{"title":"作为生物油模型化合物的苯甲酸催化加氢脱氧:使用镍支撑催化剂的反应和动力学研究","authors":"Mustapha Yusuf, Gary A. Leeke, Joseph Wood","doi":"10.1039/d4se00589a","DOIUrl":null,"url":null,"abstract":"The development of technologies for the bio-oil upgrading process is a crucial step towards achieving sustainable energy production. This study investigates the effects of support properties during the hydrodeoxygenation (HDO) of benzoic acid as a bio-oil model compound with the aim to produce a catalyst of superior activity and selectivity. Three Ni-based catalysts were prepared: microporous m-Ni/ZSM-5, mesoporous h-Ni/ZSM-5, and Ni/SiO<small><sub>2</sub></small>. The h-Ni/ZSM-5 exhibited the highest concentration of acid sites, strongest metal-support interaction and best metal dispersion. The highest conversion of benzoic acid was recorded over the h-Ni/ZSM-5 catalyst (97%). Ni/SiO<small><sub>2</sub></small> catalysts produced toluene, while others produced benzene and cyclohexane in addition. This was linked to a synergy between support acidity and metal sites. The catalyst from the nearly neutral support, Ni/SiO<small><sub>2</sub></small>, showed higher activity (91% conversion) compared to m-Ni/ZSM-5 (84%), which was attributed to the mesoporous nature of Ni/SiO<small><sub>2</sub></small>, allowing more access to active sites for bulk benzoic acid molecules. A kinetic model was developed using the Langmuir–Hinshelwood–Hougen–Watson (LHHW) approach. A mechanism assuming dual-site adsorption of dissociatively adsorbed hydrogen was shown to be the most accurate representation of the three-phase benzoic acid HDO. The observed activation energy from the model was 137.2 kJ mol<small><sup>−1</sup></small>.","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0000,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Catalytic hydrodeoxygenation of benzoic acid as a bio-oil model compound: reaction and kinetics using nickel-supported catalysts\",\"authors\":\"Mustapha Yusuf, Gary A. Leeke, Joseph Wood\",\"doi\":\"10.1039/d4se00589a\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The development of technologies for the bio-oil upgrading process is a crucial step towards achieving sustainable energy production. This study investigates the effects of support properties during the hydrodeoxygenation (HDO) of benzoic acid as a bio-oil model compound with the aim to produce a catalyst of superior activity and selectivity. Three Ni-based catalysts were prepared: microporous m-Ni/ZSM-5, mesoporous h-Ni/ZSM-5, and Ni/SiO<small><sub>2</sub></small>. The h-Ni/ZSM-5 exhibited the highest concentration of acid sites, strongest metal-support interaction and best metal dispersion. The highest conversion of benzoic acid was recorded over the h-Ni/ZSM-5 catalyst (97%). Ni/SiO<small><sub>2</sub></small> catalysts produced toluene, while others produced benzene and cyclohexane in addition. This was linked to a synergy between support acidity and metal sites. The catalyst from the nearly neutral support, Ni/SiO<small><sub>2</sub></small>, showed higher activity (91% conversion) compared to m-Ni/ZSM-5 (84%), which was attributed to the mesoporous nature of Ni/SiO<small><sub>2</sub></small>, allowing more access to active sites for bulk benzoic acid molecules. A kinetic model was developed using the Langmuir–Hinshelwood–Hougen–Watson (LHHW) approach. A mechanism assuming dual-site adsorption of dissociatively adsorbed hydrogen was shown to be the most accurate representation of the three-phase benzoic acid HDO. The observed activation energy from the model was 137.2 kJ mol<small><sup>−1</sup></small>.\",\"PeriodicalId\":104,\"journal\":{\"name\":\"Sustainable Energy & Fuels\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.0000,\"publicationDate\":\"2024-06-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Sustainable Energy & Fuels\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1039/d4se00589a\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Sustainable Energy & Fuels","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4se00589a","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Catalytic hydrodeoxygenation of benzoic acid as a bio-oil model compound: reaction and kinetics using nickel-supported catalysts
The development of technologies for the bio-oil upgrading process is a crucial step towards achieving sustainable energy production. This study investigates the effects of support properties during the hydrodeoxygenation (HDO) of benzoic acid as a bio-oil model compound with the aim to produce a catalyst of superior activity and selectivity. Three Ni-based catalysts were prepared: microporous m-Ni/ZSM-5, mesoporous h-Ni/ZSM-5, and Ni/SiO2. The h-Ni/ZSM-5 exhibited the highest concentration of acid sites, strongest metal-support interaction and best metal dispersion. The highest conversion of benzoic acid was recorded over the h-Ni/ZSM-5 catalyst (97%). Ni/SiO2 catalysts produced toluene, while others produced benzene and cyclohexane in addition. This was linked to a synergy between support acidity and metal sites. The catalyst from the nearly neutral support, Ni/SiO2, showed higher activity (91% conversion) compared to m-Ni/ZSM-5 (84%), which was attributed to the mesoporous nature of Ni/SiO2, allowing more access to active sites for bulk benzoic acid molecules. A kinetic model was developed using the Langmuir–Hinshelwood–Hougen–Watson (LHHW) approach. A mechanism assuming dual-site adsorption of dissociatively adsorbed hydrogen was shown to be the most accurate representation of the three-phase benzoic acid HDO. The observed activation energy from the model was 137.2 kJ mol−1.
期刊介绍:
Sustainable Energy & Fuels will publish research that contributes to the development of sustainable energy technologies with a particular emphasis on new and next-generation technologies.