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Green innovations in natural paper ink: trends, applications, and future prospects

  • Nicky Rahmana Putra EMAIL logo and Bramantyo Airlangga EMAIL logo
Published/Copyright: May 23, 2025
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Abstract

Natural inks have emerged as eco-friendly alternatives to synthetic inks in the paper printing industry due to their biodegradability, non-toxicity, and sustainability. Derived from renewable sources such as plants, algae, minerals, and fungi, these inks reduce environmental pollution and dependence on petroleum-based materials. This review highlights recent advancements in natural ink extraction, formulation, and application, emphasizing improvements in physical and chemical properties. Studies show natural indicator inks using Lycium ruthenicum anthocyanins achieve a sensitivity of 2178.57 μA mM−1 cm−2 with a rapid response time of 18 s. Cobalt blue pigments derived from dolomite and kaolin tailings demonstrate high color performance (L* = 37.63, a* = 10.68, b* = −54.87) and 94.96 % light absorption efficiency. Packaging papers containing triticale straw fibers reduced color variation (ΔE*) by 20 % after aging and rubbing tests. Plasma treatment and nano-chitosan coatings have improved color depth by up to 214 % and washing durability after 45 cycles. Despite these advancements, challenges remain in enhancing color fastness, water resistance, and scalability. This review outlines future research directions focused on advanced extraction, formulation optimization, and life cycle assessments to promote the industrial application of sustainable natural inks.


Corresponding author: Nicky Rahmana Putra, Higher College of Technology (HCT), Ruwais, United Arab Emirates, E-mail: ickyrahman1309@gmail.com; and Bramantyo Airlangga, Department of Chemical Engineering, Institut Teknologi Sepuluh Nopember, Surabaya, East Java, Indonesia, E-mail:

Acknowledgments

We would like thank you to Higher College of Technology (HCT) and Institut Teknologi Sepuluh Nopember, Indonesia.

  1. Research ethics: Not applicable.

  2. Informed consent: Not applicable.

  3. Author contributions: Nicky Rahmana Putra = Writing Originial Draft, Bramantyo Airlangga = Writing Originial Draft.

  4. Use of Large Language Models, AI and Machine Learning Tools: Not applicable.

  5. Conflict of interest: Not applicable.

  6. Research funding: Not funding.

  7. Data availability: Not applicable.

References

Agurto, M.E.P., Gutierrez, S.M.V., Chen, H.L., and Robinson, S.C. (2017). Wood-rotting fungal pigments as colorant coatings on oil-based textile dyes. Coatings 7: 152, https://doi.org/10.3390/coatings7100152.Search in Google Scholar

Akyol, E. and Çakar Sevim, P. (2023). Dyes used for colouring manuscripts and their effect on cellulose degradation. Restaurator 44: 345–360, https://doi.org/10.1515/res-2023-0014.Search in Google Scholar

Al Kiey, S.A., Hasanin, M.S., and Heakal, F.E.T. (2022). Green and sustainable chitosan–gum Arabic nanocomposites as efficient anticorrosive coatings for mild steel in saline media. Sci. Rep. 12: 13209, https://doi.org/10.1038/s41598-022-17386-7.Search in Google Scholar PubMed PubMed Central

Almoulki, T. and Akkaya, E. (2023). Using chlorella vulgaris as a natural-textile dye. Environ. Res. Technol. 6: 326–331, https://doi.org/10.35208/ert.1264338.Search in Google Scholar

Attard-Montalto, N., Ojeda, J.J., Reynolds, A., Ismail, M., Bailey, M., Doodkorte, L., De Puit, M., and Jones, B.J. (2014). Determining the chronology of deposition of natural fingermarks and inks on paper using secondary ion mass spectrometry. Analyst 139: 4641–4653, https://doi.org/10.1039/c4an00811a.Search in Google Scholar PubMed

Attard Montalto, N., Ojeda, J.J., and Jones, B.J. (2013). Determining the order of deposition of natural latent fingerprints and laser printed ink using chemical mapping with secondary ion mass spectrometry. Sci. Justice 53: 2–7, https://doi.org/10.1016/j.scijus.2012.05.007.Search in Google Scholar PubMed

