Inks For 3D Printing Research Articles

Chitosan-based electroconductive inks without chemical reaction for cost-effective and versatile 3D printing for electromagnetic interference (EMI) shielding and strain-sensing applications

The burgeoning interest in biopolymer 3D printing arises from its capacity to meticulously engineer tailored, intricate structures, driven by the intrinsic benefits of biopolymers—renewability, chemical functionality, and biosafety. Nevertheless, the accessibility of economical and versatile 3D-printable biopolymer-based inks remains highly constrained. This study introduces an electroconductive ink for direct-ink-writing (DIW) 3D printing, distinguished by its straightforward preparation and commendable printability and material properties. The ink relies on chitosan as a binder, carbon fibers (CF) a low-cost electroactive filler, and silk fibroin (SF) a structural stabilizer. Freeform 3D printing manifests designated patterns of electroconductive strips embedded in an elastomer, actualizing effective strain sensors. The ink's high printability is demonstrated by printing complex geometries with porous, hollow, and overhanging structures without chemical or photoinitiated reactions or support baths. The composite is lightweight (density 0.29 ± 0.01 g/cm3), electroconductive (2.64 ± 0.06 S/cm), and inexpensive (20 USD/kg), with tensile strength of 20.77 ± 0.60 MPa and Young's modulus of 3.92 ± 0.06 GPa. 3D-printed structures exhibited outstanding electromagnetic interference (EMI) shielding effectiveness of 30–31 dB, with shielding of >99.9 % incident electromagnetic waves, showcasing significant electronic application potential. Thus, this study presents a novel, easily prepared, and highly effective biopolymer-based ink poised to advance the landscape of 3D printing technologies.

3D printing of rice starch incorporated peanut protein isolate paste: Rheological characterization and simulation of flow properties

This study investigates the viscosity and creep behavior of peanut protein isolate (PPI) paste incorporated with rice starch (RS) for potential applications in 3D printing. The change in flow properties during the 3D printing was also studied by numerical simulation. The paste exhibited shear-thinning behavior with yield stress. The pressure predicted from the Herschel-Bulkley model showed higher values than those derived from the Power-Law model. The PPI and RS levels had negligible influence on velocity and shear rate; however, they showed greater dependence on the inflow rate. The fractional element model described the creep data well (R2 > 0.9). The addition of PPI resulted in increased viscosity, simulated pressure, and mean extrusion force, with similar effects observed for RS, except at higher PPI levels. Furthermore, the 3D-printed objects revealed that deformations were pronounced at low concentrations of PPI and RS, while resolution suffered when employing higher concentrations of PPI and RS. Industrial relevanceUsing peanut protein isolate, a plant-based high protein ingredient in 3D printing, reduces energy consumption, thereby reducing carbon footprints, offers improved functional properties, and diversifies dietary options by offering an alternative protein source from peanuts. The printing is influenced by the rheological properties of food ink. Thus, knowing the rheological properties of food ink can help researchers and industries to prepare food inks with desired properties. The observations of numerical simulation of this work have the potential to offer practical insights for designing 3D printing systems. In summary, this work has the potential to aid in improving and developing food ink for 3D printing, hence enhancing the performance of extrusion-based 3D food printers.

All‐Printed Electrically Driven Lighting via Electrochemiluminescence

AbstractElectrochemiluminescence (ECL) has attracted significant attention as a promising light‐emitting technology owing to its simple configuration and solution processability. ECL has wide applications in biological and chemical sensors, lighting, and displays. ECL lighting devices are fabricated as sandwiched structures with a transparent electrode on top, which limits their widespread adoption. Intricate structures with high precision and customizable designs can be directly fabricated using 3D printing. However, 3D printing of ECL devices is challenging because of poor printability and structural integrity of ECL luminophore inks. Here, all‐printed electrically driven lighting is demonstrated using the direct ink writing method. The ECL reactive layer and electrodes are directly printed using a side‐by‐side electrode configuration. A 3D printable ECL ink is developed by incorporating silica nanoparticles as rheological modifiers to realize well‐defined patterns with high structural integrity. Graphene is introduced on Ag multilayer electrodes to embrace both the electrical conductivity and electrochemical stability for efficient ECL operation. This all‐printing approach allows the fabrication of ECL devices with complex designs, such as combs and spirals. Moreover, it facilitates seamless printing on various substrate materials, making this technology an asset in the fields of biology, chemistry, and electronics.

