活性炭负载无卤素铜催化剂催化液相甲醇一步氧化合成甲缩醛性能

李心灵; 林慧博; 卢洁; 肖婉婧; 李文杰; 何梓瑞; 邓志勇

doi:10.12434/j.issn.2097-2547.20240284

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活性炭负载无卤素铜催化剂催化液相甲醇一步氧化合成甲缩醛性能

甲醇合成与催化转化 | 更新时间：2025-05-29

- 活性炭负载无卤素铜催化剂催化液相甲醇一步氧化合成甲缩醛性能
- Performance of halogen-free activated carbon loaded copper catalysts for one-step oxidation of liquid-phase methanol to dimethoxymethane
- 低碳化学与化工 2025, 50(5): 110-119.
- 作者机构：
  
  成都信息工程大学资源环境学院中-塞环境与能源“一带一路”联合实验室大气环境模拟与污染控制四川省高校重点实验室，四川成都 610225
- 作者简介：
  
  李心灵，（1999—），硕士研究生，研究方向为催化新材料、碳一化学，E-mail：1033493270@qq.com。
  邓志勇，（1983—），博士，教授，研究方向为催化新材料、碳一化学和精细化工，E-mail：dengzhiyong@cuit.edu.cn。
- 基金信息：
  
  四川省科技计划(2021YFG0225;2024ZHCG0126);四川省中央引导地方科技发展专项自由探索类基础研究(2022ZYD0049);大学生创新创业训练项目(202410621346)
- DOI：10.12434/j.issn.2097-2547.20240284
  中图分类号： TQ519;O621
- 收稿日期：2024-07-03，
  
  修回日期：2024-08-19，
  
  纸质出版日期：2025-05-25
- 稿件说明：
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李心灵,林慧博,卢洁等.活性炭负载无卤素铜催化剂催化液相甲醇一步氧化合成甲缩醛性能[J].低碳化学与化工,2025,50(05):110-119.

LI Xinling,LIN Huibo,LU Jie,et al.Performance of halogen-free activated carbon loaded copper catalysts for one-step oxidation of liquid-phase methanol to dimethoxymethane[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(05):110-119.
李心灵,林慧博,卢洁等.活性炭负载无卤素铜催化剂催化液相甲醇一步氧化合成甲缩醛性能[J].低碳化学与化工,2025,50(05):110-119. DOI： 10.12434/j.issn.2097-2547.20240284.

LI Xinling,LIN Huibo,LU Jie,et al.Performance of halogen-free activated carbon loaded copper catalysts for one-step oxidation of liquid-phase methanol to dimethoxymethane[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(05):110-119. DOI： 10.12434/j.issn.2097-2547.20240284.

摘要

为解决卤素铜催化剂在液相甲醇一步氧化合成甲缩醛反应中腐蚀不锈钢设备的问题，采用等体积浸渍法制备了无卤素铜负载的活性炭（Cu/AC）催化剂，考察了Cu/AC催化剂液相甲醇一步氧化合成甲缩醛的催化性能。通过N

吸/脱附

、XRD、XPS、TEM和H

-TPR等对Cu/AC催化剂的理化性质进行了表征。考察了Cu负载量、焙烧温度对Cu/AC催化剂结构及催化性能的影响。结果表明，当Cu负载量（质量分数）为5.0%、焙烧温度为200 ℃时，Cu颗粒均匀地分散在活性炭表面，且此时Cu颗粒粒径最小（12.0 nm）、Cu

和Cu

含量最高，催化剂催化性能最好。在反应温度为130 ℃、O

压力为3.0 MPa条件下，甲醇转化率和甲缩醛选择性分别为8.1%和92.7%。其中，5Cu/AC-200催化剂循环5次后甲缩醛选择性从首次的92.7%增大至循环后的100.0%。

Abstract

To solve the defects of corrosion on stainless steel equipment with halogen-containing copper catalysts in the one-step oxidation of liquid methanol to synthesize dimethoxymethane

halogen-free activated carbon loaded copper (Cu/AC) catalysts were prepared by equal volume impregnation method. The catalytic performance of Cu/AC catalysts for the one-step oxidation of liquid-phase methanol to dimethoxymethane was investigated. The physicochemical properties of the Cu/AC catalysts were characterized by N

adsorption/desorption

XRD

XPS

TEM and H

-TPR. The effects of Cu loadings and calcination temperatures on the structure and catalytic performance of Cu/AC catalysts were investigated. The results show that when the Cu loading (mass fraction) is 5% and the calcination temperature is 200 ℃

the Cu particles are dispersed uniformly on the surface of the activated carbon with the smallest particle size (12.0 nm) and Cu

and Cu

contents are the highest and the catalyst shows the best catalytic performance. The methanol conversion and dimethoxymethane selectivity are 8.1% and 92.7%

respectively

under the conditions of temperature of 130 ℃ and O

pressure of 3 MPa. Among them

the selectivity of dimethoxymethane increases from 93.9% in the first cycle to 100.0% after 5 cycles of 5Cu/AC-200 catalyst.

关键词

Keywords

references

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