title: Incorporation of Alkylamine into Metal-Organic Frameworks through a Brønsted Acid-Base Reaction for CO2Capture.
abstract: The escalating atmospheric CO2concentration is one of the most urgent environmental concerns of our age. To effectively capture CO2, various materials have been studied. Among them, alkylamine-modified metal-organic frameworks (MOFs) are considered to be promising candidates. In most cases, alkylamine molecules are integrated into MOFs through the coordination bonds formed between open metal sites (OMSs) and amine groups. Thus, the alkylamine density, as well as the corresponding CO2uptake in MOFs, are severely restricted by the density of OMSs. To overcome this limit, other approaches to incorporating alkylamine into MOFs are highly desired. We have developed a new method based on Brønsted acid-base reaction to tether alkylamines into Cr-MIL-101-SO3H for CO2capture. A systematic optimization of the amine tethering process was also conducted to maximize the CO2uptake of the modified MOF. Under the optimal amine tethering condition, the obtained tris(2-aminoethyl)amine-functionalized Cr-MIL-101-SO3H (Cr-MIL-101-SO3H-TAEA) has a cyclic CO2uptake of 2.28 mmol g-1at 150 mbar and 40 °C, and 1.12 mmol g-1at 0.4 mbar and 20 °C. The low-cost starting materials and simple synthetic procedure for the preparation of Cr-MIL-101-SO3H-TAEA suggest that it has the potential for large-scale production and practical applications.
authors: Department of Chemistry, Texas A&M University, College Station, Texas, 77842-3012, United States.
authors: Hao
authors: H
authors: Li
authors: Department of Chemistry, Texas A&M University, College Station, Texas, 77842-3012, United States.
authors: Kecheng
authors: K
authors: Wang
authors: Department of Chemistry, Texas A&M University, College Station, Texas, 77842-3012, United States.
authors: Dawei
authors: D
authors: Feng
authors: Department of Chemistry, Texas A&M University, College Station, Texas, 77842-3012, United States.|Department of Materials Science and Engineering, Texas A&M University, College Station, Texas, 77843, United States.
authors: Ying-Pin
authors: YP
authors: Chen
authors: Profusa, Inc., 345 Allerton Ave. South, San Francisco, California, 94080, United States.
authors: Wolfgang
authors: W
authors: Verdegaal
authors: Department of Chemistry, Texas A&M University, College Station, Texas, 77842-3012, United States. zhou@chem.tamu.edu.|Department of Materials Science and Engineering, Texas A&M University, College Station, Texas, 77843, United States. zhou@chem.tamu.edu.
authors: Hong-Cai
authors: http://orcid.org/0000-0002-9029-3788
authors: HC
authors: Zhou
mesh_terms: D000143:Acids / Q000737:chemistry*; D000327:Adsorption; D000468:Alkalies / Q000737:chemistry*; D000588:Amines / Q000737:chemistry*; D002245:Carbon Dioxide / Q000737:chemistry*; D008670:Metals / Q000737:chemistry*; D009930:Organic Chemicals / Q000737:chemistry*; D017550:Spectroscopy, Fourier Transform Infrared; D013696:Temperature
chemical_list: D000143:Acids; D000468:Alkalies; D000588:Amines; D008670:Metals; D009930:Organic Chemicals; D002245:Carbon Dioxide
keywords: Brønsted acid-base reaction; amine tethering; carbon dioxide capture; metal-organic frameworks; systematic optimization