☆ 4.7 Article

Investigation of the Active-Site Structure of Cu-CHA Catalysts for the Direct Oxidation of Methane to Methanol Using In Situ UV-Vis Spectroscopy

ENERGY & FUELS (2023)

相关参考文献

注意：仅列出部分参考文献，下载原文获取全部文献信息。

Article Chemistry, Physical

Oxidation of Methane to Methanol by Water Over Cu/SSZ-13: Impact of Cu Loading and Formation of Active Sites

Hailong Zhang et al.

Summary: Cu/SSZ-13 catalysts with different Cu loadings (1-5 wt.%) were prepared and their catalytic performance for the direct conversion of methane to methanol was investigated. The results showed that the catalytic performance depended on the Cu loading, with 2 wt.% Cu presenting the best performance. CuO nanoparticles, CuxOy clusters, and monomeric [CuOH](+) species were observed on Cu/SSZ-13 catalysts. The high coverage of CuO nanoparticles on the catalyst with 5 wt.% Cu resulted in the loss of catalytic reactivity, despite the presence of active CuxOy and [CuOH](+) sites. The improved catalytic performance in the cyclic stepwise process was attributed to the re-dispersion of CuO nanoparticles and/or large clusters, as well as the re-oxidation of Cu(I) cations from the self-reduction of [CuOH](+) species.

CHEMCATCHEM (2022)

添加到收藏夹

Article Chemistry, Physical

Relationships among the Catalytic Performance, Redox Activity, and Structure of Cu-CHA Catalysts for the Direct Oxidation of Methane to Methanol Investigated Using In Situ XAFS and UV-Vis Spectroscopies

Junya Ohyama et al.

Summary: The catalytic performance of Cu zeolites for the direct conversion of methane to methanol was investigated. The reduction rate of Cu-CHA was found to be highly correlated with catalytic activity. The reduction of Cu2+ is associated with the activation of C-H bonds in CH4, which is the rate-determining step for the reaction. The local structure of Cu-CHA affects selectivity, turnover frequency, and Cu2+ reduction rate.

ACS CATALYSIS (2022)

添加到收藏夹

Article Chemistry, Physical

Speciation of Cu-Oxo Clusters in Ferrierite for Selective Oxidation of Methane to Methanol

Lei Tao et al.

Summary: Cu-oxo nanoclusters in Cu-exchanged ferrierite act as active sites for the oxidation of methane to methanol via a three-step process. These active sites are dimeric Cu clusters stabilized at pairs of negatively charged aluminum oxygen tetrahedra.

CHEMISTRY OF MATERIALS (2022)

添加到收藏夹

Article Chemistry, Physical

Selective Catalytic Reduction of NOx with NH3 over Cu/SSZ-13: Elucidating Dynamics of Cu Active Sites with In Situ UV-Vis Spectroscopy and DFT Calculations

Yani Zhang et al.

Summary: In this study, we use in situ UV-vis spectroscopic studies combined with theoretical calculations to investigate the transformation behavior of Z(2)Cu(II) and ZCu(II)OH active sites in Cu/SSZ-13 catalyst under SCR-relevant conditions. We find that ZCu(II)OH readily transforms into a double O-bridged dicopper species, while Z(2)Cu(II) does not undergo such a transformation. Despite these differences, both species exhibit similar spectroscopic features under NH3 oxidation and NH3-SCR conditions, providing important information for understanding the NH3-SCR mechanism and catalyst design.

JOURNAL OF PHYSICAL CHEMISTRY C (2022)

添加到收藏夹

Article Engineering, Chemical

Hetero-Metallic Active Sites in Omega (MAZ) Zeolite-Catalyzed Methane Partial Oxidation: A DFT Study

Linzhe Wang et al.

