期刊文献+

碱土金属对CuZrO_(2)催化剂上乙醇制备酮类化合物性能的影响

Effect of alkaline-earth metals on the catalytic performance of CuZrO_(2)for ketone synthesis from ethanol
原文传递
导出
摘要 以碱土金属通过共沉淀法改性CuZrO_(2)催化剂,制得了不同碱土金属改性的M-CuZrO_(2)催化剂(M=Mg、Ca、Sr和Ba),并将其用于催化乙醇一步法制备酮类化合物的反应中。采用BET、XRD、氢气程序升温还原(H_(2)-TPR)、乙醇程序升温表面反应(乙醇-TPSR)、CO_(2)程序升温脱附(CO_(2)-TPD)以及XPS对催化剂的体相结构、性质进行了研究。结果表明,以碱土金属Ba改性的Ba-CuZrO_(2)催化剂上Cu 2p_(3/2)结合能较高,有利于乙醇分子中O—H键断裂形成乙醛,且该催化剂表面乙醛脱附量最大、中强碱性位(晶格氧)碱性最强,明显促进了缩合反应的进行。在350℃、0.1 MPa、N_(2)为载气、气时空速(GHSV)为2000 h^(–1)、乙醇进样量为1.8 mLC2H5OH/(mL_(cat)·h)的条件下,Ba-CuZrO_(2)催化剂上乙醇转化率和酮类产物选择性最高,分别为98.1%和51.1%,且在45 h内具有较好的催化稳定性。 M-CuZrO_(2)catalysts(M=Mg,Ca,Sr and Ba)were prepared by modification of CuZrO_(2) catalysts with different alkaline-earth metals via co-precipitation method,and then employed to catalyze the one-step synthesis of ketones from ethanol.The structure and properties of catalysts obtained were characterized and analyzed by BET,XRD,H_(2)-TPR,ethanol-TPSR,CO_(2)-TPD and XPS.The results showed that Ba-CuZrO_(2) catalyst exhibited higher Cu 2p_(3/2) electron binding energy,which was in favor of the O—H bond breakage in ethanol molecules to acetaldehyde formation.Moreover,Ba-CuZrO_(2) catalyst displayed largest acetaldehyde desorption and strongest alkalinity of medium strength alkaline site(lattice oxygen),which demonstrated a significant promotion effect on the condensation reaction.Under reaction conditions of 350℃,0.1 MPa,N_(2)as carrier gas,GHSV 2000 h^(–1) and ethanol feed of 1.8 mLC2H5OH/(mLcat·h),catalysis with Ba-CuZrO_(2) achieved highest ethanol conversion rate and ketone product selectivity,98.1%and 51.1%respectively.Moreover,Ba-CuZrO_(2) catalyst maintained stable catalytic activity within 45 h.
作者 魏玲 曾春阳 解红娟 武应全 WEI Ling;ZENG Chunyang;XIE Hongjuan;WU Yingquan(Public Experimental Center,Taiyuan University,Taiyuan 030032,Shanxi,China;China Petroleum ChemicalIndustry Federation,Beijing 100723,China;State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,Shanxi,China)
出处 《精细化工》 EI CAS CSCD 北大核心 2022年第8期1662-1667,共6页 Fine Chemicals
基金 山西省高等学校科技创新项目(2021L577) 山西省自然科学基金(20210302123009)。
关键词 碱土金属 CuZrO_(2)催化剂 乙醇 酮类化合物 缩合反应 催化技术 alkaline-earth metals CuZrO2 catalyst ethanol ketones condensation reaction catalysis technology
  • 相关文献

参考文献12

二级参考文献93

  • 1赵继芳.乙醛缩合法制乙酸乙酯的研究[J].上海化工,2004,29(8):22-24. 被引量:5
  • 2杨树武,周卓华.Cu/ZnO/Al_2O_3/ZrO_2催化剂上乙醇脱氢合成乙酸乙酯Ⅰ.催化反应性能及机理[J].催化学报,1996,17(1):5-9. 被引量:25
  • 3刘灿培,林金火,曾玲玲,吴莎.漆酚与苯胺重氮盐的偶联反应[J].中国生漆,2006,25(1):1-5. 被引量:4
  • 4GB2760--2011,食品添加剂使用标准[s].
  • 5Mull R E Ouanidines with Antihypertensive Activity[J]. Journal of Organic Compounds, 1960, 25(9): 1953-1956.
  • 6Shih Yun-Er, Chen Chao-Tung. Synthesis of Guancthidin,: Sulfate[J]. Bulletin of the Institute of ('hemistr), Academica Sinica, 1980, 27(5): 19-22.
  • 7Dauben H J. Cycloheptanonc[J]. Organic Syntheses, 1963. 8(4): 221-227.
  • 8陈秀英,余一成.胍乙啶的合成[J].药学学报.1964.11(4):281-284.
  • 9Jaffarullah R, Arumugam A, Jha V K, et al. Reduction and Degradation Behavior of Sinter Under Simulated Vertical Probe Trial Condition[J]. Iron Steel Inst Jpn Int, 2008, 48 (7) :918.
  • 10Yamaguchi K, Higuchl K, Hosotani Y, et al. Influence of Micro Pore on Reducibility and Permeability of Sinter Above 1000℃ in Blast Furnaee[J]. Tetsu-to-Haganfi, 1998, 84 (10): 702.

共引文献31

相关作者

内容加载中请稍等...

相关机构

内容加载中请稍等...

相关主题

内容加载中请稍等...

浏览历史

内容加载中请稍等...
;
使用帮助 返回顶部