Berger-Karin, C., Hendriks, U., and Geyer-Lippmann, J. (2008). Comparison of natural and artificial aging of ballpoint inks. J. Forensic Sci. 53: 989–992, https://doi.org/10.1111/j.1556-4029.2008.00770.x.Search in Google Scholar PubMed

Borges, J.G., Garcia, V.A.D.S., and de Carvalho, R.A. (2019). Extraction of active compounds from different parts of pomegranate and incorporation into a potential delivery model system using a printing technique: incorporation of pomegranate extract using a printing technique. Food Biosci. 32: 100480, https://doi.org/10.1016/j.fbio.2019.100480.Search in Google Scholar

Cernencu, A., Lungu, A., Stancu, I.C., Vasile, E., and Iovu, H. (2019). Polysaccharide-based 3d printing inks supplemented with additives. UPB Scientific Bulletin, Series B: Chemistry and Materials Science 81: 175–186, Available at: https://www.scopus.com/inward/record.uri?eid=2-s2.0-85076595533&partnerID=40&md5=9d22ef98e2615f4ef8e13765b9b21053.Search in Google Scholar

Chang, C.W., Lee, J.J., and Lu, K.T. (2021). The effects of adding heartwood extractives from acacia confusa on the lightfastness improvement of refined oriental lacquer. Polymers 13: 4085, https://doi.org/10.3390/polym13234085.Search in Google Scholar PubMed PubMed Central

Chou, D.T., Wells, D., Hong, D., Lee, B., Kuhn, H., and Kumta, P.N. (2013). Novel processing of iron-manganese alloy-based biomaterials by inkjet 3-D printing. Acta Biomater. 9: 8593–8603, https://doi.org/10.1016/j.actbio.2013.04.016.Search in Google Scholar PubMed

Crowley, A.S. (1970). Repair and conservation of palm-leaf manuscripts. Restaurator 1: 105–114, https://doi.org/10.1515/rest.1970.1.2.105.Search in Google Scholar

Da Costa, A.C.A., Da Fonseca, N.F., De Carvalho, S.S., Dos Santos, F.C.S.C., Barki, L., De Freitas, D.S., Herbst, M.H., and Lutterbach, M.T.S. (2013). Archaeometric investigations on naturally and thermally-aged iron-gall inks using different tannin sources. Cent. Eur. J. Chem. 11: 1729–1739, https://doi.org/10.2478/s11532-013-0303-7.Search in Google Scholar

Desvergnes, A.C. and Berghe, I.V. (2018). Dyestuff identification and significance of interleaves from Moroccan manuscripts of Dalā’il al-Khayrāt. Stud. Conserv. 63: 236–250, https://doi.org/10.1080/00393630.2017.1314585.Search in Google Scholar

Domingos, E., De Carvalho, T.C., Pereira, I., Vasconcelos, G.A., Thompson, C.J., Augusti, R., Rodrigues, R.R.T., Tose, L.V., Santos, H., Araujo, J.R., et al.. (2017). Paper spray ionization mass spectrometry applied to forensic chemistry-drugs of abuse, inks and questioned documents. Anal. Methods 9: 4400–4409, https://doi.org/10.1039/c7ay01091e.Search in Google Scholar

Dorris, G. and Page, N. (1999) Natural and accelerated aging of old newspapers printed with black mineral oil inks and coloured vegetable oil inks. Part I: Deinkability. In: Research Forum on recycling, proceedings, pp. 43–53, Available at: https://www.scopus.com/inward/record.uri?eid=2-s2.0-0033312296&partnerID=40&md5=89c3e17fbc1fe26f638ad5481f90e7f8.Search in Google Scholar

Fathurrohmah, N.N., Murti, S.T.C., and Suryani, C.L. (2023). Effect of Zn–chlorophyll complexes formation on the color stability of pandan (Pandanus amaryllifolius) leaf extract. Food Sci. Technol. (United States) 11: 161–167, https://doi.org/10.13189/fst.2023.110304.Search in Google Scholar

Fillat, U., Prieto, A., Camarero, S., Martínez, Á.T., and Martínez, M.J. (2012). Biodeinking of flexographic inks by fungal laccases using synthetic and natural mediators. Biochem. Eng. J. 67: 97–103, https://doi.org/10.1016/j.bej.2012.05.010.Search in Google Scholar

