The effects of cell density and intrinsic porosity on structural properties and adsorption kinetics in 3D-printed zeolite monoliths

Lawson, Shane; Adebayo, Busuyi O.; Robinson, Chad T.; Al-Naddaf, Qasim; Rownaghi, Ali A.; Rezaei, Fateme

doi:10.1016/j.ces.2020.115564

Cited by 64 publications

(79 citation statements)

References 48 publications

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“…The surface topographies were rough and contained macropores of ≈5–10 µm in diameter, which were likely formed during methylcellulose removal (Figure S3b,c, Supporting Information). [ 30 ] It is also worth noting here that an even dispersion of crystalline phases was observed across the monolith surface. After imaging this phase at high magnification (Figure S3d, Supporting Information), the phase was found to be ≈5 um in diameter.…”

Section: Resultsmentioning

confidence: 79%

A Novel Method of 3D Printing High‐Loaded Oxide/H‐ZSM‐5 Catalyst Monoliths for Carbon Dioxide Reduction in Tandem with Propane Dehydrogenation

Lawson

Farsad

Adebayo

et al. 2020

Advanced Sustainable Systems

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Oxidative propane dehydrogenation using CO2 (CO2‐ODHP) is a potential alternative for propylene synthesis. In this study, bifunctional catalysts (V2O5, ZrO2, Cr2O3, and Ga2O3 doped H‐ZSM‐5) are synthesized through additive manufacturing for CO2‐ODHP. Characterization and correlation between the various characterizations and the catalytic results indicates that the direct 3D printing of metal oxides alongside H‐ZSM‐5 can considerably modify the surface properties and bulk oxide phase dispersion, thus leading to enhanced metal oxide reducibility and exceptional CO2‐ODHP performance. Among the metal monoliths, the mixed oxide sample with 5 wt% Cr, 10 wt% V, 10 wt% Zr, 10 wt% Ga and 65 wt% H‐ZSM‐5 displays the best activity, achieving ≈40% propane conversion, 95% propylene selectivity, and zero benzene/toluene/xylene production. Upon eliminating CO2, the catalyst monoliths all retain their long‐term stability; however, the propane conversions decrease by ≈3% and the propylene selectivities decreased by 5–15%. Nevertheless, all five samples examined here demonstrate exceptional catalytic activities and prolonged stabilities, which are attributed to the even distribution of surface acid sites produced by direct printing of the oxide and zeolite components. Overall, this study presents a novel way of manufacturing bifunctional structured catalysts that exhibit exceptional ODHP performance.

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Section: Resultsmentioning

confidence: 79%

A Novel Method of 3D Printing High‐Loaded Oxide/H‐ZSM‐5 Catalyst Monoliths for Carbon Dioxide Reduction in Tandem with Propane Dehydrogenation

Lawson

Farsad

Adebayo

et al. 2020

Advanced Sustainable Systems

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“…As such, when applying this approach to other zeolites, a good starting point for paste optimization would be to begin using only pectin, followed by incremental gelatin addition to minimize ink spreading. It is also worth noting here that, in our earlier techniques [1,[11][12][13][14][15][16], the paste formulation and densification processes took place over the course of 1-3 days, whereas this new technique yielded a printable paste in less than 5 min, meaning that this new method allows for much faster rheological optimization. Therefore, utilizing sacrificial biopolymers for zeolite gelation and 3D printing can be considered a superior technique from a rapid manufacturing perspective, as it dramatically reduced binding time from traditional paste formulation.…”

Section: Monolith Formulationmentioning

confidence: 86%

“…After producing the zeolite/biopolymer inks, the monoliths were 3Dprinted using our established setup [1,[11][12][13][14][15][16]. The zeolite 13X and 5A monoliths were printed using 0.84 mm (Nordson) tips, however, the ZSM-5 and South African monoliths were printed using 1.36 mm tips because those inks displayed denser rheologies and could not be extruded through the smaller bores.…”

Section: Monolith Formulationmentioning

confidence: 99%

“…An important alternative to traditional manufacturing, 3D printing technologywhich digitally tunes the scaffold geometry prior to its formulation with AutoCAD or some equivalenthas cemented itself as a facile way of producing ceramic contactors containing various supports, including metals/metal oxides, metal-organic frameworks (MOFs), and zeolites [1,[11][12][13][14][15][16][17][18]. In a pioneering work in 2016 [1], our group formulated zeolite 13X and 5A monoliths with 90 wt% loading by binding the commercial powders to bentonite clay through 3D printing technique.…”

