[1]潘明希,罗传宝,徐莉萍,等.烷基叔胺的合成及其新催化剂表征与性能研究[J].徐州工程学院学报(自然科学版),2017,(1):59-66.
 PAN Mingxi,LUO Chuanbao,XU Liping,et al.Synthesis of Alkyl Tertiary Amines and the Characterization and Properties of its New Catalysts[J].Journal of Xuzhou Institute of Technology(Natural Sciences Edition),2017,(1):59-66.
点击复制

烷基叔胺的合成及其新催化剂表征与性能研究()
分享到:

《徐州工程学院学报》(自然科学版)[ISSN:1674-358X/CN:32-1789/N]

卷:
期数:
2017年第1期
页码:
59-66
栏目:
专家特稿
出版日期:
2017-02-28

文章信息/Info

Title:
Synthesis of Alkyl Tertiary Amines and the Characterization and Properties of its New Catalysts
文章编号:
1674-358X(2017)01-0059-08
作者:
潘明希罗传宝徐莉萍周 涛杨新蔚丛 畅周康钰
中南大学 化学化工学院,湖南 长沙 410083
Author(s):
PAN MingxiLUO ChuanbaoXU LipingZHOU TaoYANG XinweiCHONG ChangZHOU Kangyu
College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
关键词:
烷基叔胺 Ni-Cu-Mg-Fe负载型催化剂 KBH4
Keywords:
Alkyl Tertiary Amine Ni-Cu-Mg-Fe supported catalyst KBH4
分类号:
O625.67
文献标志码:
A
摘要:
文章主要研究一种在烷基叔胺成产工艺脱氢加氢阶段有着极大应用价值的新型非均相Ni-Cu-Mg-Fe负载型催化剂.采用Fe元素对传统的Ni-Cu-Mg(Zn)催化剂改性,使用KBH4对催化剂活化还原,通过XPS、XRD和SEM等手段及叔胺合成对比反应分析可知:Fe的添加可提高催化剂活性组分的分散度,因此Ni-Cu-Mg-Fe负载型催化剂在脱氢和加氢方面展现出了比Ni-Cu-Mg(Zn)负载型催化剂和Ni-Cu-Zn-Fe负载型催化剂更高的活性; Ni-Cu-Mg-Fe四元负载型催化剂活性组分最佳物质的量比为1.25:1:0.3:0.6,此配比的四元催化剂对叔胺的选择性为96.3%.
Abstract:
The traditional Ni-Cu-Mg(Zn)catalyst was modified with Fe element and the catalyst was activated with KBH4.XPS,XRD and SEM were used to analyze the reaction of tertiary amine synthesis.The result show that the addition of Fe improves the dispersion of the active components of the catalyst, so the Ni-Cu-Mg-Fe catalyst exhibited higher catalytic activity on the aspect of dehydrogenation and hydrogenation than the Ni-Cu-Mg(Zn)catalyst and Ni-Cu-Zn-Fe catalyst; the optimal molar ratio of the Ni-Cu-Mg-Fe catalyst is nNi:nCu:nMg:nFe=1.25:1:0.3:0.6 which could improve the yield of the tertiary amine to 96.3%.

参考文献/References:

