Reaction of nitrous oxide with methane to synthesis gas:A thermodynamic and catalytic study

作     者：Naseer A.Khan Eric M.Kennedy Bogdan Z.Dlugogorski Adesoji A.Adesina Michael Stockenhuber 

作者机构：Priority Research Centre for Energy(PRCfE)The University of NewcastleCallaghanNSW 2308Australia Department of Chemical EngineeringUETPeshawarKPKPakistan School of Engineering and Information TechnologyMurdoch UniversityMurdochWA 6150Australia ATODATECH LLCBrentwoodCA 94513USA 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2017年第26卷第1期

页      面：155-162页

核心收录：

学科分类：0820[工学-石油与天然气工程] 081702[工学-化学工艺] 0808[工学-电气工程] 0817[工学-化学工程与技术] 08[工学] 0807[工学-动力工程及工程热物理] 0827[工学-核科学与技术] 0703[理学-化学] 

主　　题：Gibbs free energy minimization N2O CH4 Synthesis gas 

摘      要：The aim of the present study is to explore the coherence of thermodynamic equilibrium predictions with the actual catalytic reaction of CH4 with N2O,particularly at higher CH4 *** this purpose,key process variables,such as temperature(300℃-550℃) and a molar feed ratio(N2O/CH4 = 1,3,and 5),were altered to establish the conditions for maximized *** experimental study was conducted over the Co-ZSM-5 catalyst in a fixed bed tubular reactor and then compared with the thermodynamic equilibrium compositions,where the equilibrium composition was calculated via total Gibbs free energy minimization *** results suggest that molar feed ratio plays an important role in the overall reaction products *** for N2O conversions,and irrespective of N2O/CH4feed ratio,the thermodynamic predictions coincide with experimental data obtained at approximately 475℃-550℃,indicating that the reactions are kinetically limited at lower range of *** example,theoretical calculations show that the H2 yield is zero in presence of excess N2O(N2O/CH4= 5).However over a Co-ZSM-5 catalyst,and with a same molar feed ratio(N2O/CH4) of 5,the H2yield is initially 10%at 425℃,while above450℃ it drops to ***,H2yield steadily increases with temperature and with the level of CH4 conversion for reactions limited by N2O concentration in a reactant *** maximum attainable(from thermodynamic calculations and at a feed ratio of N2O/CH4=3) H2yield at 550℃ is 38%,whereas at same temperature and over Co-ZSM-5,the experimentally observed yield is about 19%.Carbon deposition on Co-ZSM-5 at lower temperatures and CH4 conversion(less than 50%) was also *** higher temperatures and levels of CH4conversion(above 90%),the deposited carbon is suggested to react with N2O to form CO2.