{"title":"Multi-catalytic active site biochar-based catalysts for glucose isomerized to fructose: Experiments and density functional theory study","authors":"","doi":"10.1007/s42114-024-00861-2","DOIUrl":null,"url":null,"abstract":"<h3>Abstract</h3> <p>This work provides an innovative method for preparing different isomerization catalysts by impregnating different proportions of MgCl<sub>2</sub> and AlCl<sub>3</sub> and combining different K compounds on cellulose-derived biochar, followed by pyrolysis. Results show MgO and Al(OH)<sub>3</sub> existing in <sub>4</sub>Mg-<sub>1</sub>Al-C catalyst can obtain better catalytic effect on glucose isomerization than the singe of Al presenting in <sub>0</sub>Mg-<sub>1</sub>Al-C catalyst. Moreover, the synergism effects of the multi-catalytic active sites such as β-<sub>,</sub> γ-Al(OH)<sub>3</sub>, KCl, MgO, and K<sub>4</sub>H<sub>2</sub>(CO<sub>3</sub>)<sub>3</sub> in Mg-Al-KHCO<sub>3</sub>-C catalyst can further lead to an increase in glucose isomerization, compared to the <sub>4</sub>Mg-<sub>1</sub>Al-C catalyst. The X-ray diffraction results present that the value of O/Al in Mg-Al-KHCO<sub>3</sub>-C catalyst is as high as 13.38, which provides many unsaturated acidic catalysis sites and benefits the glucose isomerization. Simultaneously, the TPD results reveal that the main active sites (MgO, Al(OH)<sub>3</sub>, and K<sub>4</sub>H<sub>2</sub>(CO<sub>3</sub>)<sub>3</sub>) in Mg-Al-KHCO<sub>3</sub>-C catalyst can provide weakly acidic and basic sites and avoid strongly acidic and basic sites to excessively attack the glucose. Based on the DFT analysis, the results indicate that the MgO has a great effect on the ring-opening reaction to form acyclic glucose, while Al(OH)<sup>3+</sup> has a great effect on promoting acyclic glucose hydrogen transfer isomerized to form fructose. Compared to other carbon-based metal catalysts, the prepared Mg-Al-KHCO<sub>3</sub>-C has excellent catalytic performance, which gives a higher fructose yield (38.7%) and selectivity (87.72%) and glucose conversion (44.12%) at 100 °C in 30 min. In this study, we develop a highly efficient Mg-Al-K-biochar catalyst for glucose isomerization and provide an efficient method for cellulose valorization.</p>","PeriodicalId":7220,"journal":{"name":"Advanced Composites and Hybrid Materials","volume":null,"pages":null},"PeriodicalIF":23.2000,"publicationDate":"2024-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Composites and Hybrid Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1007/s42114-024-00861-2","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, COMPOSITES","Score":null,"Total":0}
引用次数: 0
Abstract
This work provides an innovative method for preparing different isomerization catalysts by impregnating different proportions of MgCl2 and AlCl3 and combining different K compounds on cellulose-derived biochar, followed by pyrolysis. Results show MgO and Al(OH)3 existing in 4Mg-1Al-C catalyst can obtain better catalytic effect on glucose isomerization than the singe of Al presenting in 0Mg-1Al-C catalyst. Moreover, the synergism effects of the multi-catalytic active sites such as β-, γ-Al(OH)3, KCl, MgO, and K4H2(CO3)3 in Mg-Al-KHCO3-C catalyst can further lead to an increase in glucose isomerization, compared to the 4Mg-1Al-C catalyst. The X-ray diffraction results present that the value of O/Al in Mg-Al-KHCO3-C catalyst is as high as 13.38, which provides many unsaturated acidic catalysis sites and benefits the glucose isomerization. Simultaneously, the TPD results reveal that the main active sites (MgO, Al(OH)3, and K4H2(CO3)3) in Mg-Al-KHCO3-C catalyst can provide weakly acidic and basic sites and avoid strongly acidic and basic sites to excessively attack the glucose. Based on the DFT analysis, the results indicate that the MgO has a great effect on the ring-opening reaction to form acyclic glucose, while Al(OH)3+ has a great effect on promoting acyclic glucose hydrogen transfer isomerized to form fructose. Compared to other carbon-based metal catalysts, the prepared Mg-Al-KHCO3-C has excellent catalytic performance, which gives a higher fructose yield (38.7%) and selectivity (87.72%) and glucose conversion (44.12%) at 100 °C in 30 min. In this study, we develop a highly efficient Mg-Al-K-biochar catalyst for glucose isomerization and provide an efficient method for cellulose valorization.
期刊介绍:
Advanced Composites and Hybrid Materials is a leading international journal that promotes interdisciplinary collaboration among materials scientists, engineers, chemists, biologists, and physicists working on composites, including nanocomposites. Our aim is to facilitate rapid scientific communication in this field.
The journal publishes high-quality research on various aspects of composite materials, including materials design, surface and interface science/engineering, manufacturing, structure control, property design, device fabrication, and other applications. We also welcome simulation and modeling studies that are relevant to composites. Additionally, papers focusing on the relationship between fillers and the matrix are of particular interest.
Our scope includes polymer, metal, and ceramic matrices, with a special emphasis on reviews and meta-analyses related to materials selection. We cover a wide range of topics, including transport properties, strategies for controlling interfaces and composition distribution, bottom-up assembly of nanocomposites, highly porous and high-density composites, electronic structure design, materials synergisms, and thermoelectric materials.
Advanced Composites and Hybrid Materials follows a rigorous single-blind peer-review process to ensure the quality and integrity of the published work.