron microscopy intensified the interest of the catalysis community in controlling the dispersion of supported metals down to the single-atom active site level and revealing their intrinsic catalytic properties. Pioneering works in the ever-growing field of single-atom catalysis investigated late transition metals (group 8 to 11) supported on transition metal oxides for the CO oxidation and water-gas shift reactions. Since then, various single-atom catalysts, most often supported on oxides, have been evaluated in a broad panel of thermal oxidation reactions, and have often shown remarkable performances. Besides CO oxidation over oxidesupported noble metals, which represents the major part of the literature, this chapter reviews the main classes of oxidation reactions, including total and selective oxidations of hydrocarbons and oxygenates, on 2 oxide-or carbon-supported catalysts. Throughout the chapter, we emphasize several aspects that we consider important, such as the coordination environment and stability of single metal atoms, as well as their compared performance with supported nanoparticles. Figure 3. a) Aberration-corrected STEM image of Pt atoms (identified by yellow circles) on ca. 5 nm diameter anatase TiO2 particles. Adapted with permission from [72], Copyright 2017 ACS. b) CO probemolecule FTIR spectra of a Pt/TiO2 SAC as a function of temperature during a TPD measurement. c) DFT-calculated structure of CO bound to PtO2 adsorbed at a TiO2(145) step edge. b and c adapted with permission from [73], Copyright 2018 Elsevier. d) Schematic showing the structural transformation of isolated Pt species as a function of environmental conditions. Adapted with permission from [74],Copyright 2019 Springer Nature. e) DFT-calculated reaction pathway for CO oxidation on a Pd/TiO2 SAC that was supported by spectroscopic and kinetic analyses. Adapted with permission from [75],

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“…Single atom catalysts (SACs), which essentially involve singleatom active sites on supports, have been extensively studied ever since the pioneering series of work by Zhang and coworkers in 2011. [1][2][3][4][5][6][7][8][9][10][11] Single atoms, which can be envisioned as being downsized from nanoparticles (NPs), may exhibit a superb catalytic performance in various catalytic reactions due to their low coordination number, strong metal-support interaction and quantized band structure or discrete energy levels. However, the inherent ineffectiveness for reactions that require simultaneous participation of more active metal atoms frequently prevents SACs from working, in addition to everchanging interactions between the reactants and supported single atoms, 4,[12][13][14] the available chemical environment and metal-support interactions.…”

Section: Introductionmentioning

confidence: 99%

“…In contrast to extensively adopted approaches to anchoring single atoms, a new strategy to stabilize single atoms on supports is proposed in our previous study, 8 where the oxide support is made as thin as possible so that its surface free energy can be effectively augmented by its underlying bulk metal substrate. Once the surface free energy of the ultrathin oxide support becomes comparable with that of the metal species or chemical potential of an individual metal atom, the single metal atom can then be thermally stabilized on the ultrathin oxide lm without aggregation.…”

Section: Introductionmentioning

confidence: 99%

“…In the past few decades, plenty of SACs have been prepared and reported. 2,[6][7][8][94][95][96][97][98][99][100][101][102][103][104][105][106][107][108][109][110][111] However, the insight at the atomic level of charge transfer between single atoms and their supports is still elusive. A clear picture of charge transfer can obviously help understand the extraordinary catalytic performance of SACs as well as the promoter effects of alkali metals and halogens in conventional heterogeneous catalysis.…”

Section: Introductionmentioning

confidence: 99%

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