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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

    Structural Modulation of Ni-Zn Intermetallic/Carbide Catalysts using Forced Dynamic CO₂ and CH₄ Reforming Conditions
    ACS Catal. Year: 2026 DOI:https://doi.org/10.1021/acscatal.5c07375
    Authors: Bai, Mohamed, Dally, Velisoju, Davaasuren, Meijerink, Hedhili, Castaño
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    Intrinsic microkinetic effects of spray-drying and SiC co-support on Mn–Na₂WO₄/SiO₂ catalysts used in oxidative coupling of methane
    React. Chem. Eng. Year: 2025 DOI:https://doi.org/10.1039/D4RE00403E
    Authors: Lezcano, Kulkarni, Velisoju, Realpe, Castaño
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    Microkinetic Modeling to Decode Catalytic Reactions and Empower Catalytic Design
    ChemCatChem Year: 2024 DOI:https://doi.org/10.1002/cctc.202301720
    Authors: Kulkarni, Lezcano, Velisoju, Realpe, Castaño
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    Enlarging the Three-Phase Boundary to Raise CO2/CH4 Conversions on Exsolved Ni–Fe Alloy Perovskite Catalysts by Minimal Rh Doping
    ACS Catal. Year: 2024 DOI:https://doi.org/10.1021/acscatal.4c00151
    Authors: Yao, Bai, Davaasuren, Melinte, Morlanes, Cerrillo, Velisoju, Kolubah, Zheng, Han, Bakr, Gascon, Mohamed, Cheng, Castaño
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    Engineering the TiOx Overlayer on Ni Catalyst to Balance Conversion and Stability for Methane Dry-CO2 Reforming
    ACS Sustainable Chem. Eng. Year: 2024 DOI:https://doi.org/10.1021/acssuschemeng.3c07051
    Authors: Bai, Yao, Cheng, Mohamed, Telalovic, Melinte, Emwas, Gascon
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    Highly Efficient and Stable Methane Dry Reforming Enabled by a Single-Site Cationic Ni Catalyst
    J. Am. Chem. Soc. Year: 2023 DOI:https://doi.org/10.1021/jacs.3c04581
    Authors: Cheng, Yao, Ou, Hu, Zheng, Li, Morlanes, Cerrillo, Castaño, Gascon, Han
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    Robust data curation for improved kinetic modeling in oxidative coupling of methane using high-throughput reactors
    Chem. Eng. Sci. Year: 2024 DOI:https://doi.org/10.1016/j.ces.2023.119412
    Authors: Lezcano, Gobouri, Realpe, Kulkarni, Velisoju, Castaño
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    Overcoming the kinetic and deactivation limitations of Ni catalyst by alloying it with Zn for the dry reforming of methane
    J. CO2 Util. Year: 2023 DOI:https://doi.org/10.1016/j.jcou.2023.102573
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    Multi-technique operando methods and instruments for simultaneous assessment of thermal catalysis structure, performance, dynamics, and kinetics
    Chem Catal. Year: 2023 DOI:https://doi.org/10.1016/j.checat.2023.100666
    Authors: Velisoju, Kulkarni, Cui, Rabee, Paalanen, Rabeah, Maestri, Brückner, Ruiz-Martinez, Castaño
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    Post-Synthetic Surface Modification of Metal–Organic Frameworks and Their Potential Applications
    Small Methods Year: 2023 DOI:https://doi.org/10.1002/smtd.202201413
    Authors: Figueroa-Quintero, Villalgordo-Hernández, Delgado-Marín, Narciso, Velisoju, Castaño, Gascon, Ramos-Fernandez
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