{"title":"Cycloaddition of limonene epoxide and CO2 over Zn/SBA-15 catalysts for limonene carbonate synthesis","authors":"Carina Mosquera, Aída Luz Villa","doi":"10.1016/j.jcou.2024.102817","DOIUrl":null,"url":null,"abstract":"<div><p>The cycloaddition reaction of CO<sub>2</sub> with epoxides such as limonene epoxide (LE) to form cyclic carbonates is considered a promising alternative for reducing CO<sub>2</sub> emissions. In this work, CO<sub>2</sub> fixation on LE to produce cyclic carbonates was carried out over Zn/SBA-15 with tetrabutylammonium bromide (TBAB) as co-catalyst and over NH<sub>3</sub>X-Zn/SBA-15 (X= Cl, Br, or I) catalysts. The catalysts were characterized by FT-IR, XRD, N<sub>2</sub> adsorption–desorption isotherms, TEM, NH<sub>3</sub>-TPD, XPS, TGA and Py-FTIR. The Zn/SBA-15 support mainly presents Lewis’s acid sites of medium acidity; the surface area was 512 m<sup>2</sup>/g and 378 m<sup>2</sup>/g and the pore size were 9 nm and 7.2 nm, for Zn/SBA-15 and NH<sub>3</sub>Cl-Zn/SBA-15, respectively. The functionalization of Zn/SBA-15 was verified by FTIR, UV-vis, and XPS analysis. It was found that when Zn/SBA-15 was used as catalyst that reaction time had a significative effect on LE conversion and in the case of limonene carbonate selectivity, co-catalyst concentration variation had the main effect. Zn/SBA-15 catalyst can be reused up to 5 times without significant changes neither in conversion nor in limonene carbonate selectivity. The best LE conversion and limonene carbonate selectivity was 33% and 93%, respectively (1 M LE, 200 mg Zn/SBA-15, 7% TBAB; 30 bar, 18 h, 700 rpm and 20 mL diethyl carbonate). The reported catalytic system is a promising system for obtaining limonene carbonate using a heterogeneous catalyst.</p></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2212982024001525/pdfft?md5=116508844f4fbede31cd7f651156a3ab&pid=1-s2.0-S2212982024001525-main.pdf","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of CO2 Utilization","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2212982024001525","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The cycloaddition reaction of CO2 with epoxides such as limonene epoxide (LE) to form cyclic carbonates is considered a promising alternative for reducing CO2 emissions. In this work, CO2 fixation on LE to produce cyclic carbonates was carried out over Zn/SBA-15 with tetrabutylammonium bromide (TBAB) as co-catalyst and over NH3X-Zn/SBA-15 (X= Cl, Br, or I) catalysts. The catalysts were characterized by FT-IR, XRD, N2 adsorption–desorption isotherms, TEM, NH3-TPD, XPS, TGA and Py-FTIR. The Zn/SBA-15 support mainly presents Lewis’s acid sites of medium acidity; the surface area was 512 m2/g and 378 m2/g and the pore size were 9 nm and 7.2 nm, for Zn/SBA-15 and NH3Cl-Zn/SBA-15, respectively. The functionalization of Zn/SBA-15 was verified by FTIR, UV-vis, and XPS analysis. It was found that when Zn/SBA-15 was used as catalyst that reaction time had a significative effect on LE conversion and in the case of limonene carbonate selectivity, co-catalyst concentration variation had the main effect. Zn/SBA-15 catalyst can be reused up to 5 times without significant changes neither in conversion nor in limonene carbonate selectivity. The best LE conversion and limonene carbonate selectivity was 33% and 93%, respectively (1 M LE, 200 mg Zn/SBA-15, 7% TBAB; 30 bar, 18 h, 700 rpm and 20 mL diethyl carbonate). The reported catalytic system is a promising system for obtaining limonene carbonate using a heterogeneous catalyst.
期刊介绍:
The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials.
The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications.
The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.