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Gold nanoparticles on mesoporous Cerium-Tin mixed oxide for aerobic oxidation of benzyl alcohol
Journal of Molecular Catalysis A: Chemical Pub Date : 2016 , DOI: 10.1016/j.molcata.2016.03.026
Chiranjit Santra , Malay Pramanik , Kyoko K. Bando , Sudip Maity , Biswajit Chowdhury

In the era of sustainable chemistry the development of nanocatalysis has drawn special attention. Here we report the preparation of nanocrystalline, mesoporous cerium-tin oxide solid solutions and tested for selective oxidation of benzyl alcohol, cinnamyl alcohol, 4-methylbenzyl alcohol, 2-octanol, and geraniol using molecular oxygen as an oxidant. Among different mesoporous supports with Ce/Sn compositions (98/2, 95/5, 90/10 and 80/20, the highest activity was found for the Ce-Sn mixed oxide (Ce/Sn = 95/5) supported gold nanoparticles. The microkinetic study shows that there was no mass transfer limitation in three phase catalytic system. The supports and the corresponding gold catalysts were extensively characterized by N2 physisorption, XRD, H2-TPR, NH3-TPD, TEM, XPS, RAMAN and XAFS techniques. The nanocrystalline solid solution of CexSn1-xO2 was detected by XRD analysis. The presence of oxide vacancy was confirmed by XPS and RAMAN studies. The reducibility of Ce-Sn mixed oxide support increased upon gold deposition which was confirmed by H2-TPR techniques. The TPD study indicates the alteration of acid-basic sites of the CeO2 oxide upon incorporation of tin and gold nanoparticles. The cooperative role between the gold species and the ceria-tin support has been observed while correlating the catalytic activity results with the characterization studies.

中文翻译:

介孔铈锡复合氧化物上的金纳米颗粒有氧氧化苯甲醇

在可持续化学时代,纳米催化的发展引起了人们的特别关注。在这里,我们报告了纳米晶,介孔铈锡氧化物固溶体的制备,并测试了使用分子氧作为氧化剂对苯甲醇,肉桂醇,4-甲基苯甲醇,2-辛醇和香叶醇的选择性氧化。在具有Ce / Sn组成(98 / 2、95 / 5、90 / 10和80/20)的不同介孔载体中,发现Ce-Sn混合氧化物(Ce / Sn = 95/5)负载的金纳米颗粒的活性最高微动力学研究表明,三相催化体系没有传质限制,载体和相应的金催化剂具有N 2物理吸附,XRD,H 2 -TPR,NH 3广泛表征。-TPD,TEM,XPS,RAMAN和XAFS技术。通过XRD分析来检测Ce x Sn 1-x O 2的纳米晶固溶体。XPS和RAMAN研究证实了氧化物空位的存在。Ce-Sn混合氧化物载体的还原性随着金的沉积而增加,这通过H 2 -TPR技术得到了证实。TPD研究表明,在掺入锡和金纳米颗粒后,CeO 2氧化物的酸碱性位点发生了变化。在将催化活性结果与表征研究联系起来的同时,还观察到了金和铈-锡载体之间的协同作用。
更新日期:2017-01-31
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