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Dawson结构磷钨酸稀土盐的制备、表征及其催化合成四氢呋喃研究
  • ISSN号:1001-9731
  • 期刊名称:功能材料
  • 时间:2013.6.30
  • 页码:1736-1740
  • 分类:O614.33[理学—无机化学;理学—化学] O643.32[理学—物理化学;理学—化学]
  • 作者机构:[1]浙江工业大学化学工程与材料学院,浙江杭州310014, [2]九江学院化学与环境工程学院,江西九江332005
  • 相关基金:国家自然科学基金资助项目(21161009);江西省自然科学基金资助项目(20122BAB213001,20114BAB213002);江西省教育厅科技资助项目(GJJll613)
  • 相关项目:负载Dawson型磷钨酸盐催化剂的设计合成、催化性能及负载机制研究
中文摘要:

用复分解法合成出通式为RE2P2W18O62(RE—La,Ce,Y)的3种Dawson结构磷钨酸稀土盐,利用IR、SEM、XRD、Py—IR对其结构和酸性进行了表征,并用于催化1,4-丁二醇液相环化脱水合成四氢呋喃。考察了稀土元素种类、催化剂用量、反应时间、反应温度等因素对四氢呋喃收率的影响。结果表明RE2P2W18O62表现出优异的催化活性,当磷钨酸镧用量占1,4-丁二醇质量的1.2%,反应温度为180℃,反应时间为25min,THF收率可达97.6%,催化剂重复使用5次,催化活性有所降低,THF收率仍可达86.6%。采用TG—DTA和Py—IR方法对使用前后催化剂表征结果显示,积碳结焦使催化剂Lewis酸中心减小是催化剂失活的原因。与传统酸性催化剂相比,采用RE2P2W18O62作为反应催化剂不仅提高了反应收率(高于浓硫酸),简化了工艺流程,无酸腐蚀和污染问题,且催化剂无需处理即可重复使用多次。

英文摘要:

Three kinds of rare earth phosphotungstates with dawson structure tormutateo as RE2P2W18O62 (RE=La,Ce,Y)were prepared and used in catalytic synthesis of tetrahydrofuran from 1,4-butanediol. The cata lysts were charactered by FT-IR, XRD and SEM. The influences of rare earth element, catalyst dosage, reac- tion temperature and reaction time were investigated. The results indicated that La2P2W18 062 showed the best catalytic properties in synthesis of tetrahydrofuran among the three rare earth heteropoly salts. Under the opti- mal condition, i.e. m(catalyst) 1.2%(relative to the dosage of 1,4 butanediol), the reaction temperature(oil bath) was 180℃, the reaction time was 25 rain, the average yield of tetrahydrofuran could reach 97.6G. After reaction these catalysts could be recycled and still exhibited catalytic activity with a yield of 86.6% after five cy- cle reactions. It was found by means of TG-DTA and Py IR that the catalyst deactivation was due to decrease of the Lewis acid sites,which was caused by coking on catalyst surface. Compared with using sulfuric acid as cata lyst, the present procedure is a green productive technology characterized by process simplification, higher yield and no corrosion for facilities. Moreover, the La2PeWlsO62 can be used for many times.

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期刊信息
  • 《功能材料》
  • 北大核心期刊(2011版)
  • 主管单位:重庆材料研究院
  • 主办单位:重庆材料研究院
  • 主编:黄伯云
  • 地址:重庆北碚区蔡家工业园嘉德大道8号
  • 邮编:400707
  • 邮箱:gnclwb@126.com
  • 电话:023-68264739
  • 国际标准刊号:ISSN:1001-9731
  • 国内统一刊号:ISSN:50-1099/TH
  • 邮发代号:78-6
  • 获奖情况:
  • 2008、2011年连续获中国精品科技期刊,2010获重庆市双十佳期刊
  • 国内外数据库收录:
  • 美国化学文摘(网络版),荷兰文摘与引文数据库,美国工程索引,日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:30166