An alternative catalytic cycle for selective methane oxidation to methanol with Cu clusters in zeolites

Gallego, Mario; Corma, Avelino; Boronat, Mercedes

doi:10.1039/d3cp05802f

Cited by 4 publications

(1 citation statement)

References 43 publications

(55 reference statements)

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“…241 Additionally, many techniques and analyses have been applied for this purpose, ranging from rR spectroscopy, isotope labelling experiments and DFT calculations and machine learning. 242,243 The aim of this section is to present the approach dealing with the parameters mentioned above towards a better understanding covering the reusability of the zeolitescontaining copper-heterogenized systems. Cu-O species immobilized in zeolites micropores have been shown to be efficient catalysts for the selective oxidation of methane, among other substrates.…”

Section: Materials Framework For the Immobilization Of Copper-oxygen ...mentioning

confidence: 99%

Copper–oxygen adducts: new trends in characterization and properties towards C–H activation

De Tovar,

Leblay,

Wang

et al. 2024

Chem. Sci.

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Section: Materials Framework For the Immobilization Of Copper-oxygen ...mentioning

confidence: 99%

Copper–oxygen adducts: new trends in characterization and properties towards C–H activation

De Tovar,

Leblay,

Wang

et al. 2024

Chem. Sci.

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Mechanistic Studies of Continuous Partial Methane Oxidation on Cu−Zeolites Using Kinetic and Spectroscopic Methods

Mikes,

Kilburn,

Gounder

2024

ChemCatChem

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Over the past few decades, a significant amount of research effort has focused on investigating the active site requirements and reaction mechanisms for partial methane oxidation (PMO) to methanol over copper‐exchanged zeolites during stoichiometric and stepwise chemical looping routes. More recently, research efforts have expanded to include investigating the PMO reaction in a continuous catalytic regime, primarily focusing on determining the influence of catalyst composition on Cu speciation and structure and, in turn, on PMO rate and selectivity. The structures of candidate Cu active sites are commonly studied using a combination of ex situ and in situ spectroscopic approaches. In this perspective, we critically examine the prior literature on catalytic PMO over Cu‐zeolites to identify key knowledge gaps that remain in our understanding as motivation for future research efforts. We identify opportunities for future research to address these gaps by adapting analogous interrogation techniques that have been successfully used to elucidate the active site requirements and mechanistic details of another catalytic redox reaction cycle on Cu‐zeolites, the selective catalytic reduction (SCR) of nitrogen oxides (NOx).

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An Ab Initio Journey toward the Molecular‐Level Understanding and Predictability of Subnanometric Metal Clusters

de Lara‐Castells

2024

Small Structures

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Current advances in synthesizing and characterizing atomically precise monodisperse metal clusters (AMCs) at the subnanometer scale have opened up new possibilities in quantum materials research. Their quantizied “molecule‐like” electronic structure showcases unique stability, and physical and chemical properties differentiate them from larger nanoparticles. When integrated into inorganic materials that interact with the environment and sunlight, AMCs serve to enhance their (photo)catalytic activity and optoelectronic properties. Their tiny size makes AMCs isolated in the gas phase amenable to atom‐scale modeling using either density functional theory (DFT) or methods at a high level of ab initio theory, even addressing nonadiabatic (e.g., Jahn–Teller) effects. Surface‐supported AMCs can be routinely modeled using DFT, enabling long real‐time molecular dynamics simulations. Their optical properties can also be addressed using time‐dependent DFT or reduced density matrix (RDM) theory. These theoretical–computational efforts aim to achieve predictability and molecular‐level understanding of the stability and properties of AMCs as function of their composition, size, and structural fluxionality in different thermodynamical conditions (temperature and pressure). In this perspective, the potential of ab initio and DFT‐based modeling is illustrated through recent studies of unsupported and surface‐supported AMCs. Future directions of research are also discussed, including applications and methodological enhancements beyond the state‐of‐the‐art.

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An alternative catalytic cycle for selective methane oxidation to methanol with Cu clusters in zeolites

Abstract: The limited activation of O2 on Cu5 clusters supported on CHA zeolite favors the selective oxidation of methane to methanol.

Cited by 4 publications

References 43 publications

Copper–oxygen adducts: new trends in characterization and properties towards C–H activation

Copper–oxygen adducts: new trends in characterization and properties towards C–H activation

Mechanistic Studies of Continuous Partial Methane Oxidation on Cu−Zeolites Using Kinetic and Spectroscopic Methods

An Ab Initio Journey toward the Molecular‐Level Understanding and Predictability of Subnanometric Metal Clusters

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