Granulation of Fine Eggshell Powder to Produce Feedstock Powder for Binder Jetting Additive Manufacturing: Effects of Spraying Pressure and Slurry Feed Rate

Abstract

Eggshell powder is a sustainable calcium carbonate-based material with potential as a feedstock for binder jetting additive manufacturing. However, its irregular particles exhibit poor flowability and powder spreading characteristics. Although spray freeze drying granulation has previously been shown to improve the properties of eggshell powder, the influence of process variables on the resulting granules remains insufficiently understood. This study investigates the effects of spraying pressure and slurry feed rate on the properties of granulated eggshell powder. One-factor-at-a-time experiments were conducted to identify feasible ranges of these process variables, and a full factorial design of experiments with two replications was employed to evaluate the main and interaction effects of spraying pressure and slurry feed rate on particle size and flowability of granulated eggshell powder. Spraying pressure had a statistically significant effect on particle size, whereas slurry feed rate did not significantly affect particle size within the investigated range. Increasing spraying pressure resulted in smaller granules. Powder flowability was evaluated using both the Hausner ratio and repose angle. Both measures showed a significant interaction between spraying pressure and slurry feed rate, indicating that powder flowability depends on the combined effects of these two variables. The findings suggest that spraying pressure is the key variable governing particle size, while the combined influence of spraying pressure and slurry feed rate must be considered when controlling powder flowability. The resulting process–property relationships provide a basis for selecting spray freeze drying conditions for converting eggshell waste into more suitable granulated feedstock for binder jetting additive manufacturing.

Keywords

Eggshell powder / Spray freeze drying granulation / Spraying pressure / Slurry feed rate / Binder jetting additive manufacturing

References

[1] Zhu B, Li R, Yuan T, Li W, Cai D, Kang N. Metal binder jetting additive manufacturing: An overview of the process, materials and reinforcement methods. J. Alloys Compd. 2025, 1037, 182196. DOI: 10.1016/j.jallcom.2025.182196

[2] Khan F, Pei Z, Arman MS, Kuntzendorf S, Kao Y-T. Effects of Dispense Delay and Recoat Speed on Green Part Density and Powder Bed Density in Binder Jetting Additive Manufacturing. J. Manuf. Mater. Process. 2026, 10, 80. DOI: 10.3390/jmmp10030080

[3] Mehrabi M, Gardy J, Talebi FA, Farshchi A, Hassanpour A, Bayly AE. An investigation of the effect of powder flowability on the powder spreading in additive manufacturing. Powder Technol. 2023, 413, 117997. DOI: 10.1016/j.powtec.2022.117997

[4] Mussatto A, Groarke R, O’Neill A, Obeidi MA, Delaure Y, Brabazon D. Influences of powder morphology and spreading parameters on the powder bed topography uniformity in powder bed fusion metal additive manufacturing. Addit. Manuf. 2021, 38, 101807. DOI: 10.1016/j.addma.2020.101807

[5] Miyanaji H, Rahman KM, Da M, Williams CB. Effect of fine powder particles on quality of binder jetting parts. Addit. Manuf. 2020, 36, 101587. DOI: 10.1016/j.addma.2020.101587

[6] Barthel B, Janas F, Wieland S. Powder condition and spreading parameter impact on green and sintered density in metal binder jetting. Powder Metall. 2021, 64, 378-386. DOI: 10.1080/00325899.2021.1912923

[7] Seikh Z, Mallick MA, Gazi AS, Sekh M. An Overview of Utilization of Egg Shell Wastes: A Transformation from Waste to Wealth. J. Inst. Eng. India Ser. D 2026, 107, 1471-1485. DOI: 10.1007/s40033-024-00856-9

[8] Baláž M, Boldyreva EV, Rybin D, Pavlović S, Rodríguez-Padrón D, Mudrinić T, et al. State-of-the-Art of Eggshell Waste in Materials Science: Recent Advances in Catalysis, Pharmaceutical Applications, and Mechanochemistry. Front Bioeng. Biotechnol. 2021, 8, 612567. DOI: 10.3389/fbioe.2020.612567

[9] Marczyk J, Ostrowska K, Hebda M. Influence of binder jet 3D printing process parameters from irregular feedstock powder on final properties of Al parts. Adv. Powder Technol. 2022, 33, 103768. DOI: 10.1016/j.apt.2022.103768

[10] Du W, Miao G, Pei Z, Ma C. Comparison of Flowability and Sinterability Among Different Binder Jetting Feedstock Powders: Nanopowder, Micropowder, and Granulated Powder. J. Micro Nano-Manuf. 2021, 9, 021008. DOI: 10.1115/1.4052253

[11] Chen Q, Juste E, Lasgorceix M, Petit F, Leriche A. Binder jetting process with ceramic powders: Influence of powder properties and printing parameters. Open Ceram. 2022, 9, 100218. DOI: 10.1016/j.oceram.2022.100218