Jin, W.J., He, W.L., Lehner, S., Cheng, X.W., Gaan, S., and Guan, J.P. (2024). Edible squid ink proteoglycans as a multifunctional sustainable additive for silk coatings: fire protection, UV shielding and as a colorant. Chem. Eng. J. 495: 153320, https://doi.org/10.1016/j.cej.2024.153320.Search in Google Scholar

Karabel Ocal, S., Kiremitler, N.B., Yazici, A.F., Celik, N., Mutlugun, E., and Onses, M.S. (2022). Natural wax-stabilized perovskite nanocrystals as pen-on-paper inks and doughs. ACS Appl. Nano Mater. 5: 6201–6212, https://doi.org/10.1021/acsanm.2c00224.Search in Google Scholar

Klančnik, M. (2024). Printing with natural dye extract from Japanese knotweed leaves. Fibers Polym. 25: 4771–4785, https://doi.org/10.1007/s12221-024-00760-9.Search in Google Scholar

Klančnik, M. and Koradin, E. (2024). Extraction of anthocyanin dye from staghorn sumac fruit in various solvents and use for pigment printing. Coatings 14: 1025, https://doi.org/10.3390/coatings14081025.Search in Google Scholar

Leva, M., Gherasimescu, C., and Butnaru, R. (2011). Study regarding the ink-jet printing with reactive dyes of natural silk. The influence of pretreatment conditions on the intensity of the prints. Industria Textila 62: 151–154, Available at: https://www.scopus.com/inward/record.uri?eid=2-s2.0-79960664236&partnerID=40&md5=d260605243b0d4639fb5ac2d3d1c7cb0.Search in Google Scholar

Levinton-Shamuilov, G., Cohen, Y., Azoury, M., Chaikovsky, A., and Almog, J. (2005). Genipin, a novel fingerprint reagent with colorimetric and fluorogenic activity, Part II: optimization, scope and limitations. J. Forensic Sci. 50: 1367–1371, https://doi.org/10.1520/jfs2005055.Search in Google Scholar

Li, B. (2015). Extraction percentage analysis of inkpad seals stored under different conditions. Aust. J. Forensic Sci. 47: 421–427, https://doi.org/10.1080/00450618.2014.982182.Search in Google Scholar

Li, X., Wang, M., Liu, Z., Yang, S., Xu, N., Zhao, W., Luo, G., and Liu, S. (2024). Alleviation of the plastic deformation of gel ink under strong stress through an esterification of xanthan gum reinforcing its double helix structure. Chin. J. Chem. Eng. 67: 49–57, https://doi.org/10.1016/j.cjche.2023.08.011.Search in Google Scholar

Liao, J., Zhang, X., and Yang, X. (2017). Research on Xinyu Grass linen embroidery techniques and styles. J. Silk 54: 30–36, https://doi.org/10.3969/j.issn.1001-7003.2017.02.007.Search in Google Scholar

Liu, K., Song, A., Li, H., and Li, C. (2024). Xanthan gum ink based on Lycium ruthenicum anthocyanin as an indicator of color change for monitoring freshness of cold fresh meat. Int. J. Biol. Macromol. 276: 133788, https://doi.org/10.1016/j.ijbiomac.2024.133788.Search in Google Scholar PubMed

Liu, Y., Kralj Cigić, I., and Strlič, M. (2017). Kinetics of accelerated degradation of historic iron gall ink-containing paper. Polym. Degrad. Stab. 142: 255–262, https://doi.org/10.1016/j.polymdegradstab.2017.07.010.Search in Google Scholar

Ma, H., Sun, C., Xue, G., Wu, G., Zhang, X., Han, X., Qi, X., Lv, X., Sun, H., and Zhang, J. (2019). Facile synthesis of fluorescent carbon dots from Prunus cerasifera fruits for fluorescent ink, Fe 3+ ion detection and cell imaging. Spectrochim. Acta, Part A: Mol. Biomol. Spectrosc. 213: 281–287, https://doi.org/10.1016/j.saa.2019.01.079.Search in Google Scholar PubMed

Mahanta, D. and Tiwari, S.C. (2005). Natural dye-yielding plants and indigenous knowledge on dye preparation in Arunachal Pradesh, northeast India. Curr. Sci. 88: 1474–1480, Available at: https://www.scopus.com/inward/record.uri?eid=2-s2.0-27744518136&partnerID=40&md5=025948f7b7af1dc3bba844652d82f6e4.Search in Google Scholar

