​​

Stable catalyst design for the activation of methane to syngas, hydrogen, and chemicals


    Problem Statement

    Methane and light alkanes are species with relatively poor economic interest. Our goal is to activate C–H σ-bond to produce hydrogen, olefins, carbon monoxide, and carbon nanofibers, following different process strategies such as oxidative coupling (for olefins), CO2 dry reforming (for syngas), cracking or catalytic decomposition (for hydrogen-free of COx and sequestrated carbon nanotubes/nanofibers), cracking/co-cracking with CO or methanol. We work on developing, synthesizing, characterizing, and testing innovative catalysts with a twist of reaction engineering concepts, with a focus on multi-scale implications.

    We delve into the mechanistic insights into a series of in-house-synthesized metal-supported heterogeneous catalysts by combining them with dynamic reactors and ab initio calculations. We explore catalysts with extended lifetimes, enhanced activity, selectivity, and heat transfer. These catalysts are based on alloys-intermetallics, high entropy alloys, exsolved perovskites, and SiC, among others.

    We investigate novel reactor designs based on forced-dynamic, operando, and fluidized-bed reactors to amplify kinetic information and improve selectivity.

    CHA2023

    Goals

    • Develop a microkinetic-based modeling framework to analyze the catalyst performance
    • Scale the technical catalyst for its application in demanding exothermic (oxidative coupling of methane using SiC and spray drying) or fluidized-bed (catalytic decomposition of methane) conditions
    • Develop new catalytic concepts based on Ni-alloys (Ni-Fe, -Co, -Zn…)
    • Improve the catalyst structure-function correlations using in-situ, operando, and dynamic techniques and reactors

    Related People

    Related Publications

    Kinetics and Reactor Modeling of the Conversion of n-Pentane using HZSM-5 catalysts with Different Si/Al ratio

    by Cordero-Lanzac, Aguayo, Castaño, Bilbao
    React. Chem. Eng. Year: 2019

    Abstract

    The production of olefins and aromatics from n-pentane has been modeled using the experimental results collected in an isothermal packed bed reactor with HZSM-5 zeolite catalysts with different Si/Al ratios (15 and 140) in the temperature range of 400–550 °C. In the first stage, a lump-based kinetic model has been established, evaluating the role of the Si/Al ratio in the kinetic parameters and therefore, in the conversion, product distribution and deactivation by coke. The effect of the catalyst acidity and the reaction conditions has been explained by analyzing the used catalysts by means of N2 and tert-butylamine adsorption–desorption, temperature-programmed oxidation and confocal fluorescence microscopy. In the second stage, the kinetic parameters extracted for both catalysts have been used in simulations of an isothermal packed bed reactor in order to study the evolution of the reaction with the space time and time on stream. Certain suitable conditions (550 °C and 3.5 gcat h molC−1) for maximizing the yield and selectivity to olefins (31 and 51%, respectively, using the zeolite with Si/Al = 140) and aromatics (yield and selectivity of 53%, using the one with Si/Al = 15) in the simulated range were found.

    Keywords

    CHA MKM