(63m) Copper-Phyllosilicate Core-Shell Nanocatalysts with Balanced Active Sites for Carbon-Oxygen Hydrogenolysis Reactions

Copper-Phyllosilicate Core-shell Nanocatalysts with Balanced
Active Sites for Carbon-Oxygen
Hydrogenolysis Reactions

Hairong Yue, Weimao Fang, Changmin Liu, Jiankang Ying

College of Chemical Engineering, Sichuan University, Chengdu, China

Email: hryue@scu.edu.cn

Abstract

Hydrogenolysis of carbon-oxygen (C¨CO) bonds (e.g.,
esters, ethers, furfural, and CO₂) has emerged as a versatile synthetic
tool in organic methodology, as it could produce a variety of products (e.g.,
chemicals, fuels, and polymers). Copper-based catalysts have been intensively explored for hydrogenation
reactions as the copper sites
account for the selective hydrogenation of carbon-oxygen bonds and relatively
inactive for the hydrogenolysis of carbon-carbon bonds. Work on
understanding the active sites of copper catalysts for hydrogenation reactions indicted that both Cu⁰ and
Cu⁺ species were crucial to the activity of Cu-based
catalysts. However, researchers were not able to establish a relationship
between activity and Cu⁰/Cu⁺ active species since the conventional Cu-based
catalysts is the deactivation by metal particle growth and unstable surface Cu⁰
and Cu⁺ active species in the strong reductive H₂ and
oxidizing carbon-oxygen atmosphere.

We renctly
present on efficient approaches for fabrication of a series of copper-phyllosilicate core-shell nanocatalysts and
nanoreactors with balanced and stable Cu⁰ and Cu⁺
active species. We chose the hydrogenation
of dimethyl oxalate, ethylene cyclicarbonate
and as probe reactions for a better understanding of properties of active sites
and the structure-activity relationship. The results indicated a synergy between copper
and the oxide components and the balanced surface Cu⁰ and Cu⁺
species can greatly improve the catalytic C-O hydrogenolysis performance of the
catalysts. These nanocatalysts with
balanced and stable Cu⁰ and Cu⁺ active species, confinement effect,
intrinsic high surface of Cu⁰ and Cu⁺ and unique tunable tubular
morphology, has potential applications in the high-temperature hydrogenation reactions.

Keywords: core-shell nanocatalysts,
Hydrogenation reaction;
copper catalyst

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