Mauludifia, F., Astrinia, S.D., Meiranti, K.A., and Djaeni, M. (2019). Production of natural colorant powder from Clitoria ternatea l. using tray dryer which is dehumidified by zeolite. Pap. Present. J. Phys. Conf. Series 1295: 012018, https://doi.org/10.1088/1742-6596/1295/1/012018.Search in Google Scholar

Mei, Q., Zhou, C., Huang, L., Mao, T., and Han, K. (2025). Cost-effective, highly efficient, and stable evaporator constructed of Chinese ink impregnation superhydrophobic Xuan paper for solar-driven interfacial organic solvent purification. Sep. Purif. Technol. 353: 128534, https://doi.org/10.1016/j.seppur.2024.128534.Search in Google Scholar

Mertoglu-Elmas, G. (2017). The effect of colorants on the content of heavy metals in recycled corrugated board papers. BioResources 12: 2690–2698, https://doi.org/10.15376/biores.12.2.2690-2698.Search in Google Scholar

Mohamed, W.A., Mansour, M.M.A., and Salem, M.Z.M. (2019). Lemna gibba and Eichhornia crassipes extracts: clean alternatives for deacidification, antioxidation and fungicidal treatment of historical paper. J. Clean. Prod. 219: 846–855, https://doi.org/10.1016/j.jclepro.2019.02.097.Search in Google Scholar

Nawaz, M., Shakoor, R.A., Kahraman, R., and Montemor, M.F. (2021). Cerium oxide loaded with Gum Arabic as environmentally friendly anti-corrosion additive for protection of coated steel. Mater. Des. 198: 109361, https://doi.org/10.1016/j.matdes.2020.109361.Search in Google Scholar

Norouzi, M., Mohamadnia, Z., Ahmadi, E., Mahmoodi, N.O., and Kiyani, H. (2024). Multicolor switchable latexes containing a bicyclic aziridine compound as anticounterfeiting inks for reversible photopatterning. ACS Appl. Polym. Mater. 6: 9784–9793, https://doi.org/10.1021/acsapm.4c01643.Search in Google Scholar

Pan, X., Lü, L., Zhang, X., Sun, G., Shao, M., Huang, Y., and Shao, J. (2024). Research progress of photo-crosslinked silk fibroin 3D bioprinting ink. J. Silk 61: 50–59, https://doi.org/10.3969/j.issn.1001-7003.2024.08.006.Search in Google Scholar

Panda, S.S., Singh, N., and Singh, M.R. (2021). Development, characterization of traditional inks for restoration of ancient manuscripts and application on various substrates to understand stability. Vib. Spectrosc. 114: 103232, https://doi.org/10.1016/j.vibspec.2021.103232.Search in Google Scholar

Park, W.S. and Kim, H.J. (2022). A study on deacidification treatment of the deteriorated glue-treated Hanji using magnesium oxide. Palpu Chongi Gisul/J. Korea Tech. Assoc. Pulp Pap. Ind. 54: 163–171, https://doi.org/10.7584/JKTAPPI.2022.12.54.6.163.Search in Google Scholar

Razak, R., Barkeshli, M., and Othman, R. (2017). Traditional Malay black ink: an analysis of its recipes and characteristics. Adv. Sci. Lett. 23: 6189–6193, https://doi.org/10.1166/asl.2017.9233.Search in Google Scholar

Roldán, M.L., Centeno, S.A., and Rizzo, A. (2014). An improved methodology for the characterization and identification of sepia in works of art by normal Raman and SERS, complemented by FTIR, Py-GC/MS, and XRF. J. Raman Spectrosc. 45: 1160–1171, https://doi.org/10.1002/jrs.4620.Search in Google Scholar

Rudolf, M., Plazonić, I., Petric Maretić, K., and Bates, I. (2023). Overall stability valorization of printed sustainable packaging paper containing triticale straw pulp. Processes 11: 1465, https://doi.org/10.3390/pr11051465.Search in Google Scholar

Shen, J., Gu, H., He, Z., and Lin, W. (2023). Wattle-bark-tannin-derived carbon quantum dots as multi-functional nanomaterials for intelligent detection of Cr6+Ions, bio-imaging, and fluorescent ink applications. Ind. Eng. Chem. Res. 62: 3622–3634, https://doi.org/10.1021/acs.iecr.2c04348.Search in Google Scholar

