Synthesis of diethyl carbonate from CO2 and orthoester promoted by a CeO2 catalyst and ethanol

Wahyu S. Putro, Yusuke Munakata, Seiichiro Ijima, Shinji Shigeyasu, Satoshi Hamura, Seiji Matsumoto, Takayoshi Mishima, Keiichi Tomishige, Jun Chul Choi, Norihisa Fukaya

Research output: Contribution to journalArticlepeer-review

Abstract

The combination of a CeO2 catalyst and ethanol effectively promotes the direct synthesis of diethyl carbonate (DEC) from CO2 and an orthoester. The reaction temperature, initial CO2 pressure, and the ethanol/orthoester volume ratio were found to significantly influence DEC formation and were systematically studied to determine the optimum conditions. DEC amount of 5.2 mmol was obtained at 160 °C, 5 MPa of CO2, and a reaction time of 20 h, providing high productivity (1.21 mmolDEC mmolcatalyst−1 h−1) using a CeO2 catalyst. The recovered CeO2 catalyst was recyclable at least four times without any significant loss of activity when both triethyl orthoacetate and triethyl orthovalerate were used. A series of orthoesters bearing various alkyl substituents, aromatic substituents and halide moieties were evaluated for their activities with and without ethanol. In the presence of ethanol, orthoesters bearing longer alkyl substituents led to higher DEC yields, and orthoesters bearing aromatic and halide moieties negatively impacted DEC formation. In the absence of ethanol, triethyl orthoacetate provided the highest DEC yield; in all cases, the use of ethanol resulted in a greater DEC formation than when the reaction was performed without ethanol.

Original languageEnglish
Article number101818
JournalJournal of CO2 Utilization
Volume55
DOIs
Publication statusPublished - 2022 Jan

Keywords

  • CO
  • CeO catalyst
  • Diethyl carbonate
  • Ethanol
  • Orthoester

ASJC Scopus subject areas

  • Chemical Engineering (miscellaneous)
  • Waste Management and Disposal
  • Process Chemistry and Technology

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