Bifunctional carbon Ni/NiO nanofiber catalyst based on 5-sulfosalicylic acid for conversion of C5/C6 carbohydrates into ethyl levulinate,Reaction Chemistry & Engineering

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Bifunctional carbon Ni/NiO nanofiber catalyst based on 5-sulfosalicylic acid for conversion of C5/C6 carbohydrates into ethyl levulinate
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2020-07-30 , DOI: 10.1039/d0re00153h
Haixin Guo _{1,

2,

3,

4} , Yuya Abe _{1,

2,

3,

4} , Xinhua Qi _{5,

6,

7,

8} , Richard Lee Smith Jr _{1,

2,

3,

4,

9}

Affiliation

A method was developed for preparing bifunctional carbon Ni/NiO nanofiber catalysts that promote efficient one-pot conversion of C5/C6 carbohydrates into levulinate esters in alcohol solvents. The bifunctional catalysts were prepared via solvothermal carbonization of 5-sulfosalicylic acid/NiSO₄ without the use of sulfuric acid or hydrogen gas and had fine particle sizes (d = 5 nm to 50 nm) and contained –NH₂, –SO₃H, –COOH and phenolic –OH functional groups. Under optimal conditions, the catalysts afforded 93% selectivity of ethyl levulinate in ethanol with the major intermediate being 2-(ethoxymethyl)furan, 4,5,5-triethoxypentan-2-one and major byproduct being 2,5,5-triethoxpentan-2-one. Cooperative activity of Lewis acidity, Brønsted acidity and functional group sites of the catalyst is demonstrated for multi-step reaction sequences of C5/C6 carbohydrates with one-pot conversions and alcohols (methanol, ethanol, 1-propanol, 1-butanol) that act as both solvent and hydrogen donor source in which the bifunctional catalyst was shown to be recyclable five times with no apparent change in conversion and ca. 5% change in selectivity.

中文翻译：

基于5-磺基水杨酸的双官能碳Ni / NiO纳米纤维催化剂，用于将C5 / C6碳水化合物转化为乙酰丙酸乙酯

开发了一种制备双官能碳Ni / NiO纳米纤维催化剂的方法，该催化剂可促进C5 / C6碳水化合物在醇溶剂中有效地一锅转化为乙酰丙酸酯。通过在不使用硫酸或氢气的情况下对5-磺基水杨酸/ NiSO ₄进行溶剂热碳化来制备双功能催化剂，并且该催化剂的粒径很小（d = 5 nm至50 nm），并且含有–NH ₂，–SO ₃H，-COOH和酚-OH官能团。在最佳条件下，该催化剂在乙醇中提供了93％的乙酰丙酸乙酯选择性，主要中间体为2-（乙氧基甲基）呋喃，4,5,5-三乙氧基戊烷-2-one，主要副产物为2,5,5-三乙氧基戊烷- 2个对于具有一锅转换的C5 / C6碳水化合物和起作用的醇（甲醇，乙醇，1-丙醇，1-丁醇）的多步反应序列，证明了路易斯酸度，布朗斯台德酸度和催化剂的官能团位点的协同活性作为溶剂和氢供体来源，双功能催化剂被证明可循环使用五次，转化率和Ca值均无明显变化。选择性变化5％。

更新日期：2020-08-25

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