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Highly efficient transfer hydrodeoxygenation of vanillin over Sn~(4+)-induced highly dispersed Cu-based catalyst

机译:Sn〜(4+)诱导的高分散Cu基催化剂对香兰素的高效转移加氢脱氧

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摘要

Developing highly efficient non-noble-metal catalysts for the upgrade of abundant and low-cost renewable raw biomass into high-quality biofuels and important chemicals is especially desirable, but still remains huge challenges. Herein, Sn4+-induced highly dispersed Cu-based catalyst, Cu/Zn-Al-Sn layered double hydroxide (Cu/ZnAlSn-LDH), is delicately constructed for catalytic transfer hydrodeoxygenation of vanillin to promising 2-methoxy-4-methylphenol (MMP) biofuel using 2-propanol as hydrogen source and solvent without any external hydrogen supply. Nearly total MMP yield is achieved under moderate reaction conditions (180 degrees C, 4 h) and the turnover number (TON) value calculated in Cu/ZnAlSn-LDH is about 3 times higher than that in Sn-free catalyst (Cu/ZnAl-LDH). Characterizations results reveal that the Sn4+ species confined in the lattice of brucite-like layer of ZnAlSn-LDH are existed in electron-rich state, which can promote the formation of smaller Cu nanoparticles (1.95 nm) in Cu/ZnAlSn-LDH compared to those in Sn-free Cu/ZnAl-LDH catalyst (6.08 nm), as well as stronger metal-support interaction, thus leading to the higher catalytic performance and stability. The present findings offer a new avenue to strategically fabricate highly dispersed non-noble metal catalysts with enhanced catalytic performance by adjusting surface structures and compositions of supports for a wide range of hydrodeoxygenation of other biomass-derived compounds without any external hydrogen.
机译:开发高效的非贵金属催化剂以将丰富和低成本的可再生原料生物质升级为高质量的生物燃料和重要化学物质是特别可取的,但仍然面临巨大挑战。在此,Sn4 +诱导的高度分散的铜基催化剂Cu / Zn-Al-Sn层状双氢氧化物(Cu / ZnAlSn-LDH)精心构建,用于将香兰素催化转移加氢脱氧成有希望的2-甲氧基-4-甲基苯酚(MMP) )使用2-丙醇作为氢源和溶剂的生物燃料,无需任何外部氢供应。在中等反应条件下(180摄氏度,4小时)几乎可以达到MMP的总产率,并且Cu / ZnAlSn-LDH中计算出的周转率值(TON)约为无锡催化剂(Cu / ZnAl- LDH)。表征结果表明,限制在ZnAlSn-LDH的水镁石状层晶格中的Sn4 +物种以富电子态存在,与那些Cu / ZnAlSn-LDH相比,可促进较小的Cu纳米颗粒(1.95 nm)的形成。不含锡的Cu / ZnAl-LDH催化剂(6.08 nm)中,以及更强的金属-载体相互作用,从而导致更高的催化性能和稳定性。本发明的发现提供了新的途径,以战略性地通过调节载体的表面结构和载体组成来广泛地对其他生物质衍生的化合物进行加氢脱氧而无需任何外部氢,从而策略性地制备具有增强的催化性能的高度分散的非贵金属催化剂。

著录项

  • 来源
    《Applied Surface Science》 |2019年第30期|548-556|共9页
  • 作者单位

    East China Univ Technol, Sch Chem Biol & Mat Sci, State Key Lab Nucl Resources & Environm, Nanchang 330013, Jiangxi, Peoples R China;

    East China Univ Technol, Sch Chem Biol & Mat Sci, State Key Lab Nucl Resources & Environm, Nanchang 330013, Jiangxi, Peoples R China;

    East China Univ Technol, Sch Chem Biol & Mat Sci, State Key Lab Nucl Resources & Environm, Nanchang 330013, Jiangxi, Peoples R China;

    East China Univ Technol, Sch Chem Biol & Mat Sci, State Key Lab Nucl Resources & Environm, Nanchang 330013, Jiangxi, Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Lattice confinement; Layered double hydroxide; Cu-based catalyst; Catalytic transfer hydrodeoxygenation; Vanillin;

    机译:晶格限制;层状双氢氧化物;铜基催化剂;催化转移加氢脱氧;香兰素;

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