Waterborne Polyurethane-Urea-Based Composite Inks for 3D Printing with Enhanced Properties

Waterborne Polyurethane-Urea-Based Composite Inks for 3D Printing with Enhanced Properties

SCOBY: an alternate solution to develop cheap and nutritious food by food layered manufacturing (FLM)

PurposeIn pursuit of affordable and nutrient-rich food alternatives, the symbiotic culture of bacteria and yeast (SCOBY) emerged as a selected food ink for 3D printing. The purpose of this paper is to harness SCOBY’s potential to create cost-effective and nourishing food options using the innovative technique of 3D printing.Design/methodology/approachThis work presents a comparative analysis of the printability of SCOBY with blends of wheat flour, with a focus on the optimization of process variables such as printing composition, nozzle height, nozzle diameter, printing speed, extrusion motor speed and extrusion rate. Extensive research was carried out to explore the diverse physical, mechanical and rheological properties of food ink.FindingsAmong the ratios tested, SCOBY, with SCOBY:wheat flour ratio at 1:0.33 exhibited the highest precision and layer definition when 3D printed at 50 and 60 mm/s printing speeds, 180 rpm motor speed and 0.8 mm nozzle with a 0.005 cm3/s extrusion rate, with minimum alteration in colour.Originality/valueFood layered manufacturing (FLM) is a novel concept that uses a specialized printer to fabricate edible objects by layering edible materials, such as chocolate, confectionaries and pureed fruits and vegetables. FLM is a disruptive technology that enables the creation of personalized and texture-tailored foods, incorporating desired nutritional values and food quality, using a variety of ingredients and additions. This research highlights the potential of SCOBY as a viable material for 3D food printing applications.

Evaluation of Various Types of Alginate Inks for Light-Mediated Extrusion 3D Printing.

Naturally derived biopolymers modifying or combining with other components are excellent candidates to promote the full potential of additive manufacturing in biomedicine, cosmetics, and the food industry. This work aims to develop new photo-cross-linkable alginate-based inks for extrusion 3D printing. Specifically, this work is focused on the effect of the addition of cross-linkers with different chemical structures (polyethylene glycol diacrylate (PEGDA), N,N'-methylenebisacrylamide (NMBA), and acrylic acid (AA)) in the potential printability and physical properties of methacrylated alginate (AlgMe) hydrogels. Although all inks showed maximum photo-curing conversions and gelation times less than 2 min, only those structures printed with the inks incorporating cross-linking agents with flexible and long chain structure (PEGDA and AA) displayed acceptable size accuracy (~0.4-0.5) and printing index (Pr ~1.00). The addition of these cross-linking agents leads to higher Young's moduli (from 1.6 to 2.0-2.6 KPa) in the hydrogels, and their different chemical structures results in variations in their mechanical and rheological properties. However, similar swelling ability (~15 swelling factor), degradability (~45 days 100% weight loss), and cytocompatibility (~100%) were assessed in all the systems, which is of great importance for the final applicability of these hydrogels.

3D printed polyvinylpyrrolidone–honey-gel with adhesive and degradable ability applied as bio-tape

This study explored the development of polyvinylpyrrolidone (PVP)–honey-gel (PHG) through 3D printing, aiming to develop a multifunctional bio-tape with adhesive and degradable properties. Based on the potential of honey to promote wound healing due to its antibacterial and anti-inflammatory properties, a PVP–honey-based 3D printing ink was developed by combining honey and PVP to create PHG through 3D printing technology that can form a film with strong adhesion and flexibility. First, the chemical–physical properties of PHG and its 3D printing performance were characterized. The line width achievable in 3D printing for the PHG line can extend to ∼100 µm. In addition, the adhesive properties of the PHG film were evaluated by using a 180° peeling test on various materials (glass, copper, wood, and pig skin), highlighting its potential for diverse applications. Finally, the application of the PHG film as a bio-tape was demonstrated through a successful animal experiment on a rabbit’s skin wound. Due to its adhesive and degradable properties, the bio-tape exhibited 3D conformability and ease of removal without residue.

Plant Decellularization by Chemical and Physical Methods for Regenerative Medicine: A Review Article.

