4.8 Article

Space-Confined Self-Regulation Mechanism from a Capsule Catalyst to Realize an Ethanol Direct Synthesis Strategy

Journal

ACS CATALYSIS
Volume 10, Issue 2, Pages 1366-1374

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b02891

Keywords

tandem reaction; ethanol synthesis; dimethyl ether; syngas; capsule catalyst

Funding

  1. ACT-C of Japan Science and Technology Agency [JPMJCR12YT]
  2. CREST of Japan Science and Technology Agency [17-141003297]
  3. MIRAI of Japan Science and Technology Agency [JPMJMI17E2]
  4. JST-SATREPS project
  5. National Natural Science Foundation of China [91645113, 21978312]
  6. Key Research Program of Frontier Sciences, CAS [QYZDB-SSW-JSC043]

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A capsule catalyst, being composed of a catalytic zeolite membrane and a catalyst core, can accomplish multiple catalysis reactions or several organic synthesis reactions in a single step, enhancing energy efficiency, erasing unnecessary separation engineering, and creating many unexpected synergistic effects via tandem catalysis. This report discloses an ethanol synthesis strategy from syngas (CO + H-2) and syngas-derived dimethyl ether (DME) by a tailor-made catalyst with a macroscopic capsule structure. The macroscopically designed capsule catalyst consisted of a millimeter-sized Cu/ZnO core and a micrometer-sized H-Mordenite zeolite shell. The catalyst preparation process further successfully fabricated a zeolite shell, migrated a few Cu from the core, as the promoter of the shell, to significantly improve the catalyst performance. As the methanol byproduct can be easily recycled to DME as a reactant via a simple dehydration reaction, ethanol selectivity can reach 100% theoretically. It is demonstrated that a space-confined-self-regulation mechanism derived from a macroscopic capsule structure serves as a multifunctional switch to manipulate tandem reactions: arranging reaction steps in a favorable order and depressing side reactions simultaneously. These findings will inspire designing a heterogeneous catalyst with multiple functions, shortening the organic or catalytic synthesis route, and also open an avenue to ethanol synthesis from syngas, as DME is also simply produced from syngas.

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