ÔØ Å ÒÙ× Ö ÔØPartial oxidation of methane with nitrous oxide forms synthesis gas over cobalt exchanged ZSM-5 Please cite this article as: Naseer A. Khan, Eric M. Kennedy, Bogdan Z. Dlugogorski, Adesoji A. Adesina, Michael Stockenhuber, Partial oxidation of methane with nitrous oxide forms synthesis gas over cobalt exchanged ZSM-5, Catalysis Communications (2014), doi: 10.1016/j.catcom.2014 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.
A C C E P T E D M A N U S C R I P T ACCEPTED MANUSCRIPTPartial oxidation of methane with nitrous oxide forms synthesis gas over cobalt exchanged ZSM-5. support are proposed as the active sites for H 2 (synthesis gas) formation.
IntroductionIndustrial activities have increased N 2 O (greenhouse gas) emissions significantly [1][2][3][4]. N 2 O gas has negative impact on the stratospheric ozone layer and has been identified in the Kyoto protocol as a target molecule for greenhouse gas (GHG) emission reduction [5,6]. Projects for N 2 O mitigation can effectively reduce emissions from stationary sources (nitric and adipic acid plants) [7]. The catalytic partial oxidation of CH 4 was first reported in 1929 [11], with continuing interest from industry and academia in its development and commercial deployment [12]. Ideally, the catalytic partial oxidation of CH 4 is described by reaction; CH 4 + ½O 2 CO + 2H 2 . However, the reaction mechanism is very complex and has been studied extensively using various transition and noble metal catalysts with different supports [13]. Thermodynamically, the higher selectivity of synthesis gas (produced from CH 4 partial oxidation) is favoured at higher temperatures (>1000 °C) [14]. The production of synthesis gas at relatively moderate temperatures was recently reported where the researchers used multiple catalysts with different metal promoters and cobalt loadings [13,15].In this paper, the catalytic partial oxidation of CH 4 to synthesis gas was investigated using N 2 O as oxidant. The dissociation of N 2 O during catalytic reaction is a complex process and is expected to influence the partial oxidation mechanism of CH 4 [16,17]. We identified catalyst preparation . The process of cobalt loading (at pH of 8) was repeated 3 times (Co-ZSM-5 (S.P.) ).c) Incipient wetness impregnation was also used for loading cobalt onto a ZSM-5 support [20,19]. A mass of 2.50 g of cobalt (II) nitrate hexahydrate was dissolved in 1 ml of demineralized water.The cobalt solution was added drop wise to 9.5 g NH 4 -ZSM-5 in order to obtain a paste. The prepared catalyst is identified as Co-ZSM-5 (I.W.) .All catalysts were dried at 110 °C.
Catalytic measurements...