Enhanced CuCl dispersion by regulating acidity of MCM-41 for catalytic oxycarbonylation of ethanol to diethyl carbonate

doi:10.1007/s11705-014-1447-5

Front. Chem. Sci. Eng.

2015, Vol. 9

Issue (2) : 224-231 https://doi.org/10.1007/s11705-014-1447-5

RESEARCH ARTICLE

Enhanced CuCl dispersion by regulating acidity of MCM-41 for catalytic oxycarbonylation of ethanol to diethyl carbonate

Pengzhen CHEN,Shouying HUANG,Jijie ZHANG,Shengping WANG,Xinbin MA(

)

Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

Download: PDF(898 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Abstract

CuCl supported on molecular sieves has attracted increasing attention in catalyzing oxidative carbonylation of ethanol to diethyl carbonate. Mesoporous MCM-41 has been widely used as catalyst support due to its large surface area and well defined mesoporous structure. Considering its intrinsic weak acidity, MCM-41 was modified by a simple impregnation method to incorporate Al. The incorporation of Al components resulted in the high dispersion of Cu species and the increase of acid sites without changing the mesoporous structure of MCM-41, and thus enhanceed the catalytic activity of CuCl/MCM-41for diethyl carbonate synthesis.

Keywords MCM-41 acidity oxidative carbonylation diethyl carbonate

Corresponding Author(s): Xinbin MA

Online First Date: 17 November 2014 Issue Date: 14 July 2015

Cite this article:

Jijie ZHANG,Pengzhen CHEN,Shouying HUANG, et al. Enhanced CuCl dispersion by regulating acidity of MCM-41 for catalytic oxycarbonylation of ethanol to diethyl carbonate[J]. Front. Chem. Sci. Eng., 2015, 9(2): 224-231.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-014-1447-5
https://academic.hep.com.cn/fcse/EN/Y2015/V9/I2/224

Fig.1 Small-angle XRD patterns of (a) MCM-41, (b) AM-2.5, (c) AM-5, and (d) AM-7.5

Fig.2 Wide-angle XRD patterns of (a) MCM-41, (b) AM-2.5, (c) AM-5, and (d) AM-7.5

Fig.3 N₂ adsorption-desorption isotherms and pore size distributions of (a) MCM-41, (b) AM-2.5, (c) AM-5, and (d) AM-7.5

Tab.1 Textural properties of MCM-41 and AM-x samples.

Fig.4 IR spectra of pyridine adsorbed on (a) MCM-41, (b) AM-2.5, (c) AM-5, and (d) AM-7.5

Tab.2 Influence of Al modification on Br?nsted acid sites of MCM-41 and catalytic performance of CuCl/AM-x samples

Fig.5 ²⁷Al NMR spectra of (a) AM-2.5, (b) AM-5, and (c) AM-7.5

Fig.6 XRD patterns of CuCl dispersed on (a) MCM-41, (b) AM-2.5, (c) AM-5, and (d) AM-7.5

Fig.7 TEM images of CuCl dispersed on (a) MCM-41, (b) AM-2.5, (c) AM-5, and (d) AM-7.5

Fig.8 UV-vis DRS spectra of CuCl dispersed on (a) MCM-41, (b) AM-2.5, (c) AM-5, and (d) AM-7.5

