介孔Mn0.5Fe0.5Ox颗粒的制备及其在醇胺氧化偶联反应中的应用

程高; 凌伟钊; 陈世鸿; 罗佳锦; 王丹琳; 黄俊诗; 刘文秀; 王钊颖; 余林; 孙明

doi:10.12052/gdutxb.230124

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介孔Mn_0.5Fe_0.5O_x颗粒的制备及其在醇胺氧化偶联反应中的应用

催化与能源材料 | 更新时间：2026-05-27

- 介孔Mn_0.5Fe_0.5O_x颗粒的制备及其在醇胺氧化偶联反应中的应用
- Preparation of Mesoporous Mn_0.5Fe_0.5O_x Particles and Their Application in the Oxidative Coupling Reaction of Alcohols with Amines
- 广东工业大学学报 2023年40卷第6期页码：124-130
- 作者机构：
  
  广东工业大学轻工化工学院,广东,广州,510006
- 作者简介：
  
  程高(1988–)，男，讲师，主要研究方向为催化新材料的构筑及其应用
  孙明(1978–)，男，教授，主要研究方向为纳米材料的设计制备及其在环境催化和能源等领域的应用，E-mail：sunmgz@gdut.edu.cn
- 基金信息：
  
  广东省自然科学基金资助项目(2018A030310563);广州市科技计划项目(202201010373)
- DOI：10.12052/gdutxb.230124
  中图分类号： O625.6
- 网络首发：2023-11-25，
  
  纸质出版：2023
- 稿件说明：
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程高, 凌伟钊, 陈世鸿, 罗佳锦, 王丹琳, 黄俊诗, 刘文秀, 王钊颖, 余林, 孙明. 介孔Mn_0.5Fe_0.5O_x颗粒的制备及其在醇胺氧化偶联反应中的应用[J]. 广东工业大学学报, 2023, 40(6): 124-130. DOI: 10.12052/gdutxb.230124.

Cheng Gao, Ling Wei-zhao, Chen Shi-hong, et al. Preparation of Mesoporous Mn_0.5Fe_0.5O_x Particles and Their Application in the Oxidative Coupling Reaction of Alcohols with Amines[J]. 2023, 40(6): 124-130. DOI: 10.12052/gdutxb.230124.
程高, 凌伟钊, 陈世鸿, 罗佳锦, 王丹琳, 黄俊诗, 刘文秀, 王钊颖, 余林, 孙明. 介孔Mn_0.5Fe_0.5O_x颗粒的制备及其在醇胺氧化偶联反应中的应用[J]. 广东工业大学学报, 2023, 40(6): 124-130. DOI: 10.12052/gdutxb.230124. DOI：

Cheng Gao, Ling Wei-zhao, Chen Shi-hong, et al. Preparation of Mesoporous Mn_0.5Fe_0.5O_x Particles and Their Application in the Oxidative Coupling Reaction of Alcohols with Amines[J]. 2023, 40(6): 124-130. DOI: 10.12052/gdutxb.230124. DOI：

摘要

研发一种廉价、高效的催化剂以提高醇胺氧化偶联合成亚胺的催化活性具有重要意义。本文采用简单的共沉淀法制备了一系列锰铁双金属氧化物，并将其应用于苯甲醇和苯胺氧化偶联合成N-苄叉苯胺的催化反应，以及探索了不同的锰铁投料比对产物催化活性的影响。结果表明，锰铁投料比为1:1时的产物(Mn

0.5

)具有最佳的催化活性，其苯胺转化率为74.7%，N-苄叉苯胺的选择性和收率分别为99.9%和74.6%。通过多种表征发现，Mn

0.5

具有丰富的介孔结构和表面吸附氧物种以及优异的氧化能力，因而展现出优异的催化活性。本文所制备的高活性催化剂在醇胺氧化偶联制备亚胺的方法中具有较大的应用潜力。

Abstract

It is of great significance to develop an inexpensive and efficient catalyst to enhance the catalytic activity of oxidation coupling of alcohols with amines to imine. In this research

a series of manganese-iron bimetallic oxide catalysts have been prepared by a simple co-precipitation method

which were applied to the catalytic reaction of oxidation coupling of benzyl methanol with aniline to N-benzylideneaniline. The effects of different Fe/Mn feed ratios on the catalytic a

ctivity of the products have been explored. The Mn

0.5

sample with a Fe/Mn feed ratio of 1:1 demonstrated the best catalytic activity

giving an aniline conversion rate of 74.7%

99.9% selectivity and 74.6% yield of N-benzylidene

respectively. Through a variety of characterizations

0.5

exhibited rich mesoporous structure and surface adsorbed oxygen species

as well as excellent oxidation ability. The high-efficiency catalyst synthesized in this work has great application potential in the preparation of imines by oxidation coupling of alcohols with amines.

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references

WANG Y, ZHANG Q, LI F, et al . Donor/acceptor maleimide and itaconimide dyes: synthesis, fluorescence and electrochemical properties [J ] . Dyes and Pigments, 2020, 172: 107823.

HAN Y, XING K, ZHANG J, et al . Application of sulfoximines in medicinal chemistry from 2013 to 2020 [J ] . European Journal of Medicinal Chemistry, 2021, 209: 112885.

SU S, CHEN L, HAO L, et al . Preparation of p-amino salicylic acid-modified polysuccinimide as water-based nanocarriers for enhancing pesticide stability and insecticidal activity [J ] . Colloids and Surfaces B:Biointerfaces, 2021, 207: 111990.

