Efficient chemical fixation of CO2from direct air under environment-friendly co-catalyst and solvent-free ambient conditions
The capture and conversion of CO2from direct air into value-added products under mild conditions represents a promising step towards environmental remediation and energy sustainability. Consequently, herein, we report the first example of a Mg(ii)-based MOF exhibiting highly efficient fixation of CO2from direct air into value-added cyclic carbonates under eco-friendly co-catalyst and solvent-free mild conditions. The bifunctional MOF catalyst was rationally constructed by utilizing an eco-friendly Lewis acidic metal ion, Mg(ii), and a nitrogen-rich tripodal linker, TATAB. The MOF possesses a high BET surface area of 2606.13 m2g?1and highly polar 1D channels decorated with a high density of CO2-philic sites which promote a remarkably high CO2uptake of 50.2 wt% at 273 K with a high heat of adsorption value of 55.13 kJ mol?1. The high CO2-affinity combined with the presence of a high density of nucleophilic and Lewis acidic sites conferred efficient catalytic properties to the Mg-MOF for chemical fixation of CO2from direct air under environment-friendly mild conditions. The remarkable performance of the Mg-MOF for the fixation of CO2from direct air was further supported by in-depth theoretical calculations. Moreover, the computational studies provided an insight into the mechanistic details of the catalytic process in the absence of any co-catalyst and solvent. Overall, this work represents a rare demonstration of carbon capture and utilization (CCU) from direct air under eco-friendly mild conditions. The Royal Society of Chemistry 2021.
Das R.; Ezhil T.; Palakkal A.S.; Muthukumar D.; Pillai R.S.; Nagaraja C.M.
Journal of Materials Chemistry A, Vol-9, No. 40, pp. 23127-23139.
https://doi.org/10.1039/d1ta05138e https://www.scopus.com/inward/record.uri?eid=2-s2.0-85117506707&doi=10.1039%2fd1ta05138e&partnerID=40&md5=2852ca4d73d04a577a594ac9d5c4b7f8
Das R., Department of Chemistry, Indian Institute of Technology Ropar, Rupnagar, 140001, Punjab, India; Ezhil T., Department of Chemistry, Indian Institute of Technology Ropar, Rupnagar, 140001, Punjab, India; Palakkal A.S., Department of Chemistry, Faculty of Engineering and Technology, SRM Institute of Science and Technology, Kattankulathur, Chennai, 603203, Tamil Nadu, India; Muthukumar D., Department of Chemistry, Faculty of Engineering and Technology, SRM Institute of Science and Technology, Kattankulathur, Chennai, 603203, Tamil Nadu, India; Pillai R.S., Department of Chemistry, Faculty of Engineering and Technology, SRM Institute of Science and Technology, Kattankulathur, Chennai, 603203, Tamil Nadu, India, Department of Chemistry, Christ University, Bangalore, 560023, Karnataka, India; Nagaraja C.M., Department of Chemistry, Indian Institute of Technology Ropar, Rupnagar, 140001, Punjab, India