[12] Ranjan OP, Kumbhar AP. 10-Dry and wet granulation. In Polymers for Oral Drug Delivery Technologies ; Parambath A, Ed.; Elsevier Science Ltd.: Amsterdam, The Netherlands, 2025; pp. 463-494. DOI: 10.1016/B978-0-443-13774-7.00010-4

[13] Shanmugam S. Granulation techniques and technologies: Recent progresses. Bioimpacts 2015, 5, 55-63. DOI: 10.15171/bi.2015.04

[14] Sandler N, Lammens RF. Pneumatic dry granulation: potential to improve roller compaction technology in drug manufacture. Expert Opin. Drug Deliv. 2011, 8, 225-236. DOI: 10.1517/17425247.2011.548382

[15] Vadaga AK, Gudla SS, Nareboina GSK, Gubbala H, Golla B. Comprehensive review on modern techniques of granulation in pharmaceutical solid dosage forms. Intell. Pharm. 2024, 2, 609-629. DOI: 10.1016/j.ipha.2024.05.006

[16] Mariani M, Bertolini F, Mercadelli E, Blanco GF, Baldisserri C, Sanchez-Herencia AJ, et al. Spray drying granulation of potassium sodium niobate (KNN) for binder jetting: Feedstock preparation and influence on sintered material properties. Open Ceram. 2025, 21, 100743. DOI: 10.1016/j.oceram.2025.100743

[17] Mariani M, Frias Blanco G, Mercadelli E, Sánchez-Herencia AJ, Galassi C, Lecis N, et al. Tailoring α-alumina powder morphology through spray drying for cold consolidation by binder jetting. Open Ceram. 2022, 12, 100307. DOI: 10.1016/j.oceram.2022.100307

[18] Santos D, Maurício AC, Sencadas V, Santos JD, Fernandes MH, Gomes PS. Spray Drying: An Overview. Biomaterials-Physics and Chemistry-New Edition ; IntechOpen: London, UK, 2017. DOI: 10.5772/intechopen.72247

[19] Liu B, Wang J, Zeng J, Zhao L, Wang Y, Feng Y, et al. A review of high shear wet granulation for better process understanding, control and product development. Powder Technol. 2021, 381, 204-223. DOI: 10.1016/j.powtec.2020.11.051

[20] Scott AC, Hounslow MJ, Instone T. Direct evidence of heterogeneity during high-shear granulation. Powder Technol. 2000, 113, 205-213. DOI: 10.1016/S0032-5910(00)00354-5

[21] Ming L, Li Z, Wu F, Du R, Feng Y. A two-step approach for fluidized bed granulation in pharmaceutical processing: Assessing different models for design and control. PLoS ONE 2017, 12, e0180209. DOI: 10.1371/journal.pone.0180209

[22] Burggraeve A, Monteyne T, Vervaet C, Remon JP, Beer TD. Process analytical tools for monitoring, understanding, and control of pharmaceutical fluidized bed granulation: A review. Eur. J. Pharm. Biopharm. 2013, 83, 2-15. DOI: 10.1016/j.ejpb.2012.09.008

[23] Stunda-Zujeva A, Irbe Z, Berzina-Cimdina L. Controlling the morphology of ceramic and composite powders obtained via spray drying-A review. Ceram. Int. 2017, 43, 11543-11551. DOI: 10.1016/j.ceramint.2017.05.023

[24] Ioannou Sartzi M, Drettas D, Stramarkou M, Krokida M. A Comprehensive Review of the Latest Trends in Spray Freeze Drying and Comparative Insights with Conventional Technologies. Pharmaceutics 2024, 16, 1533. DOI: 10.3390/pharmaceutics16121533

[25] Singlard M, Paillassa A, Ferres L, Pagnoux C, Aimable A. Freeze granulation and spray drying of mixed granules of Al₂O₃ . Powder Technol. 2022, 395, 280-289. DOI: 10.1016/j.powtec.2021.09.044

[26] Kondo N, Shimamura A, Hotta M, Tatatmi J, Kawaguchi S. Comparison of alumina granules prepared by spray freeze granulation drying and spray drying. J. Ceram. Soc. Jpn. 2020, 128, 922-926. DOI: 10.2109/jcersj2.20041

[27] Rautenberg A, Lamprecht A. Spray-freeze-dried lyospheres: Solid content and the impact on flowability and mechanical stability. Powder Technol. 2022, 411, 117905. DOI: 10.1016/j.powtec.2022.117905

[28] Yamazaki R, Tatami J, Iijima M, Kawaguchi S, Kondo N. Freezing behaviour and spray freeze granulation drying of silicon nitride slurries prepared from tert-butyl alcohol and cyclohexane solvent mixtures. Adv. Powder Technol. 2025, 36, 105030. DOI: 10.1016/j.apt.2025.105030