Fabricating three-dimensional (3D) scaffolds is attractive due to various advantages for tissue engineering, such as cell migration, proliferation, and adhesion. Since cell growth depends on transmitting nutrients and cell residues, naturally vascularized scaffolds are superior for tissue engineering. Vascular passages help the inflow and outflow of liquids, nutrients, and waste disposal from the scaffold and cell growth. Porous scaffolds can be prepared by plant tissue decellularization which allows for the cultivation of various cell lines depending on the intended application. To this end, researchers decellularize plant tissues by specific chemical and physical methods. Researchers use plant parts depending on their needs, for example, decellularizing the leaves, stems, and fruits. Plant tissue scaffolds are advantageous for regenerative medicine, wound healing, and bioprinting. Studies have examined various plants such as vegetables and fruits such as orchid, parsley, spinach, celery, carrot, and apple using various materials and techniques such as sodium dodecyl sulfate, Triton X-100, peracetic acid, deoxyribonuclease, and ribonuclease with varying percentages, as well as mechanical and physical techniques like freeze-thaw cycles. The process of data selection, retrieval, and extraction in this review relied on scholarly journal publications and other relevant papers related to the subject of decellularization, with a specific emphasis on plant-based research. The obtained results indicate that, owing to the cellulosic structure and vascular nature of the decellularized plants and their favorable hydrophilic and biological properties, they have the potential to serve as biological materials and natural scaffolds for the development of 3D-printing inks and scaffolds for tissue engineering.

Regulation of rheological properties of soy protein isolate-beeswax based bigel inks for high-precision 3D printing

Bigel inks were developed for high-precision 3D food printing using soy protein isolate (SPI) hydrogel and beeswax oleogel. The ratio of hydrogel to oleogel played a crucial role in determining the rheology and moisture state of the inks. When the ratio of hydrogel to oleogel reached 7:3, the ink was softer and showed stronger shear-thinning properties, which resulted in better recoverability and stronger self-supportability. These were demonstrated by the lowest flow index (n value) of 0.135, the largest recovery viscosity of 10.920 × 105 mPa s, and the biggest yield stress (1034.200 Pa), complex modulus (G* of 6608.066 Pa), and gel strength (A value of 488.34 × 103 Pa s1/z). Additionally, the ink contained more semi-solid water (T22) and had a higher proportion of moisture freedom (A23). Consequently, the ink had a smooth extrusion while exhibiting strong mechanical properties and better structure stability. As a result, a hollow-rotating structure was achieved with a height of 20.05 mm, a gap diameter of 10.11 mm, and an inclination angle of 46.13° with precision beyond 99%. This was attributed to the presence of more β′ and β crystals with high oleogel content, which might protect the completeness of the SPI hydrogel network structure and prevent the aggregation of oleogel particles. In this turn, it improved the microstructure of the SPI-based bigel inks and made them more resistant to shearing during extrusion. This work provides a new insight into the application of SPI in personalized diets.

On the cogent formulation of an elastomeric silicone ink material for direct ink write (DIW) 3D printing

AbstractAdhesives and sealants show fine rheology with good physical and mechanical properties as viscous pastes, a possible starting point for developing direct ink writing (DIW) 3D printing ink. However, many commercial adhesives and sealants take days or weeks to cure fully. DIW 3D‐printed parts made directly from these sealants are not designed for a scalable manufacturing process and high‐volume production. Moreover, most of these adhesives and sealants have volume shrinkage during cure. A systematic understanding of formulation methods and design principles for an elastomeric silicone DIW ink can overcome these issues. This study presents the cogent formulation development of a 3D printable thermoset elastomer silicone that gels and cures isotropically in minutes, reducing cycle time for rapid ink development with no shrinkage during cure. More specifically, we outline the principles of raw material selection of a formulation to achieve excellent rheology, printability, synchronized working, and gel time fitting requirements closer to scalable manufacturing. The reaction kinetics and their corresponding 3D‐printed structural properties are also described. Interest in future work is toward a rational DIW 3D printing ink material development protocol and use of machine learning (ML).Highlights Formulation method flexibility and design principle of DIW ink. Raw material selection principle to achieve optimal rheology for DIW printing. Ink gel kinetics for large‐scale DIW manufacturing. Hydrosilylation conversion over time at different ambient temperatures. Structural properties of DIW 3D printed parts.

