Rationally designing mixed Cu–(μ-O)–M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation

Literature Information

Publication Date 2018-09-27
DOI 10.1039/C8CP04872J
Impact Factor 3.676
Authors

Ling Huang, Jian Zhou, Anmin Zheng


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Abstract

The direct conversion of methane to methanol on [Cu(μ-O)M]2+ (M = Cu, Ag, Zn, Au) bimetal centers in ZSM-5 zeolite is investigated using periodic density functional theory for the first time. Some conclusions are drawn: (1) methane activation on [Cu(μ-O)M]2+ (M = Cu, Ag, Zn, Au) in the ZSM-5 zeolite proceeds through radical-like transition states, and the ability for CH4 activation decreases in the sequence [Cu(μ-O)Ag]2+ > [Cu(μ-O)Au]2+ > [Cu(μ-O)Cu]2+ > [Cu(μ-O)Zn]2+. (2) There are two factors that can dramatically enhance C–H bond activation: a greater spin density and a less negative charge of the μ-O atom. (3) The angles ∠CuOM play a minor role in the reactivity difference among [CuOM]2+–ZSM-5 (M = Cu, Ag, Zn, Au). Our findings will provide insight into methane activation for designing highly effective catalysts applied in industrial processes.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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