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锌对非晶态Co-B合金的改性及催化肉桂醛加氢为肉桂醇的研究
  • ISSN号:1001-3555
  • 期刊名称:《分子催化》
  • 时间:0
  • 分类:O543.32[理学—物理]
  • 作者机构:[1]广州大学化学化工学院,广东广州510006, [2]广西大学化学化工学院,广西南宁530004, [3]天津大学药学院,天津300072, [4]广西大学材料科学研究所,广西南宁530004
  • 相关基金:国家自然科学基金资助项目(No.20266001)和广西高校百名中青年学科带头人资助项目(No.[2002]467).
中文摘要:

采用KBH4还原法制备了非晶态Co-B和Co-Zn-B催化剂,以肉桂醛选择加氢制肉桂醇为探针反应,研究了Zn对Co-B非晶态催化剂的修饰改性作用,并采用XRD、DSC、XPS、和H2-TPD对催化剂进行了表征.研究表明,少量的Zn没有改变Co-B催化剂的非晶结构,但提高了催化剂主体的热稳定性,其中1%的Zn可使Co-B非晶态催化剂主体结晶放热峰提高12K,并在665K出现新的H2脱附峰,说明催化剂因掺人锌形成了新的氢吸附中心,锌在催化剂中以金属态和氧化态两种形式存在.催化剂的整体均衡而局部电子分布不均衡的缺陷势结构增强了对肉桂醛分子C=O双键O原子的侧链偶合吸附与金属氧化物的金属离子对羰基的极化作用协同活化了肉桂醛的C=O双键,提高了催化剂对C=O双键的加氢选择性.加氢反应工艺条件及催化剂寿命研究表明,适宜的反应温度为413K,氢压为2.5MPa,反应时间为3.0h,肉桂醇的最高产率可达84.0%,并具有较好的催化稳定性.

英文摘要:

Amorphous Co-B and Co-Zn-B alloy catalysts were prepared by the method of chemical reduction with KBH+ in aqueous solution. Zn promotion effect to Co-B catalyst and the performance of the Co-Zn-B catalysts were investigated by the selectivity hydrogenation of cinnamaldehyde (CMA) to cinnamyl alcohol(CMO). It was indicated from XRD and DSC that the presence of Zn could hardly change the amorphous structure of Co-B catalyst, and the peak of crystalization heat of 1% Co-Zn-B catalyst was 15 K higher than Co-B catalyst which revealed that suitable Zn-content was favorable to increase the thermal stability of Co-B catalyst. On the profile of H2-TPD, a new H2-desorption peak was observed at 655 K which showed that a new H2-absorption site was formed. The results of XPS showed that the Zn composition elements of Co-Zn-B amorphous catalyst were all existed at both states of reduction and oxidation. This chemical shift of binding energy caused a deficient potential formed that was equilib- rium on the whole, but the electron distributing was unbalanced on part. The effect of the coupled absorption of this dificent site to the side-bond of C = O group and the polarization effect of the oxide metal of Co-Zn-B catalyst to carbonyl increased the selective hydrogenation of C = O group of the catalyst. The reaction conditions and stability were also investigated. The optimum reaction conditions was determined as T (temperature) = 413 K, P,2 (H2 pressure) = 2.5 MPa, and t(reaction time) =3.0 h, and the highest yield of CMO reached 84.0%. The stability of the catalyst is excellent.

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期刊信息
  • 《分子催化》
  • 中国科技核心期刊
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院兰州化学物理研究所
  • 主编:李树本
  • 地址:兰州市天水路18号
  • 邮编:730000
  • 邮箱:fzch@licp.cas.cn
  • 电话:0931-4968226
  • 国际标准刊号:ISSN:1001-3555
  • 国内统一刊号:ISSN:62-1039/O6
  • 邮发代号:54-69
  • 获奖情况:
  • 1992年获中国科学院优秀期刊三等奖,1992年获甘肃省第二届优秀科技期刊荣誉称号
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,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),中国北大核心期刊(2000版)
  • 被引量:7932