The utilization of CO2 for the synthesis of value-added chemicals can help to reduce its concentration in the atmosphere [1]. The synthesis of 2-imidazolidinone using a nontoxic CO2 as carbonyl source has drawn greater attention as CO2 is abundant, which can be used as C1 feedstock for chemical synthesis [2]. In this study, a ZnO-supported hydroxyapatite (HAP) catalyst was designed based on the active sites required for this reaction. The Zn-HAP catalyst was synthesized by the one-step hydrothermal method. This supported catalyst showed better activity than support HAP and unsupported ZnO. Higher yield could be achieved by tuning the acid-base sites by varying the ZnO loading and calcination temperature. The catalyst was characterized using different techniques such as XRD, N2 -sorption, SEM-EDS, TEM, XPS, CO2 and NH3-TPD to understand its structural and textural properties. It was found that the acidic and basic properties of the catalysts played vital roles in achieving better catalytic activity. The XPS analysis showed a decrease in the intensity of Ca 2p peaks of Zn-HAP as compared with HAP, indicating the replacement of Ca2+ by Zn2+ in the structure which results in generation of new active sites, leading to an enhanced catalytic activity. Design of experiment (DOE) was employed using response surface methodology (Central Composite Design) to optimize reaction conditions. The optimized catalyst was shown to be stable and reusable by achieving 81% of conversion for ethylene diamine and 97% selectivity for 2-imidazolidinone under moderate pressure and temperature in 10 hours. The catalyst also showed good versatility by giving good yield for the reaction between different types of amines and CO2. The activity of the catalyst correlated well with its physicochemical properties.
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Enhancing activity of HAP catalyst by hydrothermal in situ Zn incorporation for transformation of CO2 to produce cyclic urea from diamine
Published:
21 April 2025
by MDPI
in The 3rd International Electronic Conference on Catalysis Sciences
session Environmental Catalysis
Abstract:
Keywords: CO2; ethylenediamine;2-Imidazolidinone;cyclic urea;bifunctional catalyst
