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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

    Intrinsic microkinetic effects of spray-drying and SiC co-support on Mn–Na₂WO₄/SiO₂ catalysts used in oxidative coupling of methane

    by Lezcano, Kulkarni, Velisoju, Realpe, Castaño
    React. Chem. Eng. Year: 2025 DOI: https://doi.org/10.1039/D4RE00403E

    Abstract

    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.

    Keywords

    MKM HCE CHA