{"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}
引用次数: 0
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/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.