GUO X, LI M, ZHAO P, et al . Vanadium doped OMS-2 catalysts for one-pot synthesis of imine from benzyl alcohol and aniline: effects of vanadium content and precursor [J ] . Catalysis Communications, 2022, 172: 106540.

MA J, YU X, LIU X, et al . The preparation and photocatalytic activity of Ag-Pd/g-C 3 N 4 for the coupling reaction between benzyl alcohol and aniline [J ] . Molecular Catalysis, 2019, 476: 110533.

OLIVEIRA R L, LEDWA K A, CHERNYAYEVA O, et al . Cerium oxide nanoparticles confined in doped mesoporous carbons: a strategy to produce catalysts for imine synthesis [J ] . Inorganic Chemistry, 2023, 62(33): 1355 4-13565.

ALCAMAND H A, OLIVEIRA H D S, BALENA J G, et al . Synthesis, characterization, and use of nanocast LaMnO 3 perovskites in the catalytic production of imine by the gas-phase oxidative coupling of benzyl alcohol to aniline [J ] . Catalysis Communications, 2023, 175: 106606.

CHEN F, YANG T, ZHAO S, et al . Highly selective oxidation of amines to imines by Mn 2 O 3 catalyst under eco-friendly conditions [J ] . Chinese Chemical Letters, 2019, 30(12): 2282-2286.

WU S, ZHANG H, CAO Q, et al . Efficient imine synthesis via oxidative coupling of alcohols with amines in an air atmosphere using a mesoporous manganese-zirconium solid solution catalyst [J ] . Catalysis Science Technology, 2021, 11(3): 810-822.

QIN L, HUANG X, ZHAO B, et al . Iron oxide as a promoter for toluene catalytic oxidation over Fe-Mn/ γ -Al 2 O 3 catalysts [J ] . Catalysis Letters, 2020, 150(3): 802-814.

SAID S, RIAD M. Oxidation of benzyl alcohol through eco-friendly processes using Fe-doped cryptomelane catalysts [J]. Solid State Sciences, 2019, 94: 145-154.

CHEN C, LI Y, YANG Y, et al . Unique mesoporous amorphous manganese iron oxide with excellent catalytic performance for benzene abatement under UV-vis-IR and IR irradiation [J ] . Environmental Science:Nano, 2019, 6: 1233-1245.

YANG S, QI Z, WEN Y, et al . Generation of abundant oxygen vacancies in Fe doped δ -MnO 2 by a facile interfacial synthesis strategy for highly efficient catalysis of VOCs oxidation [J ] . Chemical Engineering Journal, 2023, 452(4): 139657.

WEN Z, LU J, ZHANG Y, et al . Simultaneous oxidation and immobilization of arsenite from water by nanosized magnetic mesoporous iron manganese bimetal oxides (Nanosized-MMIM) : synergistic effect and interface catalysis [J ] . Chemical Engineering Journal, 2020, 391: 123578.

MASTALIR M, GLATZ M, GORGAS N, et al . Divergent coupling of alcohols and amines catalyzed by isoelectronic hydride Mn-I and Fe-II PNP pincer complexes [J ] . Chemistry-a European Journal, 2016, 22(35): 12316-12320.

HUANG N, QU Z, DONG C, et al . Superior performance of α @ β -MnO 2 for the toluene oxidation: active interface and oxygen vacancy [J ] . Applied Catalysis A:General, 2018, 560: 195-205.

LI P, ZHAN S, YAO L, et al . Highly porous alpha-MnO 2 nanorods with enhanced defect accessibility for efficient catalytic ozonation of refractory pollutants [J ] . Journal of Hazardous Materials, 2022, 437: 129235.

ZHANG C, CAO Y, WANG Z, et al . Insights into the sintering resistance of sphere-like Mn 2 O 3 in catalytic toluene oxidation: effect of manganese salt precursor and crucial role of residual trace sulfur [J ] . Industrial Engineering Chemistry Research, 2022, 61(19): 6414-6426.

TAHIR A A, WIJAYANTHA K U, SAREMI-YARAHMADI S, et al . Nanostructured α -Fe 2 O 3 thin films for photoelectrochemical hydrogen generation [J ] . Chemistry of Materials, 2009, 21(16): 3763-3772.

QIU J, WANG W, WANG J, et al . Efficient monolithic MnO x catalyst prepared by heat treatment for ozone decomposition [J ] . Environmental Science and Pollution Research, 2022, 29: 44324-44334.

LIU Y, ZHANG P. Catalytic decomposition of gaseous ozone over todorokite-type manganese dioxides at room temperature: effects of cerium modification [J]. Applied Catalysis A:General, 2017, 530: 102-110.

SHI J, QI T, SUN B-C, et al . Catalytic oxidation of benzyl alcohol over MnO 2 : structure-activity description and reaction mechanism [J ] . Chemical Engineering Journal, 2022, 440: 135802.

WANG H, CHEN H, WANG Y, et al . Performance and mechanism comparison of manganese oxides at different valence states for catalytic oxidation of NO [J ] . Chemical Engineering Journal, 2019, 361: 1161-1172.

ALBRECHT M, RODEMERCK U, SCHNEIDER M, et al . Unexpectedly efficient CO 2 hydrogenation to higher hydrocarbons over non-doped Fe 2 O 3 [J ] . Applied Catalysis B:Environmental, 2017, 204: 119-126.

QIN J, LONG Y, GOU G, et al . Tuning effect of amorphous Fe 2 O 3 on Mn 3 O 4 for efficient atom-economic synthesis of imines at low temperature: improvingtransfer cycle of Mn 3+ /Mn 2+ in Mn 3 O 4 [J ] . Catalysis Science Technology, 2020, 10: 5628-5640.

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