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The combination catalyst of CeO2 and H-FAU zeolite was effective for the direct synthesis of diethyl carbonate from CO2 and ethanol with 2,2-diethoxypropane as a dehydrating regent, where H-FAU catalyzed hydrolysis of 2,2-diethoxypropane. The combination catalyst provided high activity and a high diethyl carbonate yield of 72% based on 2,2-diethoxypropane at a low temperature of 393 K. [ABSTRACT FROM AUTHOR]

Keywords: alkoxysilane; carbon dioxide; diethyl carbonate; sustainable catalytic synthesis; Zr catalysts EN alkoxysilane carbon dioxide diethyl carbonate sustainable catalytic synthesis Zr catalysts 755 755 1 02/17/21 20210205 NES 210205 B The Cover Feature b shows the new synthesis of diethyl carbonate from CO SB 2 sb and alkoxysilanes using a zirconium catalyst. Alkoxysilane, carbon dioxide, diethyl carbonate, sustainable catalytic synthesis, Zr catalysts. [Extracted from the article]

A heterogeneous zirconium catalyst was grafted on a ceria‐coated silica support, denoted as Zr(OEt)x/CeO2/SiO2. It exhibited higher catalytic activity compared to its homogeneous counterpart, Zr(OEt)4, in the conversion of carbon dioxide to diethyl carbonate using tetraethyl orthosilicate as a regenerable agent in the absence of any dehydrating agents under non‐protic conditions. We found that the ceria‐coated silica (CeO2/SiO2) support not only improved the catalytic activity of Zr(OEt)4 but also inhibited catalyst deactivation during catalyst recycling tests. Furthermore, we analyzed the surface of the Zr(OEt)x/CeO2/SiO2 catalysts by FE‐SEM and EDX. [ABSTRACT FROM AUTHOR]

Direct conversion of CO 2 to dialkyl carbonates such as diethyl carbonate (DEC) can contribute to mitigate CO 2 emissions. We previously proposed a new DEC synthesis method from the reaction of CO 2 and tetraethoxysilane (TEOS), an expensive functional chemical. After being used for DEC synthesis, TEOS can be regenerated from reaction of ethanol and hexaethoxy disiloxane (DS), the byproduct produced along with DEC. However, TEOS regeneration requires several processing units and high energy demand. In this study, we designed and evaluated feasibility of this new DEC synthesis process. Based on data obtained from lab experiments, the entire process, which comprised DEC synthesis and TEOS regeneration sections, was designed and optimized using process simulator Pro/II. Cradle-to-gate life cycle assessment method was applied to comprehensively evaluate the total CO 2 emissions caused by the consumption of raw materials and utilities in DEC synthesis and TEOS regeneration sections. In addition, the total production cost was evaluated. On the basis of the evaluation results, process hotspots were identified. Optimal conditions used for TEOS regeneration (ethanol/DS = 18.2) were proposed to improve total process performances. The total production cost and CO 2 emissions are 1.7 $/kg DEC, 3.6 kg CO 2 /kg DEC, respectively. The new process was compared to the most commonly used process which synthesizes DEC from the reaction of CO 2 with ethanol, assisted by the dehydrating agent 2-cyanopyridine. Our results show that the new DEC synthesis process gains higher economic and environmental viability. • A new process synthesizing DEC from CO 2 and TEOS was rigorously designed. • Economic viability and potential CO 2 emissions reduction were evaluated. • Regeneration of TEOS was the key to enhancing total process feasibility. • Optimal regeneration condition was found to reduce both cost and CO 2 emissions. • The new process can be a competitive alternative for DEC synthesis. [ABSTRACT FROM AUTHOR]