Section: Introductionmentioning

confidence: 99%

“…These samples are noted as 13X 1% , 13X 2.5% , and 13X 5% , respectively. Here, it should be noted that we selected the monolithic geometry as to demonstrate this technique because of its relevance in industrial processes and because of its use in previous works for 3D printing [1,16,19]. CO 2 , CH 4 , and N 2 adsorption isotherms were collected at 25 • C from 0 to 1 bar for the calcinated monoliths and parent powders, to demonstrate any differences between adsorption capacities, where the CO 2 /CH 4 and CO 2 /N 2 selectivities were calculated by the previously-detailed ideal adsorption solution theory (IAST) method [28].…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Binderless zeolite monoliths production with sacrificial biopolymers

Lawson

Newport

Al-Naddaf

et al. 2021

Chemical Engineering Journal

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3D printing has emerged as an attractive way of formulating structured adsorbents, as it imparts lower manufacturing costs compared to hydraulic extrusion while also allowing for unprecedented geometric control. However, binderless structures have not been fabricated by 3D printing, as ink formulation has previously required clay binders which cannot be easily removed. In this study, we report the development of a facile approach to shape engineer binderless zeolites. 3D-printed inks comprised of 13X, 5A, ZSM-5, and experimental South African zeolites were prepared using gelatin and pectin as binding agents along with dropwise addition of various solvents. After printing, the dried monoliths were calcined to remove the biopolymers and form 100% pure zeolite structures. From N 2 physisorption and CO 2 adsorption measurements at 0 • C, all monoliths showed narrowing below 1 nm from their powders, which was attributed to pore malformation caused by intraparticle bridging during calcination. The various adsorption isotherms indicated that this narrowing led to varying degrees of enhanced adsorption capacities for all three gases, as the slightly smaller pores increased electrostatic binding between the sorbent walls and captured species. Analysis of CO 2 adsorption performance revealed comparable diffusivities and adsorption capacities to the commercial bead analogues, implying that biopolymer/ zeolite printing can produce contactors which are competitive to commercial benchmarks. The binderless monoliths also exhibited faster diffusivities compared to zeolite monoliths produced by conventional direct ink writingon account of an enhancement in macroporosityhighlighting that this new method enhances the kinetic properties of 3D-printed scaffolds. As such, the sacrificial biopolymer technique is an effective and versatile approach for 3D printing binderless zeolite structures.

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3D‐Printed Porous Organic Cages for Gas Filtration: Fabrication and Flow Simulations

Ling,

Agrawal,

et al. 2024

Adv Funct Materials

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Porous organic cages (POCs) are a class of emerging porous materials with high porosity and selectivity for gas adsorption and separation. As a representative of first‐generation POCs, the cage molecule CC3, has huge potential for separating noble gases and volatile organic compounds (VOCs). 3D printing CC3 using direct ink writing (DIW) offers significant advantages to build complex structures. Through rational design, formulations that are both printable and functional are achieved. Optimised formulations have the elasto‐visco‐plastic behavior required while retaining the functional properties of the cages. The characterization of printed parts evidence that the CC3 structure and adsorption capacity are well preserved. BET surface areas vary with CC3 concentration and can reach up to ≈249 m2 g−1 for 70 wt% CC3. However, high CC3 content leads to a decrease in shrinkage, higher porosity, and low compressive strength ≈0.7 MPa. Computational fluid dynamics (CFD) is used to investigate the gas flow behavior through grid‐type structures with tailored geometric parameters. The results reveal that changing the offset distance and porosity manipulates the flow path, velocity distribution, and pressure drop. This work provides a pathway to design and fabricate structures with multi‐scale porosity that can be widely used for other functional materials and applications.

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The effects of cell density and intrinsic porosity on structural properties and adsorption kinetics in 3D-printed zeolite monoliths

Cited by 64 publications

References 48 publications

A Novel Method of 3D Printing High‐Loaded Oxide/H‐ZSM‐5 Catalyst Monoliths for Carbon Dioxide Reduction in Tandem with Propane Dehydrogenation

A Novel Method of 3D Printing High‐Loaded Oxide/H‐ZSM‐5 Catalyst Monoliths for Carbon Dioxide Reduction in Tandem with Propane Dehydrogenation

Binderless zeolite monoliths production with sacrificial biopolymers

3D‐Printed Porous Organic Cages for Gas Filtration: Fabrication and Flow Simulations

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