Meijun Li , Junyan Zhang , Stephen C. Purdy , Fan Lin , Kinga A. Unocic , Michael Cordon , Zili Wu , Huamin Wang , Jacklyn Hall , A. Jeremy Kropf , Theodore R. Krause , Brian Davison , Zhenglong Li , Andrew D. Sutton
{"title":"通过调节双功能铜-RE/β-沸石催化剂中的稀土金属来调整烯烃分布，从而实现乙醇提纯","authors":"Meijun Li , Junyan Zhang , Stephen C. Purdy , Fan Lin , Kinga A. Unocic , Michael Cordon , Zili Wu , Huamin Wang , Jacklyn Hall , A. Jeremy Kropf , Theodore R. Krause , Brian Davison , Zhenglong Li , Andrew D. Sutton","doi":"10.1016/j.apcatb.2023.123648","DOIUrl":null,"url":null,"abstract":"<div><p>Bioethanol to middle distillate technologies have offered a unique solution to produce renewable aviation fuel for decarbonizing the hard-to-electrify sectors. Here, we have developed the series of bimetallic Cu- and rare earth-containing (RE) Beta zeolite catalysts that yield high C<sub>3+</sub><span> alkene<span> selectivity from ethanol upgrading (>80% selectivity at ∼100% conversion, 623 K). The formation rates of butene isomers to C</span></span><sub>5+</sub> alkenes are linearly correlated with the strength of Lewis acidic RE identity, which follows the sequence of Yb<sub>12</sub>/Beta >Y<sub>7</sub>/Beta > Gd<sub>12</sub>/Beta > Ce<sub>10</sub>/Beta > La<sub>12</sub>/Beta. Rate measurements indicate that the RE selection plays the vital role in altering the rate of the key competitive reactions within the ethanol-to-alkenes reaction network, namely C<sub>4</sub> alcohol dehydration and C-C chain growth, which dictate alkene product distributions. These findings indicate a feasible and promising method for tailoring alkene product distributions from ethanol upgrading, which is of notable significance to the generation of renewable middle distillates.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":20.2000,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tailoring olefin distribution via tuning rare earth metals in bifunctional Cu-RE/beta-zeolite catalysts for ethanol upgrading\",\"authors\":\"Meijun Li , Junyan Zhang , Stephen C. Purdy , Fan Lin , Kinga A. Unocic , Michael Cordon , Zili Wu , Huamin Wang , Jacklyn Hall , A. Jeremy Kropf , Theodore R. Krause , Brian Davison , Zhenglong Li , Andrew D. Sutton\",\"doi\":\"10.1016/j.apcatb.2023.123648\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Bioethanol to middle distillate technologies have offered a unique solution to produce renewable aviation fuel for decarbonizing the hard-to-electrify sectors. Here, we have developed the series of bimetallic Cu- and rare earth-containing (RE) Beta zeolite catalysts that yield high C<sub>3+</sub><span> alkene<span> selectivity from ethanol upgrading (>80% selectivity at ∼100% conversion, 623 K). The formation rates of butene isomers to C</span></span><sub>5+</sub> alkenes are linearly correlated with the strength of Lewis acidic RE identity, which follows the sequence of Yb<sub>12</sub>/Beta >Y<sub>7</sub>/Beta > Gd<sub>12</sub>/Beta > Ce<sub>10</sub>/Beta > La<sub>12</sub>/Beta. Rate measurements indicate that the RE selection plays the vital role in altering the rate of the key competitive reactions within the ethanol-to-alkenes reaction network, namely C<sub>4</sub> alcohol dehydration and C-C chain growth, which dictate alkene product distributions. These findings indicate a feasible and promising method for tailoring alkene product distributions from ethanol upgrading, which is of notable significance to the generation of renewable middle distillates.</p></div>\",\"PeriodicalId\":244,\"journal\":{\"name\":\"Applied Catalysis B: Environmental\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":20.2000,\"publicationDate\":\"2023-12-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis B: Environmental\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926337323012912\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis B: Environmental","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926337323012912","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Tailoring olefin distribution via tuning rare earth metals in bifunctional Cu-RE/beta-zeolite catalysts for ethanol upgrading
Bioethanol to middle distillate technologies have offered a unique solution to produce renewable aviation fuel for decarbonizing the hard-to-electrify sectors. Here, we have developed the series of bimetallic Cu- and rare earth-containing (RE) Beta zeolite catalysts that yield high C3+ alkene selectivity from ethanol upgrading (>80% selectivity at ∼100% conversion, 623 K). The formation rates of butene isomers to C5+ alkenes are linearly correlated with the strength of Lewis acidic RE identity, which follows the sequence of Yb12/Beta >Y7/Beta > Gd12/Beta > Ce10/Beta > La12/Beta. Rate measurements indicate that the RE selection plays the vital role in altering the rate of the key competitive reactions within the ethanol-to-alkenes reaction network, namely C4 alcohol dehydration and C-C chain growth, which dictate alkene product distributions. These findings indicate a feasible and promising method for tailoring alkene product distributions from ethanol upgrading, which is of notable significance to the generation of renewable middle distillates.
期刊介绍：
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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