Siraj, S., Al-Marzouqi, A.H., and Iqbal, M.Z. (2022). Development and mechano-chemical characterization of polymer composite sheets filled with silica microparticles with potential in printing industry. Polymers 14: 3351, https://doi.org/10.3390/polym14163351.Search in Google Scholar PubMed PubMed Central

Song, A., Wu, Y., and Li, C. (2025). Development and application of a time-temperature hydroxyethyl cellulose ink based on Clitoria ternatea L. blue petals anthocyanin and N-Hydroxyphthalimide for food freshness monitoring. Int. J. Biol. Macromol. 299: 140060, https://doi.org/10.1016/j.ijbiomac.2025.140060.Search in Google Scholar PubMed

Song, A., Wu, Y., Li, H., and Li, C. (2024). Development of xanthan gum intelligent oil-in-water ink and its application in pork freshness preservation. Int. J. Biol. Macromol. 275: 133576, https://doi.org/10.1016/j.ijbiomac.2024.133576.Search in Google Scholar PubMed

Tanveer, A., Gupta, S., Dwivedi, S., Yadav, S., and Yadav, D. (2024). Recycling of printed Xerographic paper using Aspergillusassiutensis enzyme cocktail: an integrated approach to sustainable development. Environ. Sci. Pollut. Res. 31: 39217–39231, https://doi.org/10.1007/s11356-024-33780-2.Search in Google Scholar PubMed

Wang, X.F., Yu, J., Xie, M.X., Yao, Y.T., and Han, J. (2008). Identification and dating of the fountain pen ink entries on documents by ion-pairing high-performance liquid chromatography. Forensic Sci. Int. 180: 43–49, https://doi.org/10.1016/j.forsciint.2008.06.008.Search in Google Scholar PubMed

Xu, K. and Luo, Y. (2023). Packaging ink microcapsules with high stability and biocompatibility based on natural dye gardenia blue. Colloids Surf. A Physicochem. Eng. Asp. 658: 130778, https://doi.org/10.1016/j.colsurfa.2022.130778.Search in Google Scholar

Xu, Y., Fang, K., Chen, W., Zhang, X., and Zhang, C. (2022). Enhanced reactive dye inkjet printing performance of antimicrobial silk fabrics surface modified with plasma and chitosan. Fibers Polym. 23: 2586–2596, https://doi.org/10.1007/s12221-022-4470-z.Search in Google Scholar

Yang, H., Mu, B., Zong, L., Zhu, Y., and Wang, A. (2023). Cleaner preparation of high blueness cobalt blue composite pigments using dolomite and kaolin tailing sand. J. Clean. Prod. 395: 136445, https://doi.org/10.1016/j.jclepro.2023.136445.Search in Google Scholar

Yu, X., Yang, L., Zhao, T., Zhang, R., Yang, L., Jiang, C., Zhao, J., Liu, B., and Zhang, Z. (2017). Multicolorful ratiometric-fluorescent test paper for determination of fluoride ions in environmental water. RSC adv. 7: 53379–53384, https://doi.org/10.1039/c7ra09972j.Search in Google Scholar

Zalke, J.B., Narkhede, N.P., Pandhurnekar, C.P., Rotake, D.R., and Singh, S.G. (2024). Non-enzymatic glucose detection with screen-printed chemiresistive sensor using green synthesised silver nanoparticle and multi-walled carbon nanotubes-zinc oxide nanofibers. Nanotechnology 6: 065502, https://doi.org/10.1088/1361-6528/ad090c.Search in Google Scholar PubMed

Zhao, Y., Wang, J., Wu, F., Xiong, H., Xue, P., and Fan, J. (2024). Preparation, properties and applications of natural biomass materials (Ⅺ) Highly branched, high concentration-low viscosity plant polysaccharides: Arabic gum. China Surfactant Deterg. Cosmet. 54: 1298–1306, https://doi.org/10.3969/j.issn.2097-2806.2024.11.002.Search in Google Scholar

Received: 2025-03-11
Accepted: 2025-05-05
Published Online: 2025-05-23
Published in Print: 2025-12-17

© 2025 Walter de Gruyter GmbH, Berlin/Boston

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