{"title":"利用光热转换效应从生物衍生脂肪酸脱羧反应中生产高通量烷烃","authors":"Chunlin Hao , Bin Li , Guibao Guo , Shengli An","doi":"10.1016/j.fuproc.2024.108072","DOIUrl":null,"url":null,"abstract":"<div><p>Heating is the most straightforward means to achieve rapid, high-throughput production for thermal catalytic reactions, but photocatalysis reactions rarely use it because its intrinsic driving force depends on the effective separation of photogenerated charges, which generally shows little or sometimes negative dependence on temperature. Here we demonstrate that the heat generated by the photothermal conversion of Bi<sub>2</sub>O<sub>3</sub> nanoparticles can be utilized to dramatically accelerate the photocatalytic decarboxylation of long-chain fatty acids to C<sub>n-1</sub> n-alkanes. Using high-boiling solvents to maximize reaction temperatures, C<sub>n-1</sub> n-alkane can therefore be obtained in very high concentrations (e.g., ∼0.5 M) in a single operation, 5 orders of magnitude higher than the previous both semiconductor photocatalytic and algal photoenzyme transformations limited in the range ∼ 1–10<sup>2</sup> μM. Comprehensive characterizations unveil that the heat from incident light enables the standing C-chain at low temperature down onto the surface of catalyst, which allows the photoinduced hole/electron to readily approach and react with the more strained C-COO<sup>−</sup> bonds. This study manifests that the vast majority of incident light energy can be utilized in the form of heat to improve the reaction efficiency to as meet industrial output levels as possible.</p></div>","PeriodicalId":326,"journal":{"name":"Fuel Processing Technology","volume":"256 ","pages":"Article 108072"},"PeriodicalIF":7.2000,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0378382024000420/pdfft?md5=160ad4295a8f9d3470ae8b8da41c95e3&pid=1-s2.0-S0378382024000420-main.pdf","citationCount":"0","resultStr":"{\"title\":\"High-flux alkane production from bio-derived fatty acid decarboxylation enabled by photothermal conversion effect\",\"authors\":\"Chunlin Hao , Bin Li , Guibao Guo , Shengli An\",\"doi\":\"10.1016/j.fuproc.2024.108072\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Heating is the most straightforward means to achieve rapid, high-throughput production for thermal catalytic reactions, but photocatalysis reactions rarely use it because its intrinsic driving force depends on the effective separation of photogenerated charges, which generally shows little or sometimes negative dependence on temperature. Here we demonstrate that the heat generated by the photothermal conversion of Bi<sub>2</sub>O<sub>3</sub> nanoparticles can be utilized to dramatically accelerate the photocatalytic decarboxylation of long-chain fatty acids to C<sub>n-1</sub> n-alkanes. Using high-boiling solvents to maximize reaction temperatures, C<sub>n-1</sub> n-alkane can therefore be obtained in very high concentrations (e.g., ∼0.5 M) in a single operation, 5 orders of magnitude higher than the previous both semiconductor photocatalytic and algal photoenzyme transformations limited in the range ∼ 1–10<sup>2</sup> μM. Comprehensive characterizations unveil that the heat from incident light enables the standing C-chain at low temperature down onto the surface of catalyst, which allows the photoinduced hole/electron to readily approach and react with the more strained C-COO<sup>−</sup> bonds. This study manifests that the vast majority of incident light energy can be utilized in the form of heat to improve the reaction efficiency to as meet industrial output levels as possible.</p></div>\",\"PeriodicalId\":326,\"journal\":{\"name\":\"Fuel Processing Technology\",\"volume\":\"256 \",\"pages\":\"Article 108072\"},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2024-03-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S0378382024000420/pdfft?md5=160ad4295a8f9d3470ae8b8da41c95e3&pid=1-s2.0-S0378382024000420-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel Processing Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0378382024000420\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fuel Processing Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0378382024000420","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
High-flux alkane production from bio-derived fatty acid decarboxylation enabled by photothermal conversion effect
Heating is the most straightforward means to achieve rapid, high-throughput production for thermal catalytic reactions, but photocatalysis reactions rarely use it because its intrinsic driving force depends on the effective separation of photogenerated charges, which generally shows little or sometimes negative dependence on temperature. Here we demonstrate that the heat generated by the photothermal conversion of Bi2O3 nanoparticles can be utilized to dramatically accelerate the photocatalytic decarboxylation of long-chain fatty acids to Cn-1 n-alkanes. Using high-boiling solvents to maximize reaction temperatures, Cn-1 n-alkane can therefore be obtained in very high concentrations (e.g., ∼0.5 M) in a single operation, 5 orders of magnitude higher than the previous both semiconductor photocatalytic and algal photoenzyme transformations limited in the range ∼ 1–102 μM. Comprehensive characterizations unveil that the heat from incident light enables the standing C-chain at low temperature down onto the surface of catalyst, which allows the photoinduced hole/electron to readily approach and react with the more strained C-COO− bonds. This study manifests that the vast majority of incident light energy can be utilized in the form of heat to improve the reaction efficiency to as meet industrial output levels as possible.
期刊介绍:
Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.