3D printing of cyanate ester resins with interpenetration networks for enhanced thermal and mechanical properties

AbstractCyanate ester (PT‐30) resin possesses exceptional thermal and mechanical properties, including high heat distortion temperature, high glass transition temperature (Tg), and outstanding mechanical characteristics. Conversely, the Tg of the homopolymer of tris(2‐hydroxyethyl)isocyanurate triacrylate (T‐acrylate) surpasses that of other acrylates. The combination of PT‐30 and T‐acrylate results in the formation of an interpenetrating polymer network (IPN) through a dual curing mechanism. Furthermore, the combination of these two polymers enables the tuning of rheology for shear thinning behavior for Ink Extrusion 3D printing technology by adjusting the amount of photoinitiator and rheological modifier. Here, 3D printable ink was formulated using PT‐30, T‐acrylate with a higher Tg, a photoinitiator, and a powdered rheological additive. The printed structures underwent a dual‐curing process involving exposure to UV light and thermal curing. Thermomechanical properties of the printed samples were characterized using dynamic mechanical analysis, thermogravimetric analysis, and tensile testing. The successful formation of an IPN structure through the polymerization of T‐acrylate and PT‐30 was observed, resulting in improved mechanical properties and an elevated Tg. The Fourier transform infrared spectroscopy analysis verified the formation of cross‐linked samples. Overall, this study demonstrates the feasibility of Ink Extrusion 3D printing, using a cyanate ester resin and tris(2‐hydroxyethyl)isocyanurate triacrylate with a dual‐curing mechanism. The enhanced mechanical properties at elevated temperatures (~80% retention of room temperature tensile strength at 200°C for sample with 70/30 wt%) and high Tg of 349 ± 3°C for printed structures shown in this study make them suitable for high‐performance structural applications in industries such as aerospace, defense, and microelectronics.

Hydrogel Ink for 3D Printing with High and Widely Tunable Mechanical Properties via the Salting‐Out Effect

AbstractDue to the difficulty of simultaneously ensuring printability and controlling their mechanical properties, 3D printed hydrogels thus far have low modulus, far less than that of many biological tissues and organs. Therefore, their feasibility toward various biomimetic applications is currently limited. Herein, Direct‐Ink‐Writing (DIW) based 3D printable hydrogel ink with broadly adjustable mechanical properties is introduced. The salting‐out effect is utilized to effectively lower the gelation temperature of hydrogel inks with a wide range of modulus (0.193–1.072 MPa), making them all 3D printable. As a proof of concept, multi‐layered synthetic blood vessels that mimic the mechanical properties of biological blood vessels are printed, and their practicability toward surgical training is demonstrated. The versatility and simplicity of this technique make it highly promising for use in various 3D‐printed hydrogel biomaterials applications.

3D printed emulsion based on arginine-myofibrillar protein

The feasibility of preparing high internal phase Pickering emulsions (HIPPEs) from arginine (Arg) and tilapia myofibrillar protein (MP) complex particles for 3D printing was investigated. The characterization of Arg-MP solutions showed that the Arg-MP complexes had excellent emulsification potential. HIPPE stabilized by Arg-MP had a strong self-supporting and stable gel structure. Therefore, HIPPE stabilized by Arg-MP showed excellent stability. Furthermore, the viscoelasticity and thixotropic recovery of the Arg-MP-stabilized HIPPEs increased with increasing Arg concentrations. This made them suitable for 3D printing. Notably, the Arg-MP stabilized HIPPEs exhibited the best printing precision shape, resolution, and clear contours in 3D printing at an Arg concentration of 0.5 wt%. Our results provide a valuable source of food-grade materials for 3D printing inks and demonstrate a promising strategy for deep processing of tilapia myofibrillar protein.

A Molecular Rheology Dynamics Study on 3D Printing of Liquid Crystal Elastomers.

This work presents a rheological study of a biocompatible and biodegradable liquid crystal elastomer (LCE) ink for three dimensional (3D) printing. These materials have shown that their structural variations have an effect on morphology, mechanical properties, alignment, and their impact on cell response. Within the last decade LCEs are extensively studied as potential printing materials for soft robotics applications, due to the actuation properties that are produced when liquid crystal (LC) moieties are induced through external stimuli. This report utilizes experiments and coarse-grained molecular dynamics to study the macroscopic rheology of LCEs in nonlinear shear flow. Results from the shear flow simulations are in line with the outcomes of these experimental investigations. This work believes the insights from these results can be used to design and print new material with desirable properties necessary for targeted applications.