Summary: This study investigates the doping of transition metals Pd, Pt, Fe, Co, Ni, Au, and Ag in dinuclear active sites in Cu-exchanged MAZ zeolite. The calculated process of [Cu-O-M](2+)-MAZ-catalyzed methane partial oxidation is discussed, along with the geometric and electronic structural properties of hetero-metallic [Cu-O-M](2+) and various activity descriptors for reactivity. The results demonstrate an efficient method for enhancing the catalytic performance of Cu-exchanged MAZ zeolite in methane direct conversion to methanol.

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH (2021)

添加到收藏夹

Article Chemistry, Physical

First-Principles Calculations of Condition-Dependent Cu/Fe Speciation in Sulfur-Poisoned Cu- and Fe-SSZ-13 Catalysts

Vitaly Mesilov et al.

Summary: A combination of first-principles thermodynamics and density functional theory was used to predict sulfur-poisoned monomeric Cu/Fe species formed in the SSZ-13 catalyst framework. Differences in fresh and sulfur-poisoned species were found for Cu- and Fe-SSZ-13 catalysts containing different amounts of Al in 6-membered or 8-membered rings. The impact of ammonia concentration on Cu- and Fe-speciation was also investigated.

JOURNAL OF PHYSICAL CHEMISTRY C (2021)

添加到收藏夹

Review Chemistry, Multidisciplinary

Methane Oxidation to Methanol in Water

Simon J. Freakley et al.

Summary: Methane oxidation to methanol is a challenging topic due to high energy barriers and prevention of overoxidation to CO2. Over the past 50 years, low-temperature selective methane oxidation to methanol has remained an active area of research. Studies show that using molecular oxygen is more ideal, but there are still challenges in research on this aspect.

ACCOUNTS OF CHEMICAL RESEARCH (2021)

添加到收藏夹

Article Chemistry, Multidisciplinary

Spectroscopic Definition of a Highly Reactive Site in Cu-CHA for Selective Methane Oxidation: Tuning a Mono-μ-Oxo Dicopper(II) Active Site for Reactivity

Hannah M. Rhoda et al.

Summary: Experimental and theoretical studies show that the [Cu2O](2+) core in Cu-CHA exhibits higher reactivity towards methane to form methanol compared to the [Cu2O](2+) core in Cu-MFI, attributed to the stronger [Cu2OH](2+) bond and the relative orientation of coordinating bidentate O-Al-O T-sites. This work provides insights into how zeolite lattice constraints can impact active site reactivity.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

添加到收藏夹

Article Chemistry, Physical

Effect of the Co-cation on Cu Speciation in Cu-Exchanged Mordenite and ZSM-5 Catalysts for the Oxidation of Methane to Methanol

Gordon Brezicki et al.

Summary: This study demonstrates that the identity of the co-cation (H vs Na) significantly influences the Cu speciation and reactivity in Cu-MOR and Cu-ZSM-S catalysts. The choice of co-cation can be used to control active site structure and affect the selectivity of methane conversion to methanol.

ACS CATALYSIS (2021)

添加到收藏夹

Article Chemistry, Physical

Highly Selective Oxidation of Methane into Methanol over Cu-Promoted Monomeric Fe/ZSM-5

Tao Yu et al.

Summary: The study demonstrates that the Cu-modified Fe/ZSM-5 catalyst is highly efficient for the direct conversion of methane into methanol in the liquid phase using H2O2 as an oxidant. Cu species in the catalyst play a crucial role in facilitating the formation of .OH radicals, which react quickly with .CH3 radicals to form methanol. This provides valuable insights into the rational design of metal-zeolite combinations for the selective oxidation of methane into methanol.

ACS CATALYSIS (2021)

添加到收藏夹

Article Chemistry, Physical

Thermodynamics Perspective on the Stepwise Conversion of Methane to Methanol over Cu-Exchanged SSZ-13

Florian Goltl et al.

Summary: Transition-metal exchanged zeolites show high selectivity in converting methane to methanol through a stepwise process. A comprehensive theoretical study is conducted to identify thermodynamically preferred active sites in Cu-exchanged zeolite SSZ-13 during the conversion and develop a thermodynamic model for different active sites anchored in various structures supported by different local Al distributions. The results are compared with experimental measurements, showing agreement and providing insights for optimizing the conversion process.

