Integrated Capture and Conversion of CO 2 to Methanol in a Post‐Combustion Capture Solvent: Heterogeneous Catalysts for Selective CN Bond Cleavage

Kothandaraman, Jotheeswari; Lopez, Johnny Saavedra; Jiang, Yuan; Walter, Eric D.; Burton, Sarah D.; Dagle, Robert A.; Heldebrant, David J.

doi:10.1002/aenm.202202369

Integrated Capture and Conversion of CO ₂ to Methanol in a Post‐Combustion Capture Solvent: Heterogeneous Catalysts for Selective CN Bond Cleavage

Journal Article · Mon Oct 03 00:00:00 EDT 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202202369· OSTI ID:1890750

Kothandaraman, Jotheeswari ^[1]; Lopez, Johnny Saavedra ^[1]; Jiang, Yuan ^[1]; Walter, Eric D. ^[2]; Burton, Sarah D. ^[2]; Dagle, Robert A. ^[1]; ^[3]

Pacific Northwest National Laboratory Advanced Energy Systems 902 Battelle Blvd Richland WA 99352 USA
Pacific Northwest National Laboratory Institute for Integrated Catalysis 902 Battelle Blvd Richland WA 99352 USA
Pacific Northwest National Laboratory 902 Battelle Blvd Richland WA 99352 USA, Washington State University Pullman WA 99163 USA

Abstract

An efficient and selective heterogeneous catalyst is identified for the condensed‐phase hydrogenation of captured CO ₂ in the presence of an advanced water‐lean post‐combustion capture solvent, ( N ‐(2‐EthoxyEthyl)‐3‐MorpholinoPropan‐1‐Amine), 2‐EEMPA. The catalysts commonly used for gas‐phase CO ₂ hydrogenation (e.g., Cu/Zn/Al ₂ O ₃ ) cause deactivation of amine promoters via N ‐methylation by CO cleavage of formamide intermediates. A heterogeneous catalyst system that suppresses N ‐methylation of amine solvents is identified, demonstrating how Pt, supported by reducible metal oxides CeO ₂ or TiO ₂ , can be selective for CN cleavage to produce methanol. This is the first known demonstration of integrated low‐temperature thermocatalytic capture and conversion of CO ₂ to methanol in an economically viable CO ₂ capture solvent. Technoeconomic analyses performed on the state‐of‐technology suggest that methanol can be produced with a minimum selling price of $4.4/gallon ($1,460/metric ton) when using CO ₂ captured from a 650 MW natural gas combined cycle plant. Ultimately, a road map of how realistic and achievable improvements to space velocity and methanol selectivity of this integrated process can enable near cost parity to fossil‐derived methanol, with a selling price of ≈$1.4/gal ($470/metric ton), is presented.

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Sponsoring Organization:: USDOE

OSTI ID:: 1890750

Alternate ID(s):: OSTI ID: 1902482
OSTI ID: 2565401

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 46 Vol. 12; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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