Stabilizing effect of silver carp myofibrillar protein modified by high intensity ultrasound on high internal phase emulsions: Protein denaturation, interfacial adsorption and reconfiguration

This study evaluated the impact of high intensity ultrasound (HIU) on myofibrillar proteins (MP) from silver carp, and investigated the stabilizing effect of HIU-treated MP (UMP) on high internal phase emulsions (HIPEs). Ultrasonic cavitation induced protein denaturation by decreasing size and unfolding conformation, to expose more hydrophobic groups, particularly UMP at 390 W, showing the smallest particle size (181.71 nm) and most uniform distribution. These structural changes caused that UMP under 390 W exhibited the highest surface hydrophobicity, solubility (92.72 %) and emulsibility (115.98 m2/g and 70.4 min), all of which contributed to fabricating stable HIPEs with oil volume fraction up to 0.8. UMP-based HIPEs possessed tightly packed gel network and self-supporting appearance due to the adsorption of numerous proteins at the oil-water interface and the reduction of interfacial tension by protein reconfiguration. The larger interface coverage reinforced cross-linking between interfacial proteins, thus increasing the viscoelasticity and recoverability of HIPEs, also the resistance to centrifugal force, high temperature (90 °C, 30 min) and freeze-thaw cycles. These findings furnished insightful perspectives for MP deep processing through HIU, expanding the high-value application of UMP-based HIPEs in fat replacer, nutritional delivery system with high encapsulation content and novel 3D printing ink.

Development of cellulose based food-ink from cellulose powder

Three-dimensional or 3D printing studies utilizing biopolymer, a digital manufacturing technology acting as additive manufacturing, have gained global attention, particularly in the food industries. However, the utilization of cellulose powder to create food ink for 3D printing is relatively recent. Therefore, this study aimed to prepare cellulose-based food ink, analysed using carboxymethyl cellulose powder (CMC) through rheology and thermal analysis. The formulated cellulose-based food ink from carboxymethyl cellulose powder underwent examination through rheology, thermogravimetric analysis (TGA), and Fourier -transformed infrared spectroscopy (FTIR). The results showed shear-thinning behaviour for rheology properties and the presence of the hydroxyl group (–OH stretching), C–H stretching vibration and ether groups (–O– stretching), which was excellent for 3D printing. The amount of CMC powder used in the food ink formulation was increased due to the higher thermal stability of the food ink as determined by the TGA. This discovery is applicable to 3D printing in the food industry since CMC powder exhibits shear thinning behaviour at low concentrations and has stable thermal characteristics comparable to printable and edible materials.

Semisolid extrusion 3D printing of Dolutegravir-Chitosan nanoparticles laden polymeric buccal films: personalized solution for pediatric treatment.

In this work, the semi solid extrusion 3D printing process was utilized to incorporate anti-HIV drug Dolutegravir and its nanoparticles into the buccal film (BF) that was fabricated using the developed polymer ink. The composite made of polyvinyl alcohol (PVA) and sodium alginate was processed into a 3D printing polymer ink with optimum viscosity (9587 ± 219 cP) needed for the seamless extrusion through the nozzle of the 3D printer. The formulated BFs were assessed for its physical properties like weight (0.414 ± 0.3 g), thickness (1.54 ± 0.02 mm), swelling index (18.5 ± 0.91%), and mucoadhesiveness strength (0.165 ± 0.09 N) etc, The structural integrity and the surface morphology of the developed BFs were investigated by scanning electron microscopy analysis. The chemical stability and the solid-state nature of the drug in the BFs were assessed by Fourier transform infrared and x-ray diffraction analysis respectively. Further the BFs were assessed for drug dissolutionin-vitroandex-vivo, to study the effect of polymer composition and printing condition on the dissolution profile of the drug in the simulated salivary fluid. The results demonstrated that the developed PVA based polymer ink for 3D printing utilizing pressure is a versatile approach in the context of manufacturing mucoadhesive BFs customized in terms of shape and the amount of drug loaded.

