One-Step Synthesized SO₄^2–/ZrO₂-HZSM-5 Solid Acid Catalyst for Carbamate Decomposition in CO₂ Capture

Abstract

Amine-based CO₂ capture technology requires high-energy consumption because the desorption temperature required for carbamate breakdown during absorbent regeneration is higher than 110 °C. In this study, we report a stable solid acid catalyst, namely, SO₄^2-/ZrO₂-HZSM-5 (SZ@H), which has improved Lewis acid sites (LASs) and Bronsted acid sites (BASs). The improved LASs and BASs enabled the CO₂ desorption temperature to be decreased to less than 98 °C. The BASs and LASs of SZ@H preferred to donate or accept protons; thus, the amount and rate of CO₂ desorption from spent monoethanolamine were more than 40 and 37% higher, respectively, when using SZ@H than when not using any catalyst. Consequently, the energy consumption was reduced by approximately 31%. A catalyzed proton-transfer mechanism is proposed for SZ@H-catalyzed CO₂ regeneration through experimental characterization and theoretical calculations. The results reveal the role of proton transfer during CO₂ desorption, which enables the feasibility of catalysts for CO₂ capture in industrial applications.