{"title":"揭示 ZIF-8/ 镍负载氧化铝气凝胶催化剂在利用二氧化碳和甘油生产碳酸甘油酯中的活性","authors":"Gamze Özçakır, Çağlayan Açıkgöz","doi":"10.1007/s11164-024-05440-0","DOIUrl":null,"url":null,"abstract":"<div><p>Glycerol Carbonate (GC) production via carbonylation of glycerol with CO<sub>2</sub> reaction takes attention to its properties of enabling both the utilization of biodiesel by-product glycerol and the use of major greenhouse gas CO<sub>2</sub>. Herein, the synthesis of GC via glycerol carbonylation with CO<sub>2</sub> over a series of ZIF-8 on nickel-loaded Alumina Aerogel catalysts was examined for the first time in literature. ZIF-8 growth on nickel-impregnated Alumina aerogel was executed using an in situ method. Synthesized catalysts were analyzed using SEM–EDX, FT-IR, DRIFTS, XRD, and N<sub>2</sub> sorption techniques. The carbonylation reaction of glycerol was conducted in the presence of a co-reactant (propylene oxide) and solvent (methanol). The influence of reaction parameters (temperature, catalyst loading, glycerol/co-reactant molar ratio, co-reactant type, catalyst type, and reaction time) on the catalytic activity (glycerol conversion, GC selectivity and yield) of the catalysts were investigated. It obtained high glycerol conversion (73%) for AA-2Ni-5ZIF, yield (31%), and selectivity (77%) of GC for AA-5Ni-15ZIF under optimized reaction conditions (150 °C, 7 bar, 2 h, 6% catalyst loading and 0.5 glycerol/propylene oxide). Compared to the literature, this activity was found under lower CO<sub>2</sub> pressure and reaction time. Unique features of catalysts such as suitable acidity, high surface area, more than one active crystal, and the presence of propylene oxide as a co-reactant promoted the rise of glycerol conversion, GC selectivity, and yield.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"50 12","pages":"5655 - 5678"},"PeriodicalIF":2.8000,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Unveiling activity of ZIF-8/ nickel loaded alumina aerogel catalyst in glycerol carbonate production from CO2 and glycerol\",\"authors\":\"Gamze Özçakır, Çağlayan Açıkgöz\",\"doi\":\"10.1007/s11164-024-05440-0\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Glycerol Carbonate (GC) production via carbonylation of glycerol with CO<sub>2</sub> reaction takes attention to its properties of enabling both the utilization of biodiesel by-product glycerol and the use of major greenhouse gas CO<sub>2</sub>. Herein, the synthesis of GC via glycerol carbonylation with CO<sub>2</sub> over a series of ZIF-8 on nickel-loaded Alumina Aerogel catalysts was examined for the first time in literature. ZIF-8 growth on nickel-impregnated Alumina aerogel was executed using an in situ method. Synthesized catalysts were analyzed using SEM–EDX, FT-IR, DRIFTS, XRD, and N<sub>2</sub> sorption techniques. The carbonylation reaction of glycerol was conducted in the presence of a co-reactant (propylene oxide) and solvent (methanol). The influence of reaction parameters (temperature, catalyst loading, glycerol/co-reactant molar ratio, co-reactant type, catalyst type, and reaction time) on the catalytic activity (glycerol conversion, GC selectivity and yield) of the catalysts were investigated. It obtained high glycerol conversion (73%) for AA-2Ni-5ZIF, yield (31%), and selectivity (77%) of GC for AA-5Ni-15ZIF under optimized reaction conditions (150 °C, 7 bar, 2 h, 6% catalyst loading and 0.5 glycerol/propylene oxide). Compared to the literature, this activity was found under lower CO<sub>2</sub> pressure and reaction time. Unique features of catalysts such as suitable acidity, high surface area, more than one active crystal, and the presence of propylene oxide as a co-reactant promoted the rise of glycerol conversion, GC selectivity, and yield.</p></div>\",\"PeriodicalId\":753,\"journal\":{\"name\":\"Research on Chemical Intermediates\",\"volume\":\"50 12\",\"pages\":\"5655 - 5678\"},\"PeriodicalIF\":2.8000,\"publicationDate\":\"2024-11-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Research on Chemical Intermediates\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11164-024-05440-0\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Research on Chemical Intermediates","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s11164-024-05440-0","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
通过甘油与二氧化碳的羰基化反应生产碳酸甘油酯(GC),其既能利用生物柴油副产品甘油,又能利用主要温室气体二氧化碳的特性备受关注。本文首次在文献中研究了在镍负载氧化铝气凝胶催化剂上的一系列 ZIF-8 上通过甘油与 CO2 发生羰基化反应合成 GC 的过程。ZIF-8 在镍浸渍氧化铝气凝胶上的生长是采用原位法进行的。使用 SEM-EDX、FT-IR、DRIFTS、XRD 和 N2 吸附技术对合成的催化剂进行了分析。甘油的羰基化反应是在共反应物(环氧丙烷)和溶剂(甲醇)的存在下进行的。研究了反应参数(温度、催化剂负载、甘油/共反应物摩尔比、共反应物类型、催化剂类型和反应时间)对催化剂催化活性(甘油转化率、气相色谱选择性和产率)的影响。在优化的反应条件(150 °C, 7 bar, 2 h, 6% 催化剂负载和 0.5 甘油/环氧丙烷)下,AA-2Ni-5ZIF 获得了较高的甘油转化率(73%),AA-5Ni-15ZIF 获得了较高的产率(31%)和 GC 选择性(77%)。与文献相比,这种活性是在较低的 CO2 压力和反应时间下实现的。催化剂的独特特性,如合适的酸性、高比表面积、不止一种活性晶体,以及环氧丙烷作为共反应物的存在,促进了甘油转化率、气相色谱选择性和产率的提高。
Unveiling activity of ZIF-8/ nickel loaded alumina aerogel catalyst in glycerol carbonate production from CO2 and glycerol
Glycerol Carbonate (GC) production via carbonylation of glycerol with CO2 reaction takes attention to its properties of enabling both the utilization of biodiesel by-product glycerol and the use of major greenhouse gas CO2. Herein, the synthesis of GC via glycerol carbonylation with CO2 over a series of ZIF-8 on nickel-loaded Alumina Aerogel catalysts was examined for the first time in literature. ZIF-8 growth on nickel-impregnated Alumina aerogel was executed using an in situ method. Synthesized catalysts were analyzed using SEM–EDX, FT-IR, DRIFTS, XRD, and N2 sorption techniques. The carbonylation reaction of glycerol was conducted in the presence of a co-reactant (propylene oxide) and solvent (methanol). The influence of reaction parameters (temperature, catalyst loading, glycerol/co-reactant molar ratio, co-reactant type, catalyst type, and reaction time) on the catalytic activity (glycerol conversion, GC selectivity and yield) of the catalysts were investigated. It obtained high glycerol conversion (73%) for AA-2Ni-5ZIF, yield (31%), and selectivity (77%) of GC for AA-5Ni-15ZIF under optimized reaction conditions (150 °C, 7 bar, 2 h, 6% catalyst loading and 0.5 glycerol/propylene oxide). Compared to the literature, this activity was found under lower CO2 pressure and reaction time. Unique features of catalysts such as suitable acidity, high surface area, more than one active crystal, and the presence of propylene oxide as a co-reactant promoted the rise of glycerol conversion, GC selectivity, and yield.
期刊介绍:
Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry.
The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.