Formulation and Processing of Dual Functional Adsorbent/Catalyst Structured Monoliths using an Additively Manufactured Contactor for Direct Capture/Conversion of CO2 with Cogeneration of Ethylene

Author

Shane Lawson
Khaled Baamran
Kyle Newport
Fateme Rezaei, Missouri University of Science and TechnologyFollow
Ali A. Rownaghi, Missouri University of Science and TechnologyFollow

Abstract

Utilizing CO₂ as a mild oxidant for oxidative dehydrogenation of ethane (ODHE) is an attractive way of recycling this greenhouse contaminant. Typically, CO₂ capture and conversion processes are performed in separate beds, however, combining these processes into one bed incurs advantages of lower thermal gradient and reduced energy costs. This study formulated the first generation of structured dual-functional materials (DFMs) by directly 3D printing metal-oxide-CaO/ZSM-5 inks into monolithic contactors. Specifically, we 3D-printed monoliths with V, Ga, Ni, or Ti dopants to perform metal screening and determine which metal generates the best structured DFM for combined CO₂ capture and utilization in ODHE. The samples were vigorously characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), N₂ physisorption, NH₃-temperature programmed desorption (NH₃-TPD), H₂-temperature programmed reduction (H₂-TPR), energy dispersive spectroscopy (EDS), and Pyridine Fourier Transform Infrared Spectroscopy (Py-FTIR). Their CO₂ capture/ODHE performances were assessed with CO₂ adsorption at 600 °C and ODHE of 25 mL/min 7% C₂H₆ at 700 °C. The combined adsorption/catalysis experiments indicated that the best performance was observed in V-CaO/ZSM-5 which achieved a staggeringly high CO₂ capture (5.4 mmol/g), 65.2% CO₂ conversion, 36.5% C2H6 conversion, 98% C₂H₄ selectivity, and 35.8% C₂H₄ yield as well as zero thermal cracking after 40 min-on-stream. This performance exceeded that of any previously reported material for combined CO₂ capture and ODHE utilization, indicating this novel printing method can generate DFMs with exceptional potential for combined CO₂ capture and utilization processes.

Recommended Citation

S. Lawson et al., "Formulation and Processing of Dual Functional Adsorbent/Catalyst Structured Monoliths using an Additively Manufactured Contactor for Direct Capture/Conversion of CO2 with Cogeneration of Ethylene," Chemical Engineering Journal, vol. 431, article no. 133224, Elsevier, Mar 2022.

The definitive version is available at https://doi.org/10.1016/j.cej.2021.133224

Department(s)

Chemical and Biochemical Engineering

Comments

National Science Foundation, Grant CBET-1802049

Keywords and Phrases

Additive manufacturing; Combined CO Capture/Conversion 2; Dual functional adsorbent/Catalyst Monoliths; Ethylene production

International Standard Serial Number (ISSN)

1385-8947

Document Type

Article - Journal

Document Version

Final Version

File Type

text

Language(s)

English

Rights

© 2023 Elsevier, All rights reserved.

Publication Date

01 Mar 2022