Reply to: “Pitfalls in identifying active catalyst species”

Hernández, Xavier Isidro Pereira; DeLaRiva, Andrew; Muravev, Valery; Kunwar, Deepak; Xiong, Haifeng; Sudduth, Berlin; Engelhard, Mark H.; Kovařík, Libor; Hensen, Emiel J. M.; Wang, Yong; Datye, Abhaya K.

doi:10.1038/s41467-020-18193-2

Cited by 53 publications

(115 citation statements)

References 14 publications

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“…Figure 3 shows spectra obtained after CO adsorption (at 25 °C, under conditions that ensured the surface saturation), followed by an Ar flow to eliminate CO. For the as‐synthesized materials, intense bands were observed at 2085 and 2095 cm −1 for Pt/CeO 2 nanocubes (Figure 3a) and Pt/CeO 2 nanowires (Figure 3b), respectively. The symmetric bands at high wavenumber, 2085–2095 cm −1 , can be assigned to the CO adsorbed on ionic Pt δ+ (δ>0) species corresponding to atomically dispersed Pt sites, [19,49,50] partial oxidation of Pt sites (PtO x ) due to a Pt−O−Ce interaction, [51,52] or also oxidation of Pt precursors during the calcination process. The FWHM (full width at half maximum) of CO band at 2095 cm −1 for a Pt/CeO 2 nanowires (Figure 3b) is ∼23 cm −1 , suggesting Pt single‘s uniformity sites as observed by other authors [53] .…”

Section: Resultsmentioning

confidence: 99%

Towards the Effect of Pt⁰/Pt^δ+ and Ce³⁺ Species at the Surface of CeO₂ Crystals: Understanding the Nature of the Interactions under CO Oxidation Conditions

Borges

Silva²,

Braga

et al. 2021

ChemCatChem

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We synthesized CeO2 nanowires and nanocubes showing {110}+{100} and {100} surfaces predominantly, respectively, once the different surface energies play a crucial role in the behavior of Ce4+/Ce3+ reversibility. We found out that Pt/CeO2 nanowires presented more Ce3+ content, oxygen vacancies, and atomically dispersed Pt, indicating a stronger Pt−Ce interaction. In contrast, the Pt/CeO2 nanocubes presented a higher contribution of Ptδ+ species, suggesting a well‐controlled Pt particle size (∼1 nm) and significant interaction with ceria, with oxygen species more available at the surface. Thus, we suggest that the ceria‘s different surface energies may lead to different Pt distributions of species over the supports. H2‐reduction treatment led to changes in Pt structure that showed a better catalysis performance for the Pt/CeO2 nanowires essentially, supported by XPS and CO‐DRIFTS. Nevertheless, this step did not cause improved activity to the point of overcoming the nanocubes‐based catalyst, and the reasons were fully discussed. Herein, we propose that catalysts′ performance depends on a complex combination of several materials′ characteristics. These features may lead to different reaction pathways depending on the pre‐treatment of the samples.

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Section: Resultsmentioning

confidence: 99%

Towards the Effect of Pt⁰/Pt^δ+ and Ce³⁺ Species at the Surface of CeO₂ Crystals: Understanding the Nature of the Interactions under CO Oxidation Conditions

Borges

Silva²,

Braga

et al. 2021

ChemCatChem

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“…The emergence of single‐atom catalysts (SACs) can effectively utilize the platinum group metals, which are not abundant. [ 85 ] At the same time, it is necessary to maximize the utilization efficiency of precious metals for supported noble metal catalysts. [ 86–88 ] The definition of SACs is that the active center on the catalyst support is a single atom; this concept was first proposed by Zhang and coworkers.…”

Section: Loading Metals Onto Ceo2mentioning

confidence: 99%

“…DFT study found that the top site of the Au atom is the most stable site for CO adsorption. Pereira‐Hernández et al [ 85 ] reduced a Pt/CeO 2 single‐atom catalyst at 275 °C in a CO atmosphere, and some single‐atom Pt species were converted into Pt nanoparticles. They found that the presence of Pt single atoms can improve the reducibility of lattice oxygen on the CeO 2 support and Pt NPs can adsorb CO molecules.…”