[1] LI Y,LI Q,ZHI L,et al.Catalytic amination of octanol for synthesis of trioctylamine and catalyst characterization[J].Catalysis letters,2011,141(11):1635-1642.
[2] XU L W,LI L,CAI Y F.Aldol Reaction-Homogeneous//Encyclopedia of Catalysis[J].Waohington:Wiley-Interscience,2011.
[3] 李运玲.催化胺化制三烷基叔胺的研究[D].太原:山西大学,2012.
[4] RUCKER R P,WHITTAKER A M,DANG H,et al.Synthesis of tertiary alkyl amines from terminal alkenes:copper-catalyzed amination of alkyl boranes.[J].Journal of the American Chemical Society,2012,134(38):6571-6574.
[5] KIMURA H.Progress in one-step amination of long-chain fatty alcohols with dimethylamine-development of key technologies for industrial applications,innovations,and future outlook[J].Catalysis Reviews:Science and Engineering,2011,53(1):1-90.
[6] KIMURA H,MATSUTANI K,TSUTSUMI S,et al.Basic function of Cu/Ni-based catalyst in a colloidal state for one-pot amination alcohols to N,N-dimethyl tertiary amines[J].Catalysis letters,2005,99(3):119-131.
[7] LI Y,LI Q,ZHI L,et al.Catalytic amination of octanol for synthesis of trioctylamine and catalyst characterization[J].Catalysis letters,2011,141(11):1635-1642.
[8] NAGHASH A R,ETSELL T H,XU S.XRD and XPS Study of Cu-Ni Interactions on Reduced Copper-Nickel-Aluminum Oxide Solid Solution Catalysts[J].Chemistry of Materials,2006,18(10):2480-2488.
[9] BRIDIER B,PéREZ-RAMíREZ J.Cooperative effects in ternary Cu-Ni-Fe catalysts lead to enhanced alkene selectivity in alkyne hydrogenation.[J].Journal of the American Chemical Society,2013,132(12):4321-4327.
[10] 侯文端.多功能有机催化剂的设计、合成及催化硝基烯的Michael/Mannich串联反应研究[D].重庆:西南大学,2003.
[11] KIMURA H,YOKOTA Y,SAWAMOTO Y.Amination of alcohols,using Cu/Ni-based colloidal catalyst,for consecutive reaction system[J].Catalysis letters,2005,99(3/4):133-140.
[12] JIMÉNEZ-LPEZ A,RODRÍGUEZ-CASTELLN E,MAIRELES-TORRES P,et al.Chromium oxide supported on zirconium- and lanthanum-doped mesoporous silica for oxidative dehydrogenation of propane[J].Applied Catalysis A General,2001,218(1/2):295-306.
[13] HAO Y,WANG X,PERRET N,et al.Support effects in the gas phase hydrogenation of butyronitrile over palladium[J].Maney Publishing Suitec Josephs Well Hanover Walk Leeds Ls3ab Uk,2015,1(1):4-10.
[14] ABELL S,VERBOEKEND D,BRIDIER B,et al.Activated takovite catalysts for partial hydrogenation of ethyne,propyne,and propadiene[J].Journal of Catalysis,2008,259(1):85-95.
[15] LIU X,MENG C,HAN Y.Defective graphene supported MPd12(M = Fe,Co,Ni,Cu,Zn,Pd)nanoparticles as potential oxygen reduction electrocatalysts:a first-principles study[J].Journal of Physical Chemistry C,2013,117(3):1350-1357.
[16] 陈利花,梁小平.纳米六角片状镁铝水滑石晶体的共沉淀法制备[J].徐州工程学院学报(自然科学版),2012,27(2):30-33.
[17] WATSON A J A,MAXWELL A C,WILLIAMS J M J.Borrowing hydrogen methodology for amine synthesis under solvent-free microwave conditions[J].The Journal of Organic Chemistry,2011,76(7):2328-2331.
[18] FAUNGNAWAKIJ K,KIKUCHI R,FUKUNAGA T,et al.Stability enhancement in Ni-promoted Cu-Fe spinel catalysts for dimethyl ether steam reforming[J].Journal of Physical Chemistry C,2009,113(43):18455-18458.
[19] 杨水金,王强,段国滨,等.H4SiW12O40/ZrO2-Al2O3催化合成丁酮1,2-丙二醇缩酮[J].徐州工程学院学报(自然科学版),2012,27(3):22-26.
[20] CANGIANO M D L A,OJEDA M W,CARRERAS A C,et al.A study of the composition and microstructure of nanodispersed Cu-Ni alloys obtained by different routes from copper and nickel oxides[J].Materials Characterization,2010,61(61):1135-1146.
[21] KIM T H,MIN J,PARK J K.Bifunctionalized mesoporous molecular sieve for perchlorate removal[J].Microporous & Mesoporous Materials,2008,108(1/2/3):22-28.
[22] KIM H J,PARK S,KIM S H,et al.Biocompatible Cellulose Nanocrystals As Supports to Immobilize Lipase[J].Journal of Molecular Catalysis B:Enzymatic,2015,122:170-178.
[23] SUN J,ZHANG L,GE C,et al.Comparative study on the catalytic CO oxidation properties of CuO/CeO2 catalysts prepared by solid state and wet impregnation[J].Chinese Journal of Catalysis,2014,35(8):1347-1358.

备注/Memo

备注/Memo:
收稿日期:2016-10-03 基金项目:国家自然科学基金(21176266) 作者简介:潘明希(1990-),男,硕士研究生,主要从事叔胺合成及其催化剂表征与性能研究. 通讯作者:周 涛(1963-),男,教授,博士,博士生导师,从事纳米材料、超微细颗粒的制备和表面改性、多相流与流态化技术研究.
更新日期/Last Update: 1900-01-01