Hui Hou , Jingang Yao , Fuli Yang , Hongqing Ma , Guiying Xu
{"title":"尖晶石m_3 - xcrxo4偶联HZSM-11纳米片双功能催化剂增强CO2向芳烃的转化","authors":"Hui Hou , Jingang Yao , Fuli Yang , Hongqing Ma , Guiying Xu","doi":"10.1016/j.biombioe.2025.107946","DOIUrl":null,"url":null,"abstract":"<div><div>CO<sub>2</sub> and green hydrogen for aromatics production are effective methods to mitigate CO<sub>2</sub> emissions. Herein, Mg<sub>3-X</sub>Cr<sub>X</sub>O<sub>4</sub> spinel oxide was constructed via co-precipitation of Mg and Cr, followed by physical mixing with HZSM-11 to form a metal oxide-zeolite (OX-ZEO) bifunctional catalyst. The catalytic performance of this system in CO<sub>2</sub> aromatization was systematically evaluated. Notably, the designed catalysts followed a methanol-mediated pathway, overcoming limitations of the Anderson-Schulze-Flory distribution in aromatic hydrocarbon products. At varying Mg/Cr molar ratios, MgCr<sub>2</sub>O<sub>4</sub>/HZSM-11 exhibited the highest single-pass CO<sub>2</sub> conversion of 19.2 % and the highest aromatic selectivity of 75.2 % (excluding CO). Additionally, the optimal reaction conditions were determined for MgCr<sub>2</sub>O<sub>4</sub>/HZSM-11, achieving an excellent aromatic selectivity of 82.4 % and a CO<sub>2</sub> conversion of 22.6 % at 320 °C, a gas hourly space velocity (GHSV) of 1200 mL·gat<sup>−1</sup>·h<sup>−1</sup> and a pressure of 3.5 MPa. After 100 h, the MgCr<sub>2</sub>O<sub>4</sub>/HZSM-11 tandem catalyst maintained substantial catalytic activity, with aromatic selectivity and CO<sub>2</sub> conversion of 79.3 % and 21.1 %, respectively. This strategy offers valuable insights for designing OX-ZEO bifunctional catalysts.</div></div>","PeriodicalId":253,"journal":{"name":"Biomass & Bioenergy","volume":"199 ","pages":"Article 107946"},"PeriodicalIF":5.8000,"publicationDate":"2025-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced conversion of CO2 to aromatics over spinel Mg3-XCrXO4 coupled HZSM-11 nanosheets bifunctional catalyst\",\"authors\":\"Hui Hou , Jingang Yao , Fuli Yang , Hongqing Ma , Guiying Xu\",\"doi\":\"10.1016/j.biombioe.2025.107946\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>CO<sub>2</sub> and green hydrogen for aromatics production are effective methods to mitigate CO<sub>2</sub> emissions. Herein, Mg<sub>3-X</sub>Cr<sub>X</sub>O<sub>4</sub> spinel oxide was constructed via co-precipitation of Mg and Cr, followed by physical mixing with HZSM-11 to form a metal oxide-zeolite (OX-ZEO) bifunctional catalyst. The catalytic performance of this system in CO<sub>2</sub> aromatization was systematically evaluated. Notably, the designed catalysts followed a methanol-mediated pathway, overcoming limitations of the Anderson-Schulze-Flory distribution in aromatic hydrocarbon products. At varying Mg/Cr molar ratios, MgCr<sub>2</sub>O<sub>4</sub>/HZSM-11 exhibited the highest single-pass CO<sub>2</sub> conversion of 19.2 % and the highest aromatic selectivity of 75.2 % (excluding CO). Additionally, the optimal reaction conditions were determined for MgCr<sub>2</sub>O<sub>4</sub>/HZSM-11, achieving an excellent aromatic selectivity of 82.4 % and a CO<sub>2</sub> conversion of 22.6 % at 320 °C, a gas hourly space velocity (GHSV) of 1200 mL·gat<sup>−1</sup>·h<sup>−1</sup> and a pressure of 3.5 MPa. After 100 h, the MgCr<sub>2</sub>O<sub>4</sub>/HZSM-11 tandem catalyst maintained substantial catalytic activity, with aromatic selectivity and CO<sub>2</sub> conversion of 79.3 % and 21.1 %, respectively. This strategy offers valuable insights for designing OX-ZEO bifunctional catalysts.</div></div>\",\"PeriodicalId\":253,\"journal\":{\"name\":\"Biomass & Bioenergy\",\"volume\":\"199 \",\"pages\":\"Article 107946\"},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2025-05-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Biomass & Bioenergy\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0961953425003575\",\"RegionNum\":2,\"RegionCategory\":\"生物学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"AGRICULTURAL ENGINEERING\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Biomass & Bioenergy","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0961953425003575","RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"AGRICULTURAL ENGINEERING","Score":null,"Total":0}
Enhanced conversion of CO2 to aromatics over spinel Mg3-XCrXO4 coupled HZSM-11 nanosheets bifunctional catalyst
CO2 and green hydrogen for aromatics production are effective methods to mitigate CO2 emissions. Herein, Mg3-XCrXO4 spinel oxide was constructed via co-precipitation of Mg and Cr, followed by physical mixing with HZSM-11 to form a metal oxide-zeolite (OX-ZEO) bifunctional catalyst. The catalytic performance of this system in CO2 aromatization was systematically evaluated. Notably, the designed catalysts followed a methanol-mediated pathway, overcoming limitations of the Anderson-Schulze-Flory distribution in aromatic hydrocarbon products. At varying Mg/Cr molar ratios, MgCr2O4/HZSM-11 exhibited the highest single-pass CO2 conversion of 19.2 % and the highest aromatic selectivity of 75.2 % (excluding CO). Additionally, the optimal reaction conditions were determined for MgCr2O4/HZSM-11, achieving an excellent aromatic selectivity of 82.4 % and a CO2 conversion of 22.6 % at 320 °C, a gas hourly space velocity (GHSV) of 1200 mL·gat−1·h−1 and a pressure of 3.5 MPa. After 100 h, the MgCr2O4/HZSM-11 tandem catalyst maintained substantial catalytic activity, with aromatic selectivity and CO2 conversion of 79.3 % and 21.1 %, respectively. This strategy offers valuable insights for designing OX-ZEO bifunctional catalysts.
期刊介绍:
Biomass & Bioenergy is an international journal publishing original research papers and short communications, review articles and case studies on biological resources, chemical and biological processes, and biomass products for new renewable sources of energy and materials.
The scope of the journal extends to the environmental, management and economic aspects of biomass and bioenergy.
Key areas covered by the journal:
• Biomass: sources, energy crop production processes, genetic improvements, composition. Please note that research on these biomass subjects must be linked directly to bioenergy generation.
• Biological Residues: residues/rests from agricultural production, forestry and plantations (palm, sugar etc), processing industries, and municipal sources (MSW). Papers on the use of biomass residues through innovative processes/technological novelty and/or consideration of feedstock/system sustainability (or unsustainability) are welcomed. However waste treatment processes and pollution control or mitigation which are only tangentially related to bioenergy are not in the scope of the journal, as they are more suited to publications in the environmental arena. Papers that describe conventional waste streams (ie well described in existing literature) that do not empirically address ''new'' added value from the process are not suitable for submission to the journal.
• Bioenergy Processes: fermentations, thermochemical conversions, liquid and gaseous fuels, and petrochemical substitutes
• Bioenergy Utilization: direct combustion, gasification, electricity production, chemical processes, and by-product remediation
• Biomass and the Environment: carbon cycle, the net energy efficiency of bioenergy systems, assessment of sustainability, and biodiversity issues.