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

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.

Graphical abstract

Keywords

MCM-41 / acidity / oxidative carbonylation / diethyl carbonate

References

[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 Nb^V/Ce^IV-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, Mäki-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 Cu^I 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 Brønsted 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 Cu^I(NO), Cu^I(NO)₂ and Cu^II(NO)_X (X= O^- and/or NO2-) complexes in Cu^I-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. Cu^I-Y and Cu^II-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 NO_x and VOCs. Microporous and Mesoporous Materials, 2009, 117(1–2): 153–160

Acknowledgements

Financial support from the National Natural Science Foundation of China (Grant No. 21325626, 20936003, 20876112), Specialized Research Fund for the Doctoral Program of Higher Education (SRFDP) (No. 20090032110021) and the Program of Introducing Talents of Discipline to Universities (No. B06006) is gratefully acknowledged.

RIGHTS & PERMISSIONS

2014 Higher Education Press and Springer-Verlag Berlin Heidelberg