ACS CATALYSIS (2021)

添加到收藏夹

Article Chemistry, Physical

Cu-Erionite Zeolite Achieves High Yield in Direct Oxidation of Methane to Methanol by Isothermal Chemical Looping

Jie Zhu et al.

CHEMISTRY OF MATERIALS (2020)

添加到收藏夹

Article Chemistry, Inorganic & Nuclear

Methane Activation on H-ZSM-5 Zeolite with Low Copper Loading. The Nature of Active Sites and Intermediates Identified with the Combination of Spectroscopic Methods

Anton A. Gabrienko et al.

INORGANIC CHEMISTRY (2020)

添加到收藏夹

Article Nanoscience & Nanotechnology

Methane Utilization to Methanol by a Hybrid Zeolite@Metal-Organic Framework

Thidarat Imyen et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

添加到收藏夹

Article Chemistry, Multidisciplinary

Structure and Reactivity of Oxygen-Bridged Diamino Dicopper(II) Complexes in Cu-Ion-Exchanged Chabazite Catalyst for NH3-Mediated Selective Catalytic Reduction

Chiara Negri et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

添加到收藏夹

Article Chemistry, Applied

Evolution of active sites during selective oxidation of methane to methanol over Cu-CHA and Cu-MOR zeolites as monitored by operando XAS

Elisa Borfecchia et al.

CATALYSIS TODAY (2019)

添加到收藏夹

Article Engineering, Chemical

Methane-to-Methanol via Chemical Looping: Economic Potential and Guidance for Future Research

Jean-Paul Lange et al.

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH (2019)

添加到收藏夹

Article Chemistry, Physical

Insights into the Speciation of Cu in the Cu-H-Mordenite Catalyst for the Oxidation of Methane to Methanol

Gordon Brezicki et al.

ACS CATALYSIS (2019)

添加到收藏夹

Article Chemistry, Physical

First-Principles Study of Oxidation State and Coordination of Cu-Dimers in Cu-SSZ-13 during Methane-to-Methanol Reaction Conditions

Unni Engedahl et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2019)

添加到收藏夹

Article Chemistry, Physical

Al Organization in the SSZ-13 Zeolite. Al Distribution and Extraframework Sites of Divalent Cations

Kinga Mlekodaj et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2019)

添加到收藏夹

Article Chemistry, Multidisciplinary

Second-Sphere Effects on Methane Hydroxylation in Cu-Zeolites

Benjamin E. R. Snyder et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2018)

添加到收藏夹

Article Chemistry, Physical

Direct Stepwise Oxidation of Methane to Methanol over Cu-SiO2

Selmi E. Bozbag et al.

ACS CATALYSIS (2018)

添加到收藏夹

Article Chemistry, Physical

Direct Methane to Methanol: The Selectivity-Conversion Limit and Design Strategies

Allegra A. Latimer et al.

ACS CATALYSIS (2018)

添加到收藏夹

Review Chemistry, Multidisciplinary

Theoretical Overview of Methane Hydroxylation by Copper-Oxygen Species in Enzymatic and Zeolitic Catalysts

M. Haris Mahyuddin et al.

ACCOUNTS OF CHEMICAL RESEARCH (2018)

添加到收藏夹

Article Chemistry, Multidisciplinary

On the Mechanism Underlying the Direct Conversion of Methane to Methanol by Copper Hosted in Zeolites; Braiding Cu K-Edge XANES and Reactivity Studies

Mark A. Newton et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2018)

添加到收藏夹

Article Chemistry, Multidisciplinary

The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment

Dimitrios K. Pappas et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2018)

添加到收藏夹

Article Chemistry, Multidisciplinary

Methane to Methanol: Structure Activity Relationships for Cu-CHA

Dimitrios K. Pappas et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2017)

添加到收藏夹

Article Chemistry, Physical

Formation of [Cu2O2]2+ and [Cu2O]2+ toward C-H Bond Activation in Cu-SSZ-13 and Cu-SSZ-39

Bahar Ipek et al.

