One-Pot Synthesis of Tetraethylenepentamine-Containing Municipal Solid Waste Incineration Bottom Ash-Based Geopolymer for CO2 Capture
摘要
Amine-modified geopolymer sorbents show promise for CO2 capture, but still face challenges such as limited adsorption sites and the requirement for strong alkaline activators. In this study, a novel one-pot synthesis approach is developed to prepare tetraethylenepentamine-containing geopolymer adsorbents (TEPA-GS) from municipal solid waste incineration bottom ash, granulated blast furnace slag and TEPA, using a relatively small amount of NaOH/Na2SiO3 solution. Notably, TEPA not only incorporates into the geopolymer matrix via Si-NH2 bonds to create basic sites for CO2 adsorption, but also served as alkali activator during geopolymerization, thereby reducing reliance on conventional strong alkalis. The CO2 adsorption capacity increased with TEPA content from 10 to 30%, reaching a maximum uptake of 1.82 mmol/g. This value exceeds with that of conventional geopolymers synthesized via strong alkali activation, and is comparable to those of several reported amine-modified geopolymer prepared through strong alkaline activation and complex multi-step synthetic routes. CO2-TPD analysis confirmed that the incorporation of TEPA leads to an amino-dominated adsorption mechanism, characterized by weak chemical adsorption that facilitates reversible CO2 capture while residual physical adsorption sites remain preserved in the system. The adsorption kinetic test revealed that the adsorption is controlled by both chemisorption and physisorption, with chemisorption being predominant. Cyclic adsorption–desorption tests demonstrated reasonable reproducibility, with a 17.6% capacity decrease after five cycles, with the second cycle exhibiting the greatest loss due to amine evaporation. This work provides a feasible one-pot synthetic approach for developing amine-modified geopolymer sorbents with reduced dependence on strong alkaline activators.