{"title":"利用平面诱导荧光对多环芳烃热液分解过程进行原位可视化:机理分析","authors":"Xiangjin Meng, Hongchao Dai, Wenjun Lin, Hongfang Liu, Xingang Qi, Xiao Cai, Jinhua Wang, Zuohua Huang, Hui Jin, Liejin Guo","doi":"10.1016/j.cej.2024.153238","DOIUrl":null,"url":null,"abstract":"<div><p>Hydrothermal decomposition of coal or biomass for hydrogen production is a clean and efficient technology. Comprehending the hydrothermal decomposition mechanism of Polycyclic Aromatic Hydrocarbons (PAHs) is pivotal for advancing biomass or coal hydrothermal reaction technology. Traditional non-in situ measurement methods present challenges in thoroughly exploring the intricacies of PAHs’ hydrothermal reaction mechanisms. To address this issue, this study establishes an in situ visualization platform leveraging planar laser-induced fluorescence (PLIF) technology. Fluorescence signals emanating from naphthalene are meticulously measured in situ across diverse temperature conditions (450 °C-650 °C). The decomposition rate characteristics of PAH in hydrothermal process are thereby elucidated. A proportional increase in the reaction rate of naphthalene with elevated temperatures, concomitant with an augmented risk of coking. Moreover, the generation of hydroxyl radicals (OH) during the hydrothermal decomposition process was observed in the in situ visualization platform. Afterwards, to promote the generation of OH radicals and improve the conversion of PAHs, small molecule additives (formic acid, acetic acid, methanol, and ethanol) were added into the reactions. The experimental results indicate that the addition of small molecules increases the conversion rate of PAH and significantly reduces coking. These radicals effectively occupy reactive sites on naphthalene, thereby suppressing the coking proclivity of PAHs. This work provides a novel method to investigate the mechanism of hydrothermal process and offers a potential way to improve the conversion efficiency.</p></div>","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"494 ","pages":"Article 153238"},"PeriodicalIF":13.2000,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"In situ visualization of polycyclic aromatic hydrocarbon hydrothermal decomposition process utilizing planar induced fluorescence: A mechanistic analysis\",\"authors\":\"Xiangjin Meng, Hongchao Dai, Wenjun Lin, Hongfang Liu, Xingang Qi, Xiao Cai, Jinhua Wang, Zuohua Huang, Hui Jin, Liejin Guo\",\"doi\":\"10.1016/j.cej.2024.153238\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Hydrothermal decomposition of coal or biomass for hydrogen production is a clean and efficient technology. Comprehending the hydrothermal decomposition mechanism of Polycyclic Aromatic Hydrocarbons (PAHs) is pivotal for advancing biomass or coal hydrothermal reaction technology. Traditional non-in situ measurement methods present challenges in thoroughly exploring the intricacies of PAHs’ hydrothermal reaction mechanisms. To address this issue, this study establishes an in situ visualization platform leveraging planar laser-induced fluorescence (PLIF) technology. Fluorescence signals emanating from naphthalene are meticulously measured in situ across diverse temperature conditions (450 °C-650 °C). The decomposition rate characteristics of PAH in hydrothermal process are thereby elucidated. A proportional increase in the reaction rate of naphthalene with elevated temperatures, concomitant with an augmented risk of coking. Moreover, the generation of hydroxyl radicals (OH) during the hydrothermal decomposition process was observed in the in situ visualization platform. Afterwards, to promote the generation of OH radicals and improve the conversion of PAHs, small molecule additives (formic acid, acetic acid, methanol, and ethanol) were added into the reactions. The experimental results indicate that the addition of small molecules increases the conversion rate of PAH and significantly reduces coking. These radicals effectively occupy reactive sites on naphthalene, thereby suppressing the coking proclivity of PAHs. This work provides a novel method to investigate the mechanism of hydrothermal process and offers a potential way to improve the conversion efficiency.</p></div>\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"494 \",\"pages\":\"Article 153238\"},\"PeriodicalIF\":13.2000,\"publicationDate\":\"2024-06-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1385894724047260\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1385894724047260","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
In situ visualization of polycyclic aromatic hydrocarbon hydrothermal decomposition process utilizing planar induced fluorescence: A mechanistic analysis
Hydrothermal decomposition of coal or biomass for hydrogen production is a clean and efficient technology. Comprehending the hydrothermal decomposition mechanism of Polycyclic Aromatic Hydrocarbons (PAHs) is pivotal for advancing biomass or coal hydrothermal reaction technology. Traditional non-in situ measurement methods present challenges in thoroughly exploring the intricacies of PAHs’ hydrothermal reaction mechanisms. To address this issue, this study establishes an in situ visualization platform leveraging planar laser-induced fluorescence (PLIF) technology. Fluorescence signals emanating from naphthalene are meticulously measured in situ across diverse temperature conditions (450 °C-650 °C). The decomposition rate characteristics of PAH in hydrothermal process are thereby elucidated. A proportional increase in the reaction rate of naphthalene with elevated temperatures, concomitant with an augmented risk of coking. Moreover, the generation of hydroxyl radicals (OH) during the hydrothermal decomposition process was observed in the in situ visualization platform. Afterwards, to promote the generation of OH radicals and improve the conversion of PAHs, small molecule additives (formic acid, acetic acid, methanol, and ethanol) were added into the reactions. The experimental results indicate that the addition of small molecules increases the conversion rate of PAH and significantly reduces coking. These radicals effectively occupy reactive sites on naphthalene, thereby suppressing the coking proclivity of PAHs. This work provides a novel method to investigate the mechanism of hydrothermal process and offers a potential way to improve the conversion efficiency.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.