Park, Kyung Soo Kim, Jeong Hwa Park, So Hyun Moon, Dong Ju Roh, Hyun-Seog Chung, Chan-Hwa Um, Soong Ho Choi, Joon-Hwan Bae, Jong Wook 2024-01-20T02:32:06Z 2024-01-20T02:32:06Z 2022-01-25 2017-01 1381-1169 https://pubs.kist.re.kr/handle/201004/123231 Direct activation of CH4 to oxygenates and unsaturated light hydrocarbons was investigated using Fe modified ZSM-5 and Ferrierite (FER) for a partial oxidation of CH4 with N2O oxidant. The amount of active alpha-oxygen sites and number of Bronsted acid sites on the Fe-modified zeolites were well correlated with CH4 conversion rate and product distributions. The amount of alpha-oxygen sites was largely changed according to preparation method such as wet impregnation or ion-exchange of iron precursor and types of zeolites. A large number of Bronsted acid sites and alpha-oxygen sites on the Fe-modified FER revealed a higher oxygenate formation such as methanol and dimethyl ether (DME) with COx, and a larger number of strong acid sites on Fe-modified ZSM-5 was also responsible for a higher selectivity to light hydrocarbons by a successive dehydration of oxygenates formed. The different catalytic performances were verified through proper measurements of the amount and type of acidic sites as well as the alpha-oxygen sites measured by N2O pulse chemisorption. The Fe-modified FER prepared by impregnation method possessed a larger amount of alpha-oxygen sites due to abundant Bronsted acid sites, which was responsible for a higher rate of CH4 conversion to oxygenates with the help of N2O decomposition on the alpha-oxygen sites originated from iron oxide nanoparticles. (C) 2016 Elsevier B.V. All rights reserved. English ELSEVIER SCIENCE BV Direct activation of CH4 to oxygenates and unsaturated hydrocarbons using N2O on Fe-modified zeolites Article 10.1016/j.molcata.2016.11.008 1 JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, v.426, pp.130 - 140 JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL 426 130 140 N scie scopus 000391076300016 2-s2.0-85000501198 Chemistry, Physical Chemistry Article SELECTIVE CATALYTIC-REDUCTION NITROUS-OXIDE DECOMPOSITION DIMETHYL ETHER SYNTHESIS PARTIAL OXIDATION METHANE OXIDATION SURFACE OXYGEN IRON CO SITES NO alpha-Oxygen sites CH4 activation N2O oxidant Fe-modified zeolites Acid sites