Single-Atom Catalysis: How Structure Influences Catalytic Performance

Parkinson, Gareth S.

doi:10.1007/s10562-019-02709-7

Cited by 94 publications

(62 citation statements)

References 67 publications

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“…The field of single‐atom catalysis (SAC) arose as the ultimate extension of attempts to reduce the precious‐metal content of supported heterogeneous catalysts. While it now seems established that supported metal adatoms can catalyze heterogeneous and electrochemical reactions, it is increasingly clear that the properties of single‐atom catalysts (SACs) differ significantly from those of supported metal nanoparticles . This is because stable adatoms must derive their stability from chemical bonds to the support lattice, which modifies their electronic structure, and thus their interaction with reactants .…”

Section: Introductionsupporting

confidence: 72%

Local Structure and Coordination Define Adsorption in a Model Ir₁/Fe₃O₄ Single‐Atom Catalyst

et al. 2019

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Single‐atom catalysts (SACs) bridge homo‐ and heterogeneous catalysis because the active site is a metal atom coordinated to surface ligands. The local binding environment of the atom should thus strongly influence how reactants adsorb. Now, atomically resolved scanning‐probe microscopy, X‐ray photoelectron spectroscopy, temperature‐programmed desorption, and DFT are used to study how CO binds at different Ir1 sites on a precisely defined Fe3O4(001) support. The two‐ and five‐fold‐coordinated Ir adatoms bind CO more strongly than metallic Ir, and adopt structures consistent with square‐planar IrI and octahedral IrIII complexes, respectively. Ir incorporates into the subsurface already at 450 K, becoming inactive for adsorption. Above 900 K, the Ir adatoms agglomerate to form nanoparticles encapsulated by iron oxide. These results demonstrate the link between SAC systems and coordination complexes, and that incorporation into the support is an important deactivation mechanism.

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Section: Introductionsupporting

confidence: 72%

Local Structure and Coordination Define Adsorption in a Model Ir₁/Fe₃O₄ Single‐Atom Catalyst

et al. 2019

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“…[ 29 ] In that context, the use of vacancy containing support should offer interesting perspectives. [ 30 ]…”

Section: Introductionmentioning

confidence: 99%

Stabilization of Metal Single Atoms on Carbon and TiO₂ Supports for CO₂ Hydrogenation: The Importance of Regulating Charge Transfer

Rivera‐Cárcamo

Scarfiello

Garcı́a

et al. 2020

Adv Materials Inter

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Supported single atoms constitute excellent models for understanding heterogenous catalysis and have achieved breakthroughs during the past years. How to prevent the aggregation and modulate activity of these species via metal‐support interaction should be considered for practical applications. This work presents simple methods involving the creation of carbon‐ (on carbon nanotube (CNT)) or oxygen‐vacancies (on TiO2) to stabilize nickel and ruthenium single atoms. The defective supports and the resulting catalysts are characterized by a large variety of techniques. These analyses show that this strategy is efficient for the preparation of ultra‐dispersed catalysts. Comparison of the catalytic performances of these catalysts for the CO2 hydrogenation reaction is also reported. Catalysts supported on TiO2 are more active and sometimes more stable than those deposited on CNT. Nickel catalysts are very selective for the production of CO, and ruthenium catalysts are more selective for the production of methane. Most importantly, it is shown that, in the case of Ru, a direct correlation exists between the electronic density on the metal and the selectivity; electron‐rich species produce selectively methane, while electron‐deficient species orientate the selectivity toward CO. This work may figure a new way for the synthesis of ultra‐dispersed catalysts for various applications.

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“…Quite a few reviews on SACs have been published in the past decades and provided excellent overviews of this rapidly growing research eld. [26][27][28][29][30][31][32][33][34][35][36][37][38][39][40][41][42][43] These reviews have already summarized synthetic strategies, structural characterization, and/or catalytic evaluations for specic reactions. In this minireview, we instead try to provide a fundamental understanding of the intrinsic principles of SACs in their catalytic performance with some very recent typical case studies in the past years.…”

Section: Introductionmentioning

confidence: 99%

A perspective on oxide-supported single-atom catalysts

Zhou

et al. 2020

Nanoscale Adv.

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Single-Atom Catalysis: How Structure Influences Catalytic Performance

Abstract: Graphical Abstract

Cited by 94 publications

References 67 publications

Local Structure and Coordination Define Adsorption in a Model Ir₁/Fe₃O₄ Single‐Atom Catalyst

Local Structure and Coordination Define Adsorption in a Model Ir₁/Fe₃O₄ Single‐Atom Catalyst

Stabilization of Metal Single Atoms on Carbon and TiO₂ Supports for CO₂ Hydrogenation: The Importance of Regulating Charge Transfer

A perspective on oxide-supported single-atom catalysts

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Single-Atom Catalysis: How Structure Influences Catalytic Performance

Abstract: Graphical Abstract

Cited by 94 publications

References 67 publications

Local Structure and Coordination Define Adsorption in a Model Ir1/Fe3O4 Single‐Atom Catalyst

Local Structure and Coordination Define Adsorption in a Model Ir1/Fe3O4 Single‐Atom Catalyst

Stabilization of Metal Single Atoms on Carbon and TiO2 Supports for CO2 Hydrogenation: The Importance of Regulating Charge Transfer

A perspective on oxide-supported single-atom catalysts

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Product

Resources

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Local Structure and Coordination Define Adsorption in a Model Ir₁/Fe₃O₄ Single‐Atom Catalyst

Local Structure and Coordination Define Adsorption in a Model Ir₁/Fe₃O₄ Single‐Atom Catalyst

Stabilization of Metal Single Atoms on Carbon and TiO₂ Supports for CO₂ Hydrogenation: The Importance of Regulating Charge Transfer