[29] Farinha S, Sá JV, Lino PR, Galésio M, Pires J, Rodrigues MÂ, et al. Spray Freeze Drying of Biologics: A Review and Applications for Inhalation Delivery. Pharm. Res. 2023, 40, 1115-1140. DOI: 10.1007/s11095-022-03442-4

[30] Ishwarya SP, Anandharamakrishnan C, Stapley AGF. Spray-freeze-drying: A novel process for the drying of foods and bioproducts. Trends Food Sci. Technol. 2015, 41, 161-181. DOI: 10.1016/j.tifs.2014.10.008

[31] Silva JM, Teixeira CCC, Tacon LA, Freitas LVD, Meneguin AB, Barud HS, et al. Nanoporous microparticles of cellulose nanofibrils: The effect of fluid bed atmospheric spray freeze drying. Powder Technol. 2025, 452, 120502. DOI: 10.1016/j.powtec.2024.120502

[32] Polozov I, Razumov N, Masaylo D, Silin A, Lebedeva Y, Popovich A. Fabrication of Silicon Carbide Fiber-Reinforced Silicon Carbide Matrix Composites Using Binder Jetting Additive Manufacturing from Irregularly-Shaped and Spherical Powders. Materials 2020, 13, 1766. DOI: 10.3390/ma13071766

[33] Miao G, Du W, Moghadasi M, Pei Z, Ma C. Ceramic binder jetting additive manufacturing: Effects of granulation on properties of feedstock powder and printed and sintered parts. Addit. Manuf. 2020, 36, 101542. DOI: 10.1016/j.addma.2020.101542

[34] Du W, Li M, Pei Z, Ma C. Roller-compaction-assisted binder jetting with different granulated zirconia powders. Manuf. Lett. 2023, 35, 576-582. DOI: 10.1016/j.mfglet.2023.08.031

[35] Huang S, Ye C, Zhao H, Fan Z, Wei Q. Binder jetting yttria stabilised zirconia ceramic with inorganic colloid as a binder. Adv. Appl. Ceram. 2019, 118, 458-465. DOI: 10.1080/17436753.2019.1666593

[36] Du W, Miao G, Liu L, Pei Z, Ma C. Binder Jetting Additive Manufacturing of Ceramics: Feedstock Powder Preparation by Spray Freeze Granulation. In Proceedings of the ASME 2019 14th International Manufacturing Science and Engineering Conference, Erie, PA, USA. 10-14 June 2019; Volume 1: Additive Manufacturing; Manufacturing Equipment and Systems; Bio and Sustainable Manufacturing ; ASME: New York, NY, USA, 2019; V001T01A006. DOI: 10.1115/MSEC2019-3001

[37] Arman MS, Khan F, Pasha MM, Sanders J, Pei Z. Granulation of fine eggshell powder to produce feedstock powder for binder jetting additive manufacturing: A feasibility study. Mater. Today Commun. 2025, 46, 112918. DOI: 10.1016/j.mtcomm.2025.112918

[38] Standard Test Method for Apparent Density of Free-Flowing Metal Powders Using the Hall Flowmeter Funnel. Available online: https://store.astm.org/b0212-17.html (accessed on 2 July 2026).

[39] Standard Test Method for Tap Density of Metal Powders and Compounds. Available online: https://store.astm.org/b0527-23.html (accessed on 2 July 2026).

[40] Passerine BFG, Breitkreitz MC. Important Aspects of the Design of Experiments and Data Treatment in the Analytical Quality by Design Framework for Chromatographic Method Development. Molecules 2024, 29, 6057. DOI: 10.3390/molecules29246057

[41] Marques A, Cunha A, Faria S, Silva FS, Carvalho O. Predictive models on the influence of laser texturing parameters on the Inconel 718 surface by using Nd: YVO4 laser. Opt. Laser Technol. 2022, 154, 108320. DOI: 10.1016/j.optlastec.2022.108320

[42] Mandato S, Rondet E, Delaplace G, Barkouti A, Galet L, Accart P, et al. Liquids’ atomization with two different nozzles: Modeling of the effects of some processing and formulation conditions by dimensional analysis. Powder Technol. 2012, 224, 323-330. DOI: 10.1016/j.powtec.2012.03.014

[43] Yu B, Feng YJ, Wohn LS, Huang C, Li YF, Jia Z. Spray-drying of alumina powder for APS: Effect of slurry properties and drying conditions upon particle size and morphology of feedstock. Bull. Mater. Sci. 2011, 34, 1653-1661. DOI: 10.1007/s12034-011-0373-0

[44] Schappo H, Giry K, Damia C, Hotza D. Screening method for producing suitable spray-dried HA powder for SLS application. Powder Technol. 2021, 384, 62-69. DOI: 10.1016/j.powtec.2021.02.004