Sherif Hegazy, Hanan H. Ibrahim, Timo Weckman, Tao Hu, Sari Tuomikoski, Ulla Lassi, Karoliina Honkala, Varsha Srivastava
{"title":"Synergistic pyrolysis of Cellulose/Fe-MOF Composite: A Combined experimental and DFT study on dye removal","authors":"Sherif Hegazy, Hanan H. Ibrahim, Timo Weckman, Tao Hu, Sari Tuomikoski, Ulla Lassi, Karoliina Honkala, Varsha Srivastava","doi":"10.1016/j.cej.2024.158654","DOIUrl":null,"url":null,"abstract":"We propose the development of an innovative composite material formed through the pyrolysis of oxidized cellulose derived from sawdust, utilizing iron-based MOF as a precursor. This novel material incorporates multiple iron-based components (Fe<sub>3</sub>O<sub>4</sub>, Fe<sub>3</sub>C and Fe<sup>0</sup>) within a biochar matrix. We employed the composite to adsorb a cationic dye from aqueous solution. Batch adsorption studies explored the effects of pH, contact time, and initial dye concentration. The experimental data fitted well with the pseudo-second-order kinetic model, suggesting chemisorption as the primary mechanism, while equilibrium adsorption results fitted to the Langmuir isotherm model, described monolayer adsorption displaying the highest adsorption capacity (106 mg/g). A fixed-bed column experiment further demonstrated effective removal of methylene blue (MB) dye, achieving an initial breakthrough time of approximately 12 h, and exhibiting an adsorption capacity (q<sub>e</sub> = 71.14 mg/g) surpassing batch adsorption capacity at the same concentration (q<sub>e</sub> batch = 52.53 mg/g), signifying the practical utility of the materials. In addition, pyrolysis-derived biochar samples displayed improved total organic carbon (TOC) removal efficiency, with P-Cell-MOF achieving 93 % TOC removal. Density functional theory (DFT) calculations were employed to investigate the binding of MB on the various materials derived from the pyrolysis of cellulose with MOF. The calculations show that MB chemisorbs on both Fe (110) and Fe<sub>3</sub>C (001) surfaces while only physisorption was observed on Fe<sub>3</sub>O<sub>4</sub>(111) and graphene. These computational findings align well with the experimental data and provide an explanation for the enhanced TOC removal observed with the P-Cell-MOF.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"1 1","pages":""},"PeriodicalIF":13.3000,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2024.158654","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}
引用次数: 0
Abstract
We propose the development of an innovative composite material formed through the pyrolysis of oxidized cellulose derived from sawdust, utilizing iron-based MOF as a precursor. This novel material incorporates multiple iron-based components (Fe3O4, Fe3C and Fe0) within a biochar matrix. We employed the composite to adsorb a cationic dye from aqueous solution. Batch adsorption studies explored the effects of pH, contact time, and initial dye concentration. The experimental data fitted well with the pseudo-second-order kinetic model, suggesting chemisorption as the primary mechanism, while equilibrium adsorption results fitted to the Langmuir isotherm model, described monolayer adsorption displaying the highest adsorption capacity (106 mg/g). A fixed-bed column experiment further demonstrated effective removal of methylene blue (MB) dye, achieving an initial breakthrough time of approximately 12 h, and exhibiting an adsorption capacity (qe = 71.14 mg/g) surpassing batch adsorption capacity at the same concentration (qe batch = 52.53 mg/g), signifying the practical utility of the materials. In addition, pyrolysis-derived biochar samples displayed improved total organic carbon (TOC) removal efficiency, with P-Cell-MOF achieving 93 % TOC removal. Density functional theory (DFT) calculations were employed to investigate the binding of MB on the various materials derived from the pyrolysis of cellulose with MOF. The calculations show that MB chemisorbs on both Fe (110) and Fe3C (001) surfaces while only physisorption was observed on Fe3O4(111) and graphene. These computational findings align well with the experimental data and provide an explanation for the enhanced TOC removal observed with the P-Cell-MOF.
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.