Abstract

The capture and catalytic conversion of CO2 into value-added chemicals is a promising and sustainable approach to tackle the global warming and energy crisis. The nitrogen-rich porous organic polymers are excellent materials for CO2 capture and separation. Herein, we present a nitrogen-rich heptazine-based microporous polymer for the cycloaddition reaction of CO2 with epoxides in the absence of metals and solvents. HMP-TAPA, being rich in the nitrogen site, showed a high CO2 uptake of 106.7 mg/g with an IAST selectivity of 30.79 toward CO2 over N2. Furthermore, HMP-TAPA showed high chemical and water stability without loss of any structural integrity. Besides CO2 sorption, the catalytic activity of HMP-TAPA was checked for the cycloaddition of CO2 and terminal epoxides, resulting in cyclic carbonate with high conversion (98%). They showed remarkable recyclability up to 5 cycles without loss of activity. Overall, this study represents a rare demonstration of the rational design of POPs (HMP-TAPA) for multiple applications.

Highlights

  • Carbon dioxide (CO2) has attracted significant attention as a greenhouse gas which is considered to be a major contributor for global warming and subsequent climate changes. (Aresta et al, 2014; Pera-Titus, 2014; Mukherjee et al, 2019)

  • To construct a heptazine-based polymeric network, Trichloro heptazine (TCH) and Tris-(4-aminopenyl) amine were taken into an RB flask, which further underwent a substitution nucleophilic reaction in the presence of DIPEA for 72 h

  • The absorption band at 1641 cm−1 harmonized to the C N stretching vibration of the heptazine moiety, which could be further validated by vanishing of C-Cl stretching vibration at 942 cm−1 in HMP-Tris (4-amino phenyl) amine (TAPA) (Ma et al, 2016)

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Summary

Introduction

Carbon dioxide (CO2) has attracted significant attention as a greenhouse gas which is considered to be a major contributor for global warming and subsequent climate changes. (Aresta et al, 2014; Pera-Titus, 2014; Mukherjee et al, 2019). After probing the chemical structure of the framework, the porous nature of the catalyst was investigated by measuring N2 adsorption–desorption isotherms at 77 K (Figure 2A). The observed selectivity for HMP-TAPA is 26.27 and 30.97 at 273 and 298 K, respectively, which is the highest achieved value among the heptazine-based porous polymers reported so far (Dang et al, 2015).

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