介孔磷酸铌一锅法高效催化木糖制备糠醛

引用本文: 李相呈, 张宇, 夏银江, 胡必成, 钟霖, 王艳芹, 卢冠忠. 介孔磷酸铌一锅法高效催化木糖制备糠醛[J]. 物理化学学报, 2012, 28(10): 2349-2354. doi: 10.3866/PKU.WHXB201207312 shu

Citation: LI Xiang-Cheng, ZHANG Yu, XIA Yin-Jiang, HU Bi-Cheng, WANG Yan-Qin, LU Guan-Zhong. One-Pot Catalytic Conversion of Xylose to Furfural on Mesoporous Niobium Phosphate[J]. Acta Physico-Chimica Sinica, 2012, 28(10): 2349-2354. doi: 10.3866/PKU.WHXB201207312 shu

介孔磷酸铌一锅法高效催化木糖制备糠醛

基金项目:
国家自然科学基金(20973058) (20973058)

中央高校交叉学科与重大项目培育基金资助项目

摘要:

木糖转化到糠醛一般包括两步: 首先在酶、碱或路易斯(L)酸的催化作用下异构化木糖到木酮糖, 接下来木酮糖在酸的作用下脱水得到糠醛. 针对木糖水相脱水一步制备糠醛, 利用十六烷基三甲基溴化铵(CTAB)为模板剂, 借助软模板合作策略制备了一种抗水的新型固体酸催化剂, 介孔磷酸铌, 并利用X射线衍射(XRD)、N₂吸脱附、透射电镜(TEM)、氨气程序升温脱附(NH₃-TPD)和吡啶吸附傅里叶变换红外(Py-FTIR)光谱对材料的结构和酸性质进行了表征. 研究发现介孔磷酸铌不仅具有很高的比表面积(>200 m²·g^-1), 比较窄的孔径分布(3.5nm), 同时还具有很强的L酸性和布朗斯特(B)酸性. 通过L酸催化的木糖异构化为木酮糖/来苏糖和B酸催化的木酮糖/来苏糖进一步脱水得到糠醛, 实现了一步由木糖到糠醛的高效转化. 为了优化反应条件, 考察了水溶液中反应温度、投料质量比及反应时间对木糖转化率和糠醛收率的影响, 在最佳的反应条件下, 木糖的转化率为96.5%, 糠醛的收率达49.8%. 进一步地, 为了提高收率且易于分离, 利用4-甲基-2-戊酮(MIBK)/NaCl水溶液(体积比为7:3)作为反应混合溶剂, 使糠醛收率提高到68.4%.

关键词:

English

One-Pot Catalytic Conversion of Xylose to Furfural on Mesoporous Niobium Phosphate

1.
Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, P. R. China
Received Date: 11 June 2012
Available Online: 26 September 2012
Fund Project:
国家自然科学基金(20973058)

中央高校交叉学科与重大项目培育基金资助项目

Abstract:

The conversion of xylose to furfural normally involves two steps: the isomerization of xylose to xylulose catalyzed by an enzyme, a base or a Lewis acid, followed by the acid-catalyzed dehydration of xylulose to furfural. To allow a more efficient single-step conversion, a new water-tolerant solid acid catalyst, mesoporous niobium phosphate was synthesized. This synthesis was performed using a soft template approach, with cetyltriethylammonium bromide (CTAB) as the template. The structure and properties of the catalyst thus synthesized were investigated by X-ray diffraction (XRD), N₂ sorption, transmission electron microscopy (TEM), temperature-programmed desorption of NH₃ (NH₃-TPD), and pyridine sorption FTIR (Py-FTIR). These studies determined that the niobium phosphate not only had a large surface area (>200 m²·g^-1) and narrow pore size distribution (3.5 nm), but also had relatively strong Lewis and Brønsted acidity. This catalyst was found to be capable of producing furfural via a simple one-pot process, including the isomerization of xylose to xylulose and subsequent dehydration. The influence of several variables including temperature, mass ratio of xylose/catalyst, and reaction time on the extent of xylose conversion and furfural yield were studied. Under optimal conditions, the yield of furfural in aqueous solution reached 49.8% with 96.5% xylose conversion. It was further determined that both the yield and the separation of furfural could be improved by employing a methyl isobutyl ketone (MIBK)/water (volume ratio 7:3) biphase containing NaCl in the aqueous phase, resulting in a 68.4% yield.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

介孔磷酸铌一锅法高效催化木糖制备糠醛

English

One-Pot Catalytic Conversion of Xylose to Furfural on Mesoporous Niobium Phosphate

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

介孔磷酸铌一锅法高效催化木糖制备糠醛

English

One-Pot Catalytic Conversion of Xylose to Furfural on Mesoporous Niobium Phosphate

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs