{"title":"在温和条件下,使用掺杂 N 的碳化铝基 RuCo 催化剂从 MOF 中提取木质素衍生酚类物质,高效加氢脱氧生成环己醇","authors":"Shiyun Xiao, Zhouxin Peng, Yuchen Wu, Baojia Li, Hualan Zhou, Xuesong Wang, Shengkang Wang","doi":"10.1016/j.biombioe.2024.107437","DOIUrl":null,"url":null,"abstract":"<div><div>In this work, a novel RuCo bimetallic supported on N-doped carbon support containing alumina was prepared by in-situ pyrolysis using MOF-303 as the support precursor (Ru<sub>3</sub>Co<sub>1</sub>@CN-Al<sub>2</sub>O<sub>3</sub>), and it was applied to the efficient hydrodeoxygenation (HDO) of guaiacol under mild conditions (0.01 MPa H<sub>2</sub>, 200 °C, 3h), the yield of cyclohexanol reaches an impressive 83.12 %. In the absence of external hydrogen (2 MPa N<sub>2</sub>, 220 °C, 2 h), complete conversion of guaiacol was achieved, along with a remarkable 97.81 % selectivity towards cyclohexanol. The HDO of guaiacol under different atmospheres was further studied, and the possible mechanism was proposed. Characterization results indicated that the supported metals (Ru and Co) not only interacted with the N in the MOF-303 to enhance catalyst stability but also that the synergistic effect between Ru and Co was key to promoting the high yield of cyclohexanol through catalytic transfer hydrodeoxygenation (CTHDO) in isopropanol. Additionally, Ru<sub>3</sub>Co<sub>1</sub>@CN-Al<sub>2</sub>O<sub>3</sub> was also effective in achieving the HDO of macromolecular lignin. This study provides a feasible approach for the high value-added green transformation of lignin and its derivatives under mild conditions, highlighting the significant potential of MOFs for lignin valorization.</div></div>","PeriodicalId":253,"journal":{"name":"Biomass & Bioenergy","volume":"190 ","pages":"Article 107437"},"PeriodicalIF":5.8000,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient hydrodeoxygenation of lignin-derived phenolics to cyclohexanol with N-doped alumina- carbide‐based RuCo catalysts derived from MOF under mild conditions\",\"authors\":\"Shiyun Xiao, Zhouxin Peng, Yuchen Wu, Baojia Li, Hualan Zhou, Xuesong Wang, Shengkang Wang\",\"doi\":\"10.1016/j.biombioe.2024.107437\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In this work, a novel RuCo bimetallic supported on N-doped carbon support containing alumina was prepared by in-situ pyrolysis using MOF-303 as the support precursor (Ru<sub>3</sub>Co<sub>1</sub>@CN-Al<sub>2</sub>O<sub>3</sub>), and it was applied to the efficient hydrodeoxygenation (HDO) of guaiacol under mild conditions (0.01 MPa H<sub>2</sub>, 200 °C, 3h), the yield of cyclohexanol reaches an impressive 83.12 %. In the absence of external hydrogen (2 MPa N<sub>2</sub>, 220 °C, 2 h), complete conversion of guaiacol was achieved, along with a remarkable 97.81 % selectivity towards cyclohexanol. The HDO of guaiacol under different atmospheres was further studied, and the possible mechanism was proposed. Characterization results indicated that the supported metals (Ru and Co) not only interacted with the N in the MOF-303 to enhance catalyst stability but also that the synergistic effect between Ru and Co was key to promoting the high yield of cyclohexanol through catalytic transfer hydrodeoxygenation (CTHDO) in isopropanol. Additionally, Ru<sub>3</sub>Co<sub>1</sub>@CN-Al<sub>2</sub>O<sub>3</sub> was also effective in achieving the HDO of macromolecular lignin. This study provides a feasible approach for the high value-added green transformation of lignin and its derivatives under mild conditions, highlighting the significant potential of MOFs for lignin valorization.</div></div>\",\"PeriodicalId\":253,\"journal\":{\"name\":\"Biomass & Bioenergy\",\"volume\":\"190 \",\"pages\":\"Article 107437\"},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-10-17\",\"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/S0961953424003908\",\"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/S0961953424003908","RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"AGRICULTURAL ENGINEERING","Score":null,"Total":0}
Efficient hydrodeoxygenation of lignin-derived phenolics to cyclohexanol with N-doped alumina- carbide‐based RuCo catalysts derived from MOF under mild conditions
In this work, a novel RuCo bimetallic supported on N-doped carbon support containing alumina was prepared by in-situ pyrolysis using MOF-303 as the support precursor (Ru3Co1@CN-Al2O3), and it was applied to the efficient hydrodeoxygenation (HDO) of guaiacol under mild conditions (0.01 MPa H2, 200 °C, 3h), the yield of cyclohexanol reaches an impressive 83.12 %. In the absence of external hydrogen (2 MPa N2, 220 °C, 2 h), complete conversion of guaiacol was achieved, along with a remarkable 97.81 % selectivity towards cyclohexanol. The HDO of guaiacol under different atmospheres was further studied, and the possible mechanism was proposed. Characterization results indicated that the supported metals (Ru and Co) not only interacted with the N in the MOF-303 to enhance catalyst stability but also that the synergistic effect between Ru and Co was key to promoting the high yield of cyclohexanol through catalytic transfer hydrodeoxygenation (CTHDO) in isopropanol. Additionally, Ru3Co1@CN-Al2O3 was also effective in achieving the HDO of macromolecular lignin. This study provides a feasible approach for the high value-added green transformation of lignin and its derivatives under mild conditions, highlighting the significant potential of MOFs for lignin valorization.
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.