助剂含量对CuLi/AC催化剂结构及甲醇氧化羰基化反应性能的影响

被引：15

作者：

任军

王冬蕾

裴永丽

秦志峰

林建英

李忠

机构：

[1] 太原理工大学煤科学与技术教育部和山西省重点实验室

来源：

高等学校化学学报 | 2013年 / 34卷 / 11期

关键词：

CuLi/AC催化剂; Li助剂; 微波辐射; 碳酸二甲酯; 氧化羰基化;

D O I：

暂无

中图分类号：

O643.36 [催化剂];

学科分类号：

070305 [高分子化学与物理];

摘要：

采用微波辐射法制备出不同助剂含量的CuLi/AC(活性炭)催化剂,考察了其在甲醇气相氧化羰基化合成碳酸二甲酯(DMC)反应中的催化性能,使用X射线衍射、扫描电子显微镜、比表面积、H2程序升温还原、X射线光电子能谱和CO程序升温脱附对催化剂的结构进行了表征.研究结果表明,添加适量的Li有助于铜物种还原为低价态的Cu0,形成颗粒尺寸更小、分布更加均匀的铜纳米颗粒,并高度分散在活性炭载体表面.催化剂活性与表面单质铜的含量有关,即Cu0是催化剂的主要活性物种,并且Cu0的晶粒尺寸越小,催化剂活性越好.添加Li后增加了催化剂表面的CO弱吸附位,有利于CO对Cu—OCH3的插入反应,因此提高了催化活性.随着Li含量的增加,DMC的时空收率逐渐升高,当Li添加质量分数达到0.15%时,DMC的时空收率达到最高值540.6 mg·g-1·h-1,甲醇转化率为4.5%,DMC选择性为81.4%.

引用

页码：2594 / 2600

页数：7

共 20 条

[1]

Oxidative carbonylation of methanol to dimethyl carbonate over CuCl/SiO 2 –TiO 2 catalysts prepared by microwave heating: The effect of support composition.[J].Jun Ren;Shusen Liu;Zhong Li;Xinglu Lu;Kechang Xie.Applied Catalysis A; General.2009, 1

[2]

Effect of Li Promoter on titania-supported Rh catalyst for ethanol formation from CO hydrogenation.[J].Adefemi Egbebi;Viviane Schwartz;Steven H. Overbury;James J. Spivey.Catalysis Today.2009, 1

[3]

Effects of zeolite structure and composition on the synthesis of dimethyl carbonate by oxidative carbonylation of methanol on Cu-exchanged Y, ZSM-5, and Mordenite [J].

Zhang, Yihua ;

Briggs, Daniel N. ;

de Smit, Emiel ;

Bell, Alexis T. .

JOURNAL OF CATALYSIS, 2007, 251 (02) :443-452

[4]

Gas-phase carbonylation of methanol to dimethyl carbonate on chloride-free Cu-precipitated zeolite Y at normal pressure.[J].M. Richter;M.J.G. Fait;R. Eckelt;M. Schneider;J. Radnik;D. Heidemann;R. Fricke.Journal of Catalysis.2006, 1

[5]

Dimethyl carbonate production via the oxidative carbonylation of methanol over Cu/SiO 2 catalysts prepared via molecular precursor grafting and chemical vapor deposition approaches.[J].Ian J. Drake;Kyle L. Fujdala;Alexis T. Bell;T. Don Tilley.Journal of Catalysis.2004, 1

[6]

The role of copper chloride hydroxides in the oxidative carbonylation of methanol for dimethyl carbonate synthesis.[J].Man Seok Han;Byung Gwon Lee;Byoung Sung Ahn;Hoon Sik Kim;Dong Ju Moon;Suk In Hong.Journal of Molecular Catalysis. A; Chemical.2003, 1

[7]

Developments in the production and application of dimethylcarbonate.[J].Daniele Delledonne;Franco Rivetti;Ugo Romano.Applied Catalysis A; General.2001, 1

[8]

Dimethyl carbonate synthesis by oxidative carbonylation on activated carbon supported CuCl2 catalysts:: catalytic properties and structural change [J].

Tomishige, K ;

Sakaihori, T ;

Sakai, S ;

Fujimoto, K .

APPLIED CATALYSIS A-GENERAL, 1999, 181 (01) :95-102

[9]

Oxidative carbonylation of methanol to dimethyl carbonate by solid-state ion-exchanged CuY catalysts.[J].S.T. King.Catalysis Today.1997, 1

[10]

Reaction Mechanism of Oxidative Carbonylation of Methanol to Dimethyl Carbonate in Cu–Y Zeolite.[J].S.T King.Journal of Catalysis.1996, 2

← 1 2 →