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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

    Abdulrahman Mubarak Alsaiari
    Seba Alareeqi
    Vijay V. Kumar

    Related Publications

    Structural Modulation of Ni-Zn Intermetallic/Carbide Catalysts using Forced Dynamic CO₂ and CH₄ Reforming Conditions

    by Bai, Mohamed, Dally, Velisoju, Davaasuren, Meijerink, Hedhili, Castaño
    ACS Catal. Year: 2026 DOI: https://doi.org/10.1021/acscatal.5c07375

    Abstract

    Alloys and intermetallics have been repeatedly reported to improve the catalytic activity or stability. However, many alloys are structurally unstable under reaction conditions. Here, we systematically investigate methods to understand, control, and modulate these dynamics for NiZn catalysts during dry (CO2) reforming of methane (CH4). Initially, we modulate the Ni-rich NiZn alloy and NiZn intermetallic by varying the Ni/Zn ratio, NiZn loading, and reduction temperature. Then, we study the structural modulation of the NiZn alloys and intermetallic compounds in steady and forced dynamic conditions in a packed bed reactor, operando DRIFTS-MS, in situ XRD, and in situ TEM, revealing that the NiZn intermetallic phase dynamically transforms into a stable Ni3ZnC0.7 phase, which acts as a carbon reservoir, mitigating coke accumulation and maintaining stable performance for 50 h under realistic reforming conditions. In contrast, the Ni-rich NiZn alloy irreversibly segregates to Ni and ZnO instead of forming Ni3ZnC0.7, resulting in severe coke deposition. These insights into the NiZn phase dynamics open avenues for rational catalyst control through phase modulation.

    Keywords

    CHA CRE