Catalytic conversion of biomass-derived levulinic acid to valerate esters as oxygenated fuels using supported ruthenium catalysts
Catalytic conversion of biomass-derived levulinic acid to valerate esters as oxygenated fuels using supported ruthenium catalysts
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DOI：
10.1039/c3gc40927a
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发表时间：
2013-09
期刊：
影响因子：
9.8
通讯作者：
T. Pan;Jin Deng;Qingli Xu;Xu Yang;Q. Guo;Yao Fu
中科院分区：
文献类型：
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作者：
T. Pan;Jin Deng;Qingli Xu;Xu Yang;Q. Guo;Yao Fu
发展生物质基平台分子催化转化为含氧燃料分子，对于减少对化石资源的依赖，解决环境问题具有重要意义。戊酸烷基酯具有成为汽油和柴油可再生添加剂的潜力。在本研究中，我们研究了乙酰丙酸（LA）在负载型Ru催化剂上加氢生成戊酸酯，发现酸度是影响催化剂性能的重要因素。研制了双功能催化剂Ru/SBA-SO3H作为活性催化剂，得到了最高收率为94%的戊酸乙酯（EV）。采用氮吸附/解吸法、x射线衍射（XRD）、透射电子能谱（TEM）和x射线光电子能谱（XPS）对催化剂进行了表征。全面考察了反应条件的影响，提出并验证了可能的反应途径。双功能催化剂还可以催化LA转化为各种戊酸烷基酯。此外，在与ru基催化剂相似的反应条件下，还筛选了负载型Cu和Ni催化剂，Ni/SBA-15和SBA-SO3H的组合表现出LA转化为EV的活性。
The development of the catalytic conversion of biomass-based platform molecules into oxygenated fuel molecules is of great significance in order to reduce the dependence on fossil resources and to solve environmental problems. Alkyl valerate esters were proven to have the potential to be renewable additives of gasoline and diesel. In this work, we studied the hydrogenation of levulinic acid (LA) to valerate esters over supported Ru catalysts, and found that the acidity was an important factor for the catalyst performance. A bifunctional catalyst Ru/SBA-SO3H was developed as an active catalyst, and a highest yield of 94% to ethyl valerate (EV) was achieved. The catalyst was characterized by nitrogen adsorption/desorption methods, X-ray power diffraction (XRD), transmission electron spectroscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The effects of reaction conditions were comprehensively investigated and probable reaction pathways were proposed and verified. The conversion of LA to various alkyl valerate esters can also be catalyzed by the bifunctional catalyst. In addition, supported Cu and Ni catalysts were also screened under similar reaction conditions as Ru-based catalysts, and the combination of Ni/SBA-15 and SBA-SO3H exhibited activity for the conversion of LA to EV.