Preparation of ZrO2/Na-β and ZrO2/H-β catalysts and their catalytic performance for the Meerwein–Ponndorf–Verley reaction of cyclohexanone and isopropanol

Lin-hui Dong, Fan-fei Meng, Li-ye Liu, Jun Qiu
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Abstract

ZrO2/Na-β and ZrO2/H-β catalysts are prepared by the reflux impregnation method and are applied to the Meerwein–Ponndorf–Verley reduction of cyclohexanone and isopropanol. The catalysts are characterized by X-ray diffraction, scanning electron microscopy-energy dispersive spectrum, temperature-programmed desorption of ammonia, N2 isothermal adsorption and desorption, and inductively coupled plasma mass spectrometry. The products are identified by gas chromatography‒mass spectrometry and analyzed by gas chromatography. The experimental results showed that ZrO2/H-β exhibits higher catalytic activity for the above Meerwein–Ponndorf–Verley reduction because ZrO2/H-β has both Zr4+ and Al3+ ion acid centers, which provide the moderately strong acid needed for the reaction. Under optimized conditions, ZrO2/H-β(6) is used as the catalyst, and the conversion rate of cyclohexanone was 92.0% as determined by the area-normalized calculation based on cyclohexanone. The catalyst can be regenerated by programmed heating calcination. The conversion rate of cyclohexanone decreased to 79.4% after five recycling cycles, and its service life needs further study to be improved.
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ZrO2/Na-β和ZrO2/H-β催化剂的制备及其对环己酮与异丙醇Meerwein-Ponndorf-Verley反应的催化性能
采用回流浸渍法制备了ZrO2/Na-β和ZrO2/H-β催化剂,并将其应用于环己酮和异丙醇的Meerwein-Ponndorf-Verley还原反应。采用x射线衍射、扫描电镜-能谱、程序升温解吸氨、N2等温吸附和解吸、电感耦合等离子体质谱等手段对催化剂进行了表征。产物经气相色谱-质谱联用鉴定,气相色谱分析。实验结果表明,ZrO2/H-β对上述Meerwein-Ponndorf-Verley还原反应具有较高的催化活性,因为ZrO2/H-β同时具有Zr4+和Al3+离子酸中心,为反应提供了所需的中等强酸。在优化条件下,以ZrO2/H-β(6)为催化剂,经面积归一化计算,环己酮的转化率为92.0%。催化剂可通过程序加热煅烧再生。循环5次后,环己酮的转化率降至79.4%,其使用寿命有待进一步研究。
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来源期刊
Journal of Chemical Research-s
Journal of Chemical Research-s 化学科学, 有机化学, 有机合成
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期刊介绍: The Journal of Chemical Research is a peer reviewed journal that publishes full-length review and research papers in all branches of experimental chemistry. The journal fills a niche by also publishing short papers, a format which favours particular types of work, e.g. the scope of new reagents or methodology, and the elucidation of the structure of novel compounds. Though welcome, short papers should not result in fragmentation of publication, they should describe a completed piece of work. The Journal is not intended as a vehicle for preliminary publications. The work must meet all the normal criteria for acceptance as regards scientific standards. Papers that contain extensive biological results or material relating to other areas of science may be diverted to more appropriate specialist journals. Areas of coverage include: Organic Chemistry; Inorganic Chemistry; Materials Chemistry; Crystallography; Computational Chemistry.
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