喷雾干燥和SiC共负载对甲烷偶联Mn-Na2WO4 /SiO2催化剂的本征微动力学影响

IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Gontzal Lezcano, Shekhar R. Kulkarni, Vijay K. Velisoju, Natalia Realpe and Pedro Castaño
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引用次数: 0

摘要

本文建立了微动力学模型,评价了碳化硅(SiC)共载体和成型方法对甲烷氧化偶联Mn-Na2WO4 /SiO2催化剂的影响。该模型考虑了传质、催化和气相动力学,并使用三种Mn-Na2WO4催化剂的实验值(产物组成)进行训练,以便在保持热力学一致性的同时使用催化描述符计算动力学参数。催化剂分为浸渍法制备的sio2负载型催化剂和喷雾干燥法制备的βSiC和α + βSiC负载型催化剂。我们的分析表明,SiC的类型和制备方法如何影响其结构性质,并导致不同的CH3˙自由基氧化、HO2˙猝灭、C2H4氧化和COX转化途径,最终导致CH4转化和C2选择性。我们的方法有助于评估启动子和支持对个体和全球反应网络的影响。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Intrinsic microkinetic effects of spray-drying and SiC co-support on Mn–Na2WO4/SiO2 catalysts used in oxidative coupling of methane†

This paper presents a microkinetic model to evaluate the effects of a silicon carbide (SiC) co-support and the shaping method on Mn–Na2WO4/SiO2 catalysts used for the oxidative coupling of methane. The model considers mass transfer, catalytic, and gas-phase kinetics, and it is trained with experimental values (product composition) of three Mn–Na2WO4 catalysts for calculating the kinetic parameters using catalytic descriptors while maintaining thermodynamic consistency. The catalysts were an SiO2-supported catalyst prepared through impregnation and two SiO2–SiC-supported catalysts (with βSiC and α + βSiC) prepared via spray-drying. Our analysis shows how the type of SiC and preparation method affect the textural properties and result in distinct CH3˙ radical oxidation, HO2˙ quenching, C2H4 oxidation, and COX transformation pathways, eventually leading to CH4 conversion and C2 selectivity. Our approach facilitates the assessment of the effects of the promoter and support on individual and global reaction networks.

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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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