Section: Loading Metals Onto Ceo2mentioning

confidence: 99%

Recent Advances of Ceria‐Based Materials in the Oxidation of Carbon Monoxide

et al. 2020

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Carbon monoxide (CO) is a toxic and harmful gas pollutant. The realization of low‐temperature CO oxidation has been the focus of research. Also, CO oxidation as a typical model reaction is conducive to the in‐depth study of the catalytic reaction mechanism. Due to its unique oxygen storage/release capacity (OSC) and the easy transition between Ce3+ and Ce4+, CeO2 is widely used as a catalyst and catalyst support in many important reactions, especially the low‐temperature CO oxidation reaction. Herein, the application of cerium‐based materials in low‐temperature CO oxidation and CeO2 activity enhancement strategies in recent years are elaborated upon, including metal loading, adjustment of exposed facets of CeO2, and metal doping, through metal‐support interaction and the generation of oxygen vacancies on the CeO2 surface to improve the CO oxidation activity of cerium‐based catalysts. At the end of the review, the synthesis of Ce‐based materials and their applications and challenges in the field of CO oxidation are looked at.

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“…Thus, it is essential that the usage of noble metals is reduced and that their high catalytic activity is simultaneously retained. An effective way to maximize atom utilization is to reduce the particle size to atomically dispersed atoms [2–15] . Single‐atom catalysts (SACs) have been recently rising as a new frontier in the catalysis field.…”

Section: Introductionmentioning

confidence: 99%

“…An effective way to maximize atom utilization is to reduce the particle size to atomically dispersed atoms. [2][3][4][5][6][7][8][9][10][11][12][13][14][15] Single-atom catalysts (SACs) have been recently rising as a new frontier in the catalysis field. The discovery of SACs can be traced back for decades.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Wang

Liu

2020

ChemCatChem

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Single‐atom catalysts (SACs) have been rising recently as a new frontier in the catalysis field. Due to maximum atom utilization efficiency and tunable electronic structures, SACs exhibit highly distinctive catalytic performance from bulk counterparts. SACs with high metal loading will facilitate practical applications. To that end, this Review focuses on recent strategies to maximize metal loading. An appropriate substrate, mainly heteroatom‐doped carbon materials, is the key to avoiding aggregation or sintering during synthetic procedures. The coordination site construction and spatial confinement strategies are adopted to prepare SACs with high metal loading. Advanced characterization techniques with atomic resolution are indispensable for identification of the exact structure of SACs. This is true, especially for the applications and challenges in developing in situ/operando characterization techniques at the atomic level, which are discussed in this Review. Moreover, it is fundamentally necessary to investigate the active center structure, which facilitates any design of efficient SACs that can maximize single‐atom catalytic activity. Furthermore, this Review highlights challenges and prospects for development of SACs.

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Reply to: “Pitfalls in identifying active catalyst species”

Cited by 53 publications

References 14 publications

Towards the Effect of Pt⁰/Pt^δ+ and Ce³⁺ Species at the Surface of CeO₂ Crystals: Understanding the Nature of the Interactions under CO Oxidation Conditions

Towards the Effect of Pt⁰/Pt^δ+ and Ce³⁺ Species at the Surface of CeO₂ Crystals: Understanding the Nature of the Interactions under CO Oxidation Conditions

Recent Advances of Ceria‐Based Materials in the Oxidation of Carbon Monoxide

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

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Reply to: “Pitfalls in identifying active catalyst species”

Cited by 53 publications

References 14 publications

Towards the Effect of Pt0/Ptδ+ and Ce3+ Species at the Surface of CeO2 Crystals: Understanding the Nature of the Interactions under CO Oxidation Conditions

Towards the Effect of Pt0/Ptδ+ and Ce3+ Species at the Surface of CeO2 Crystals: Understanding the Nature of the Interactions under CO Oxidation Conditions

Recent Advances of Ceria‐Based Materials in the Oxidation of Carbon Monoxide

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

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Towards the Effect of Pt⁰/Pt^δ+ and Ce³⁺ Species at the Surface of CeO₂ Crystals: Understanding the Nature of the Interactions under CO Oxidation Conditions

Towards the Effect of Pt⁰/Pt^δ+ and Ce³⁺ Species at the Surface of CeO₂ Crystals: Understanding the Nature of the Interactions under CO Oxidation Conditions