Leveraging the Proximity and Distribution of Cu−Cs Sites for Direct Conversion of Methanol to Esters/Aldehydes

Author:

Chen Wenyao1,Zuo Ji1,Sang Keng1,Qian Gang1,Zhang Jing1,Chen De2,Zhou Xinggui1,Yuan Weikang1,Duan Xuezhi1ORCID

Affiliation:

1. State Key Laboratory of Chemical Engineering School of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

2. Department of Chemical Engineering Norwegian University of Science and Technology 7491 Trondheim Norway

Abstract

AbstractMethanol serves as a versatile building‐block for various commodity chemicals, and the development of industrially promising strategies for its conversion remains the ultimate goal in methanol chemistry. In this study, we design a dual Cu−Cs catalytic system that enables a one‐step direct conversion of methanol and methyl acetate/ethanol into high value‐added esters/aldehydes, with customized chain length and saturation by leveraging the proximity and distribution of Cu−Cs sites. Cu−Cs at a millimeter‐scale intimacy triggers methanol dehydrogenation and condensation, involving proton transfer, aldol formation, and aldol condensation, to obtain unsaturated esters and aldehydes with selectivities of 76.3 % and 31.1 %, respectively. Cu−Cs at a micrometer‐scale intimacy significantly promotes mass transfer of intermediates across catalyst interfaces and their subsequent hydrogenation to saturated esters and aldehydes with selectivities of 67.6 % and 93.1 %, respectively. Conversely, Cu−Cs at a nanometer‐scale intimacy alters reaction pathway with a similar energy barrier for the rate‐determining step, but blocks the acidic‐basic sites and diverts the reaction to byproducts. More importantly, an unprecedented quadruple tandem catalytic production of methyl methacrylate (MMA) is achieved by further tailoring Cu and Cs distribution across the reaction bed in the configuration of Cu−Cs||Cs, outperforming the existing industrial processes and saving at least 15 % of production costs.

Funder

Key Technologies Research and Development Program

National Natural Science Foundation of China

Program of Shanghai Academic Research Leader

Science and Technology Innovation Plan Of Shanghai Science and Technology Commission

Publisher

Wiley

Subject

General Chemistry,Catalysis

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