Eugene J Kim1, Rebecca L Siegelman1,2, Henry Z H Jiang1, Alexander C Forse1,3,4, Jung-Hoon Lee5,6,7, Jeffrey D Martell1, Phillip J Milner1, Joseph M Falkowski8, Jeffrey B Neaton5,6,9, Jeffrey A Reimer2,3, Simon C Weston8, Jeffrey R Long10,2,3. 1. Department of Chemistry, University of California, Berkeley, CA 94720, USA. 2. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. 3. Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA 94720, USA. 4. Berkeley Energy and Climate Institute, University of California, Berkeley, CA 94720, USA. 5. Department of Physics, University of California, Berkeley, CA 94720, USA. 6. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. 7. Computational Science Research Center, Korea Institute of Science and Technology, Seoul 02792, Republic of Korea. 8. Corporate Strategic Research, ExxonMobil Research and Engineering Company, Annandale, NJ 08801, USA. 9. Kavli Energy Nanosciences Institute, University of California, Berkeley, CA 94720, USA. 10. Department of Chemistry, University of California, Berkeley, CA 94720, USA. jrlong@berkeley.edu.
Abstract
Natural gas has become the dominant source of electricity in the United States, and technologies capable of efficiently removing carbon dioxide (CO2) from the flue emissions of natural gas-fired power plants could reduce their carbon intensity. However, given the low partial pressure of CO2 in the flue stream, separation of CO2 is particularly challenging. Taking inspiration from the crystal structures of diamine-appended metal-organic frameworks exhibiting two-step cooperative CO2 adsorption, we report a family of robust tetraamine-functionalized frameworks that retain cooperativity, leading to the potential for exceptional efficiency in capturing CO2 under the extreme conditions relevant to natural gas flue emissions. The ordered, multimetal coordination of the tetraamines imparts the materials with extraordinary stability to adsorption-desorption cycling with simulated humid flue gas and enables regeneration using low-temperature steam in lieu of costly pressure or temperature swings.
Natural gas has become the dominant source of electricity in the United States, and technologies capable of efficiently removing carbon dioxide (n class="Chemical">CO2) from the flue emissions of natural gas-fired power plants could reduce their carbon intensity. However, given the low partial pressure of CO2 in the flue stream, separation of CO2 is particularly challenging. Taking inspiration from the crystal structures of diamine-appended metal-organic frameworks exhibiting two-step cooperative CO2 adsorption, we report a family of robust tetraamine-functionalized frameworks that retain cooperativity, leading to the potential for exceptional efficiency in capturing CO2 under the extreme conditions relevant to natural gas flue emissions. The ordered, multimetal coordination of the tetraamines imparts the materials with extraordinary stability to adsorption-desorption cycling with simulated humid flue gas and enables regeneration using low-temperature steam in lieu of costly pressure or temperature swings.
Authors: Wen Li; Sunho Choi; Jeffery H Drese; Marc Hornbostel; Gopala Krishnan; Peter M Eisenberger; Christopher W Jones Journal: ChemSusChem Date: 2010-08-23 Impact factor: 8.928
Authors: Rebecca L Siegelman; Phillip J Milner; Alexander C Forse; Jung-Hoon Lee; Kristen A Colwell; Jeffrey B Neaton; Jeffrey A Reimer; Simon C Weston; Jeffrey R Long Journal: J Am Chem Soc Date: 2019-08-08 Impact factor: 15.419
Authors: Rebecca L Siegelman; Phillip J Milner; Eugene J Kim; Simon C Weston; Jeffrey R Long Journal: Energy Environ Sci Date: 2019-05-08 Impact factor: 38.532
Authors: Phillip J Milner; Jeffrey D Martell; Rebecca L Siegelman; David Gygi; Simon C Weston; Jeffrey R Long Journal: Chem Sci Date: 2017-10-26 Impact factor: 9.825
Authors: Mohsen S Yeganeh; Arben Jusufi; Shane P Deighton; Matthew S Ide; Michael Siskin; Aditya Jaishankar; Charles Maldarelli; Pedro Bertolini; Bharath Natarajan; Jessica L Vreeland; Mark A King; Andrew R Konicek Journal: Sci Adv Date: 2022-02-09 Impact factor: 14.136