Next frontiers in cleaner synthesis: 3D printed graphene-supported CeZrLa mixed-oxide nanocatalyst for CO2 utilisation and direct propylene carbonate production. (20th March 2019)

• Record Type: Journal Article
• Authors: Middelkoop, Vesna; Slater, Thomas; Florea, Mihaela; Neațu, Florentina; Danaci, Simge; Onyenkeadi, Victor; Boonen, Katrien; Saha, Basudeb; Baragau, Ioan-Alexandru; Kellici, Suela
• Is Part Of: Journal of cleaner production. Volume 214(2019)
• Page Start: 606
• Page End: 614
• Publication Date: 2019-03-20
• Subjects: Ceria-lanthana-zirconia graphene oxide -- Nanocomposite catalyst -- Continuous hydrothermal flow synthesis -- Direct-write 3D printing -- Propylene carbonate -- CO2 utilisation -- Green synthesis; Factory and trade waste -- Management -- Periodicals; Manufactures -- Environmental aspects -- Periodicals; Déchets industriels -- Gestion -- Périodiques; Usines -- Aspect de l'environnement -- Périodiques; 628.5
• DOI: 10.1016/j.jclepro.2018.12.274
• Languages: English
• ISSNs: 0959-6526

Abstract

Abstract: A rapidly-growing 3D printing technology is innovatively employed for the manufacture of a new class of heterogenous catalysts for the conversion of CO2 into industrially relevant chemicals such as cyclic carbonates. For the first time, directly printed graphene-based 3D structured nanocatalysts have been developed combining the exceptional properties of graphene and active CeZrLa mixed-oxide nanoparticles. It constitutes a significant advance on previous attempts at 3D printing graphene inks in that it does not merely explore the printability itself, but enhances the efficiency of industrially relevant reactions, such as CO2 utilisation for direct propylene carbonate (PC) production in the absence of organic solvents. In comparison to the starting powder, 3D printed GO-supported CeZeLa catalysts showed improved activity with higher conversion and no noticeable change in selectivity. This can be attributed to the spatially uniform distribution of nanoparticles over the 2D and 3D surfaces, and the larger surface area and pore volume of the printed structures. 3D printed GO-supported CeZeLa catalysts compared to unsupported 3D printed samples exhibited higher selectivity and yield owing to the great number of new weak acid sites appearing in the supported sample, as observed by NH3-TPD analysis. In addition, the catalyst's facile separation from the product has the capacity to massively reduce materials and operating costs resulting in increased sustainability. It convincingly shows the potential of these printing technologies in revolutionising the way catalysts and catalytic reactors are designed in the general quest for clean technologies and greener chemistry. Graphical abstract: Highlights: Studies of 3D printed Ce-La-Zr GO catalyst performance in CO2 utilisation reaction. Highly active Ce-La-Zr graphene oxide nanocomposite catalyst synthesised using CHFS. CHFS-continuous hydrothermal flow synthesis: controlled, rapid and efficient route. Direct synthesis of propylene carbonate in the absence of organic solvents. Improved catalytic activity of well-controlled 3D printed Ce-La-Zr-GO catalysts.