title: Reinventing Design Principles for Developing Low-Viscosity Carbon Dioxide-Binding Organic Liquids for Flue Gas Clean Up.
abstract: Anthropogenic CO2emissions from point sources (e.g., coal fired-power plants) account for the majority of the greenhouse gases in the atmosphere. Water-lean solvent systems such as CO2-binding organic liquids (CO2BOLs) are being developed to reduce the energy requirement for CO2capture. Many water-lean solvents such as CO2BOLs are currently limited by the high viscosities of concentrated electrolyte solvents, thus many of these solvents have yet to move toward commercialization. Conventional standard trial-and-error approaches for viscosity reduction, while effective, are time consuming and economically expensive. We rethink the metrics and design principles of low-viscosity CO2-capture solvents using a combined synthesis and computational modeling approach. We critically study the effects of viscosity reducing factors such as orientation of hydrogen bonding, introduction of higher degrees of freedom, and cation or anion charge solvation, and assess whether or how each factor affects viscosity of CO2BOL CO2capture solvents. Ultimately, we found that hydrogen bond orientation and strength is the predominant factor influencing the viscosity in CO2BOL solvents. With this knowledge, a new CO2BOL variant, 1-MEIPADM-2-BOL, was synthesized and tested, resulting in a solvent that is approximately 60 % less viscous at 25 mol % CO2loading than our base compound 1-IPADM-2-BOL. The insights gained from the current study redefine the fundamental concepts and understanding of what influences viscosity in concentrated organic CO2-capture solvents.
authors.affiliation: Energy Processes and Materials Division, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
authors.forename: Deepika
authors.identifier: 0000-0002-0796-6508
authors.initials: D
authors.lastname: Malhotra
authors.affiliation: Energy Processes and Materials Division, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
authors.forename: Phillip K
authors.identifier: 0000-0003-2996-0593
authors.initials: PK
authors.lastname: Koech
authors.affiliation: Energy Processes and Materials Division, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
authors.forename: David J
authors.identifier: 0000-0002-5529-526X
authors.initials: DJ
authors.lastname: Heldebrant
authors.affiliation: Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
authors.forename: David C
authors.initials: DC
authors.lastname: Cantu
authors.affiliation: Energy Processes and Materials Division, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
authors.forename: Feng
authors.initials: F
authors.lastname: Zheng
authors.affiliation: Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
authors.forename: Vassiliki-Alexandra
authors.identifier: 0000-0001-6028-7021
authors.initials: VA
authors.lastname: Glezakou
authors.affiliation: Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
authors.forename: Roger
authors.initials: R
authors.lastname: Rousseau
mesh_terms: D002245:Carbon Dioxide / Q000737:chemistry* / Q000302:isolation & purification*; D007220:Industrial Waste; D009930:Organic Chemicals / Q000737:chemistry*; D012997:Solvents / Q000737:chemistry; D014783:Viscosity
chemical_list: D007220:Industrial Waste; D009930:Organic Chemicals; D012997:Solvents; D002245:Carbon Dioxide
keywords: carbon dioxide; hydrogen bonding; molecular design; organic liquids; viscosity