ACS CATALYSIS (2017)

添加到收藏夹

Article Chemistry, Physical

Roles of Zeolite Confinement and Cu-O-Cu Angle on the Direct Conversion of Methane to Methanol by [Cu2(μ-O)]2+-Exchanged AEI, CHA, AFX, and MFI Zeolites

M. Haris Mahyuddin et al.

ACS CATALYSIS (2017)

添加到收藏夹

Article Chemistry, Multidisciplinary

Catalysis in a Cage: Condition-Dependent Speciation and Dynamics of Exchanged Cu Cations in SSZ-13 Zeolites

Christopher Paolucci et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2016)

添加到收藏夹

Article Chemistry, Physical

Roles of Water Molecules in Modulating the Reactivity of Dioxygen-Bound Cu-ZSM-5 toward Methane: A Theoretical Prediction

Takashi Yumura et al.

ACS CATALYSIS (2016)

添加到收藏夹

Article Chemistry, Physical

Monocopper Active Site for Partial Methane Oxidation in Cu-Exchanged 8MR Zeolites

Ambarish R. Kulkarni et al.

ACS CATALYSIS (2016)

添加到收藏夹

Article Chemistry, Physical

Methane Activation by Heterogeneous Catalysis

Raimund Horn et al.

CATALYSIS LETTERS (2015)

添加到收藏夹

Article Chemistry, Physical

Reaction Conditions of Methane-to-Methanol Conversion Affect the Structure of Active Copper Sites

Evalyn Mae C. Alayon et al.

ACS CATALYSIS (2014)

添加到收藏夹

Article Chemistry, Inorganic & Nuclear

Characterization of Cu-exchanged SSZ-13: a comparative FTIR, UV-Vis, and EPR study with Cu-ZSM-5 and Cu-beta with similar Si/Al and Cu/Al ratios

Filippo Giordanino et al.

DALTON TRANSACTIONS (2013)

添加到收藏夹

Article Chemistry, Inorganic & Nuclear

Role of Tyrosine Residue in Methane Activation at the Dicopper Site of Particulate Methane Monooxygenase: A Density Functional Theory Study

Yoshihito Shiota et al.

INORGANIC CHEMISTRY (2013)

添加到收藏夹

Article Chemistry, Applied

Direct methane conversion routes to chemicals and fuels

M. C. Alvarez-Galvan et al.

CATALYSIS TODAY (2011)

添加到收藏夹

Article Chemistry, Multidisciplinary

Oxygen Precursor to the Reactive Intermediate in Methanol Synthesis by Cu-ZSM-5

Pieter J. Smeets et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2010)

添加到收藏夹

News Item Multidisciplinary Sciences

Natural Gas From Shale Bursts Onto the Scene

Richard A. Kerr

SCIENCE (2010)

添加到收藏夹

Article Chemistry, Applied

Direct conversion of methane to fuels and chemicals

Anders Holmen

CATALYSIS TODAY (2009)

添加到收藏夹

Article Chemistry, Inorganic & Nuclear

Comparison of the Reactivity of Bis(μ-oxo)CuIICuIII and CuIIICuIII Species to Methane

Yoshihito Shiota et al.

INORGANIC CHEMISTRY (2009)

添加到收藏夹

Article Multidisciplinary Sciences

A [Cu2O]2+ core in Cu-ZSM-5, the active site in the oxidation of methane to methanol

Julia S. Woertink et al.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2009)

添加到收藏夹

Article Chemistry, Multidisciplinary

Selective oxidation of methane by the bis(μ-oxo)dicopper core stabilized on ZSM-5 and mordenite zeolites

MH Groothaert et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2005)

添加到收藏夹

© Peeref 2019-2024. All rights reserved.