1	Huang S, Chen P, Yan B, Wang S, Shen Y, Ma X. Modification of Y zeolite with alkaline treatment: Textural properties and catalytic activity for diethyl carbonate synthesis. Industrial & Engineering Chemistry Research, 2013, 52(19): 6349–6356
2	Tundo P, Selva M. The chemistry of dimethyl carbonate. Accounts of Chemical Research, 2002, 35(9): 706–716
3	Angela D, Michele A, Antonella A, Jayashree E, Brunella M A. Synthesis, characterization, and use of NbV/CeIV-mixed oxides in the direct carboxylation of ethanol by using pervaporation membranes for water removal. Chemistry (Weinheim an der Bergstrasse, Germany), 2012, 18(33): 10324–10334
4	Leino E, M?ki-Arvela P, Eta V, Murzin D Y, Salmi T, Mikkola J P. Conventional synthesis methods of short-chain dialkylcarbonates and novel production technology via direct route from alcohol and waste CO2. Applied Catalysis A, General, 2010, 383(1–2): 1–13
5	Zhang P, Huang S, Yang Y, Meng Q, Wang S, Ma X. Effect of SSIE structure of Cu-exchanged β and Y on the selectivity for synthesis of diethyl carbonate by oxidative carbonylation of ethanol: A comparative investigation. Catalysis Today, 2010, 149(1–2): 202–206
6	King S T. Oxidative carbonylation of methanol to dimethyl carbonate by solid-state ion-exchanged CuY catalysts. Catalysis Today, 1997, 33(1–3): 173–182
7	Li Z, Xie K, Robert C T. Studies of the interaction between CuCl and HY zeolite for preparing heterogeneous CuI catalyst. Applied Catalysis A, General, 2001, 209(1–2): 107–115
8	Zhang Y, Briggs D N, Smit E D, Bell A T. 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. Journal of Catalysis, 2007, 251(2): 443–452
9	Huang S, Wang Y, Wang Z, Yan B, Wang S, Gong J, Ma X. Cu-doped zeolites for catalytic oxidative carbonylation: The role of Br?nsted acids. Applied Catalysis A, General, 2012, 417–418: 236–242
10	Cao W, Zhang H, Yuan Y. CuCl2 immobilized on amino-functionalized MCM-41 and MCM-48 as efficient heterogeneous catalysts for dimethyl carbonate synthesis by vapor-phase oxidative carbonylation of methanol. Catalysis Letters, 2003, 91(3–4): 243–246
11	Li Z, Xie K, Robert C T. High selective catalyst CuCl/MCM-41 for oxidative carbonylation of methanol to dimethyl carbonate. Applied Catalysis A, General, 2001, 205(1–2): 85–92
12	Zhang P, Wang S, Chen S, Zhang Z, Ma X. The effects of promoters over PdCl2-CuCl2/HMS catalysts for the synthesis of diethyl carbonate by oxidative carbonylation of ethanol. Chemical Engineering Journal, 2008, 143(1–3): 220–224
13	Yang P, Cao Y, Hu J, Dai W, Fan K. Mesoporous bimetallic PdCl2-CuCl2 catalysts for dimethyl carbonate synthesis by vapor phase oxidative carbonylation of methanol. Applied Catalysis A, General, 2003, 241(1–2): 363–373
14	Du J, Xu H, Shen J, Huang J, Shen W, Zhao D. Catalytic dehydrogenation and cracking of industrial dipentene over M/SBA-15 (M= Al, Zn) catalysts. Applied Catalysis A, General, 2005, 296(2): 186–193
15	Zou J, Xu Y, Zhang X, Wang L. Isomerization of endo-dicyclopentadiene using Al-grafted MCM-41. Applied Catalysis A, General, 2012, 421–422: 79–85
16	Ryoo R, Jun S, Kim J M, Kim M J. Generalised route to the preparation of mesoporous metallosilicates via post-synthetic metal implantation. Chemical Communications, 1997, 22(22): 2225–2226
17	Ma J, Qiang L, Wang J, Tang X, Tang D. Effect of different synthesis methods on the structural and catalytic performance of SBA-15 modified by aluminum. Journal of Porous Materials, 2010, 18(5): 607–614
18	Baca M, Rochefoucauld E, Ambroise E, Krafft J M, Hajjar R, Man P P, Carrier X, Blanchard J. Characterization of mesoporous alumina prepared by surface alumination of SBA-15. Microporous and Mesoporous Materials, 2008, 110(2–3): 232–241
19	Cheralathan K K, Hayashib T, Ogura M. Post-synthesis coating of alumina on the mesopore walls of SBA-15 by ammonia/water vapour induced internal hydrolysis and its consequences on pore structure and acidity. Microporous and Mesoporous Materials, 2008, 116(1–3): 406–415
20	Luan Z, Hartmann M, Zhao D, Zhou W, Kevan L. Alumination and ion exchange of mesoporous SBA-15 molecular sieves. Chemistry of Materials, 1999, 11(6): 1621–1627
21	Spoto G, Bordiga S, Scarano D, Zecchina A. Well defined CuI(NO), CuI(NO)2 and CuII(NO)X (X= O- and/or NO2-) complexes in CuI-ZSMS prepared by interaction of H-ZSM5 with gaseous CuCl. Catalysis Letters, 1992, 13(1–2): 39–44
22	Lamberti C, Spoto G, Scarano D, Pazé C, Salvalaggio M, Bordiga S, Zecchina A, Palomino G T, D’Acapito F. CuI-Y and CuII-Y zeolites: A XANES, EXAFS and visible-NIR study. Chemical Physics Letters, 1997, 269(5–6): 500–508
23	Zhang G, Long J, Wang X, Zhang Z, Dai W, Liu P, Li Z, Wu L, Fu X. Catalytic role of Cu sites of Cu/MCM-41 in phenol hydroxylation. Langmuir, 2010, 26(2): 1362–1371
24	Karthik M, Lin L, Bai H. Bifunctional mesoporous Cu-Al-MCM-41 materials for the simultaneous catalytic abatement of NOx and VOCs. Microporous and Mesoporous Materials, 2009, 117(1–2): 153–160

[1]	Shengping WANG, Changqing MA, Yun SHI, Xinbin MA. Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis[J]. Front Chem Sci Eng, 2014, 8(1): 95-103.
[2]	ZHU Xinli, YU Kailu, CHENG Dangguo, XIA Qing, LIU Changjun, ZHANG Yueping. Modification of acidity of Mo-Fe/HZSM-5 zeolite via argon plasma treatment[J]. Front. Chem. Sci. Eng., 2008, 2(1): 55-58.

Viewed

Full text

Abstract

Cited

Shared

Discussed