The influence of zeolite morphology on the conversion of methane to methanol on copper- exchanged omega zeolite ( MAZ)

被引:26
作者
Knorpp, Amy J. [1 ]
Newton, Mark A. [1 ]
Sushkevich, Vitaly L. [2 ]
Zimmermann, Patrik P. [2 ]
Pinar, Ana B. [2 ]
van Bokhoven, Jeroen A. [1 ,2 ]
机构
[1] Swiss Fed Inst Technol, Inst Chem & Bioengn, Vladimir Prelog Weg 1, CH-8093 Zurich, Switzerland
[2] Paul Scherrer Inst, Lab Catalysis & Sustainable Chem, CH-5232 Villigen, Switzerland
关键词
ACTIVE-SITES; CATALYTIC CONVERSION; MORDENITE; OXIDATION; OXYGEN; ZSM-5; CHEMISTRY; CLUSTERS; MAZZITE; TEMPERATURE;
D O I
10.1039/c9cy00013e
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Methane is often flared due to the heavy economic burden of transportation, particularly at rural petroleum extraction sites. Directly converting methane to methanol is possible through a stepwise process with copper- exchanged zeolites. Factors affecting this conversion are not yet fully understood. Omega zeolite ( MAZ) can yield 197 mu mol per gram- zeolite, the highest reported thus far. Here we show that the synthesis and resulting morphology of the zeolite play an enormous role in the yield of methanol. High yields are only achieved when the zeolite has a longer stick- like bundled morphology ( 2- 4 mu m by 100 nm). When the zeolite forms small spherulitic aggregates, the methanol yield is severely diminished ( 60- 97 mu molmethanol per gram- zeolite). This difference originates from minute changes in the synthesis procedure, emphasizing the extreme sensitivity of zeolite properties towards synthesis conditions. This work shows that selecting a parent zeolite is crucial and is an opportunity for process optimization to achieve high and industrially- relevant methanol yields.
引用
收藏
页码:2806 / 2811
页数:6
相关论文
共 57 条
[1]   Catalytic conversion of methane to methanol over Cu-mordenite [J].
Alayon, Evalyn Mae ;
Nachtegaal, Maarten ;
Ranocchiari, Marco ;
van Bokhoven, Jeroen A. .
CHEMICAL COMMUNICATIONS, 2012, 48 (03) :404-406
[2]   Bis(μ-oxo) versus mono(μ-oxo)dicopper cores in a zeolite for converting methane to methanol: an in situ XAS and DFT investigation [J].
Alayon, Evalyn Mae C. ;
Nachtegaal, Maarten ;
Bodi, Andras ;
Ranocchiari, Marco ;
van Bokhoven, Jeroen A. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2015, 17 (12) :7681-7693
[3]   Mazzite-Na, a new zeolite from Boron, California: Its description and crystal structure [J].
Arletti, R ;
Galli, E ;
Vezzalini, G ;
Wise, WS .
AMERICAN MINERALOGIST, 2005, 90 (07) :1186-1191
[4]   Cu-ZSM-5 Zeolites for the Formation of Methanol from Methane and Oxygen: Probing the Active Sites and Spectator Species [J].
Beznis, Nadzeya V. ;
Weckhuysen, Bert M. ;
Bitter, Johannes H. .
CATALYSIS LETTERS, 2010, 138 (1-2) :14-22
[5]  
Borfecchia E., 2018, CATAL TODAY
[6]   FLARING IN ENERGY INDUSTRY [J].
BRZUSTOWSKI, TA .
PROGRESS IN ENERGY AND COMBUSTION SCIENCE, 1976, 2 (03) :129-141
[7]   Methane as raw material in synthetic chemistry: the final frontier [J].
Caballero, Ana ;
Perez, Pedro J. .
CHEMICAL SOCIETY REVIEWS, 2013, 42 (23) :8809-8820
[8]  
Cejka J., 2007, Introduction to Zeolite Molecular Sieves
[9]   SORPTION PROPERTIES OF ZEOLITE-OMEGA [J].
CHAUVIN, B ;
FAJULA, F ;
FIGUERAS, F ;
GUEGUEN, C ;
BOUSQUET, J .
JOURNAL OF CATALYSIS, 1988, 111 (01) :94-105
[10]  
CIRIC J, 1968, Patent No. 1117568