文献类型：期刊文献

中文题名：双功能炭基固体酸的制备及其催化纤维二糖醇解

英文题名：Preparation of Bifunctional Carbon-based Solid Acid and Its Catalytic Alcoholysis of Cellobiose

作者：范腾[1] 张荣花[1] 王奎[2] 潘晖[1] 冯君锋[1]

第一作者：范腾

机构：[1]南京林业大学化学工程学院,江苏南京210037;[2]中国林业科学研究院林产化学工业研究所,江苏南京210042

年份：2024

卷号：44

期号：2

起止页码：79-86

中文期刊名：林产化学与工业

外文期刊名：Chemistry and Industry of Forest Products

收录：CSTPCD;;Scopus;北大核心:【北大核心2023】；CSCD:【CSCD2023_2024】；

基金：国家自然科学基金资助项目(32101469)。

语种：中文

中文关键词：生物质催化转化;碳基固体酸;纤维二糖;乙酰丙酸;乙酰丙酸甲酯

外文关键词：catalytic conversion of biomass;carbon-based solid acid;cellobiose;levulinic acid;methyl levulinate

分类号：TQ35;TK6

摘要：以壳聚糖为碳源,通过金属浸渍、高温炭化制备负载铁的含氮活性炭(ACN-Fe),再进一步水热磺化制备了一系列金属负载型双功能炭基固体酸(ACN-Fe-SO_(3)H),并将其应用于催化纤维二糖醇解反应,利用X射线衍射(XRD)、拉曼(Raman)光谱、红外(FT-IR)光谱、N_(2)吸附/脱附、X射线光电子能谱(XPS)、电感耦合等离子体发射光谱(ICP-OES)和酸碱滴定等手段对催化剂进行了详细的表征。研究结果显示:固体酸中的不饱和三价铁离子具有路易斯酸性,磺酸基具有布朗斯特酸性,炭化温度800℃下制备的固体酸(800-ACN-Fe-SO_(3)H)具有最强的酸性(酸度0.81 mmol/g)和最大的比表面积(85.7 m^(2)/g),催化性能最佳。800-ACN-Fe-SO_(3)H用量0.20 g时,在反应温度200℃,反应时间5 h的条件下,纤维二糖的转化率为99.6%,产物乙酰丙酸(LA)和乙酰丙酸甲酯(ML)产率分别为15.6%和62.1%。催化剂经过5次循环回收,纤维二糖的转化率为93.1%,LA和ML的总产率为51.1%,表明催化剂具有良好的重复使用性,此外还初步探索了纤维二糖醇解的反应机理。
Chitosan was used as a carbon source to prepare iron-loaded nitrogen-containing activated carbon(ACN-Fe)through metal impregnation and high-temperature carbonization.A series of metal-loaded dual-functional carbon-based solid acid(ACN-Fe-SO_(3)H)catalysts were further prepared by hydrothermal sulfonation.The catalysts were applied to catalyze the alcoholysis of cellobiose.The catalysts were characterized in detail using X-ray diffraction(XRD),Raman spectroscopy,Fourier-transform infrared spectroscopy(FT-IR),N_(2)adsorption/desorption,X-ray photoelectron spectroscopy(XPS),inductively coupled plasma optical emission spectrometry(ICP-OES),and acid-base titration.The results showed that the unsaturated trivalent iron ions in the catalyst had Lewis acidity,while the sulfonic acid groups exhibited Br nsted acidity.The catalyst prepared at a carbonization temperature of 800℃(800-ACN-Fe-SO_(3)H)possessed the strongest acidity(acidity of 0.81 mmol/g)and the best structural characteristics(specific surface area of 85.7 m^(2)/g),showing the best catalytic performance.With a catalyst dosage of 0.20 g,a reaction temperature of 200℃,and a reaction time of 5 h,the cellobiose conversion rate reached 99.6%,with yields of levulinic acid(LA)and methyl levulinate(ML)of 15.6%and 62.1%,respectively.After 5 cycles,the cellobiose conversion rate remained 93.1%,with a product yield of 51.1%,indicating good catalyst reusability.Additionally,a preliminary exploration of the reaction mechanism of cellobiose alcoholysis was conducted.