Valorization of straw biomass into lignin bio-ink, bacterial cellulose and activated nanocarbon through the trade-off alkali-catalyzed glycerol organosolv biorefinery

Integrated lignocellulosic biorefinery that transforms low-value lignocellulose into multiple value-added products is crucial for a low-carbon sustainable development. Herein, a one-pot alkali-catalyzed glycerol organosolv (ALGO) pretreatment-based integrated biorefinery process to directionally produce lignin bio-inks, bacterial celluloses (BCs), and activated nanocarbons (ANCs) was proposed. ALGO pretreatment could modify the structure of dissolved lignins by glycerolysis. The extracted lignin fragments with high-purity (>90 %), uniform with low molecular weight (2500–4000 of Mw), and abundant hydrophilic aliphatic –OH were promising candidates in 3D-printable inks preparation. The glycerolysis reaction during ALGO process also enabled pretreated substrates toward high hydrolyzability and protected pretreatment liquor from generating fermentable inhibitors, making the solid fractions more liable for enzymatic deconstruction and microbial fermentation. Without any detoxification treatments, hydrolysates from ALGO pretreated substrates were used directly as carbon sources for BCs production, resulting in the BC yields were 56 % higher than that of the commercial glucose. The enzymatic hydrolysis residue and BC fermentation waste liquid were synthesized into ANCs via a facile carbonization process, which could further increase the value of ALGO biorefinery. Calculations showed that this ALGO integrated strategy rendered the conversion of ∼75 % lignins in pretreatment liquor to bio-inks and nearly 100 % solid fractions to BCs and ANCs. Unlike the conventional “lignin-first” route to obtain high-purity cellulose by sacrificing the value-adding conversion ability of by-products, the designed technical route in this work achieved a good trade-off between fractionation ability and subsequent conversion potential, inspiring further exploration of the technical correlation between biomass fractionation and bioproduct processing.

Toughening 3D printed biomimetic hydroxyapatite scaffolds: Polycaprolactone-based self-hardening inks

The application of 3D printing to calcium phosphates has opened unprecedented possibilities for the fabrication of personalized bone grafts. However, their biocompatibility and bioactivity are counterbalanced by their high brittleness. In this work we aim at overcoming this problem by developing a self-hardening ink containing reactive ceramic particles in a polycaprolactone solution instead of the traditional approach that use hydrogels as binders. The presence of polycaprolactone preserved the printability of the ink and was compatible with the hydrolysis-based hardening process, despite the absence of water in the ink and its hydrophobicity. The microstructure evolved from a continuous polymeric phase with loose ceramic particles to a continuous network of hydroxyapatite nanocrystals intertwined with the polymer, in a configuration radically different from the polymer/ceramic composites obtained by fused deposition modelling. This resulted in the evolution from a ductile behavior, dominated by the polymer, to a stiffer behavior as the ceramic phase reacted. The polycaprolactone binder provides two highly relevant benefits compared to hydrogel-based inks. First, the handleability and elasticity of the as-printed scaffolds, together with the proven possibility of eliminating the solvent, opens the door to implanting the scaffolds freshly printed once lyophilized, while in a ductile state, and the hardening process to take place inside the body, as in the case of calcium phosphate cements. Second, even with a hydroxyapatite content of more than 92 wt.%, the flexural strength and toughness of the scaffolds after hardening are twice and five times those of the all-ceramic scaffolds obtained with the hydrogel-based inks, respectively. Statement of significanceOvercoming the brittleness of ceramic scaffolds would extend the applicability of synthetic bone grafts to high load-bearing situations. In this work we developed a 3D printing ink by replacing the conventional hydrogel binder with a water-free polycaprolactone solution. The presence of polycaprolactone not only enhanced significantly the strength and toughness of the scaffolds while keeping the proportion of bioactive ceramic phase larger than 90 wt.%, but it also conferred flexibility and manipulability to the as-printed scaffolds. Since they are able to harden upon contact with water under physiological conditions, this opens up the possibility of implanting them immediately after printing, while they are still in a ductile state, with clear advantages for fixation and press-fit in the bone defect.

3D-printed metal-organic framework encapsulated Keggin heteropolyacid for catalytic purpose

To address the limitations of metal-organic frameworks for large-scale applications and the challenges associated with the heterogenization of heteropolyacids, we developed a catalytic monolith leveraging the encapsulation concept and 3D-printing technology. In this approach, a Keggin-type heteropolyacid was encapsulated within a Fe-based metal-organic framework through an in-situ method and subsequently incorporated into a 3D printing ink for the fabrication of a catalytic monolith. The monolith underwent comprehensive characterization, elucidating its morphological, structural, and mechanical features. Moreover, the catalytic performance of the 3D-printed monolith was thoroughly evaluated in Knoevenagel condensation reaction, highlighting its remarkable catalytic activity and exceptional recyclability. Characterization of the recycled catalyst, along with a hot filtration test, further confirmed the stability of the catalyst, the suppression of heteropolyacid leaching, and the manifestation of true heterogeneous catalysis.