journal article·2025-12-17

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

Nicky Rahmana Putra, Bramantyo Airlangga

Publisher page

Abstract

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.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Microplastics and Plastic Pollution

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Higher College of Technology (HCT) , Ruwais , United Arab Emirates

Department of Chemical Engineering , Institut Teknologi Sepuluh Nopember , Surabaya , East Java , Indonesia

References (55)

Show source-provided references
1. 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/coatings7100152.10.3390/coatings7100152 ↗
2. 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-2023-0014.10.1515/res-2023-0014 ↗
3. 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/s41598-022-17386-7.10.1038/s41598-022-17386-7 ↗
4. 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.1264338.10.35208/ert.1264338 ↗
5. 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.10.1039/C4AN00811A ↗
6. 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.2012.05.007.10.1016/j.scijus.2012.05.007 ↗
7. 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.10.1111/j.1556-4029.2008.00770.x ↗
8. 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.2019.100480.10.1016/j.fbio.2019.100480 ↗
9. 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.
10. 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/polym13234085.10.3390/polym13234085 ↗
11. 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.2013.04.016.10.1016/j.actbio.2013.04.016 ↗
12. Crowley, A.S. (1970). Repair and conservation of palm-leaf manuscripts. Restaurator 1: 105–114, https://doi.org/10.1515/rest.1970.1.2.105.10.1515/rest.1970.1.2.105 ↗
13. 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/s11532-013-0303-7.10.2478/s11532-013-0303-7 ↗
14. 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/10.1080/00393630.2017.1314585.10.1080/00393630.2017.1314585 ↗
15. 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.10.1039/C7AY01091E ↗
16. 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.
17. 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.2023.110304.10.13189/fst.2023.110304 ↗
18. 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.2012.05.010.10.1016/j.bej.2012.05.010 ↗
19. 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.2024.153320.10.1016/j.cej.2024.153320 ↗
20. 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.2c00224.10.1021/acsanm.2c00224 ↗
21. Klančnik, M. (2024). Printing with natural dye extract from Japanese knotweed leaves. Fibers Polym. 25: 4771–4785, https://doi.org/10.1007/s12221-024-00760-9.10.1007/s12221-024-00760-9 ↗
22. 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/coatings14081025.10.3390/coatings14081025 ↗
23. 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.
24. 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/jfs2005055.10.1520/JFS2005055 ↗
25. Li, B. (2015). Extraction percentage analysis of inkpad seals stored under different conditions. Aust. J. Forensic Sci. 47: 421–427, https://doi.org/10.1080/00450618.2014.982182.10.1080/00450618.2014.982182 ↗
26. 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.2023.08.011.10.1016/j.cjche.2023.08.011 ↗
27. 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.
28. 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.2024.133788.10.1016/j.ijbiomac.2024.133788 ↗
29. 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.2017.07.010.10.1016/j.polymdegradstab.2017.07.010 ↗
30. 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.2019.01.079.10.1016/j.saa.2019.01.079 ↗
31. 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.
32. 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/10.1088/1742-6596/1295/1/012018.10.1088/1742-6596/1295/1/012018 ↗
33. 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.2024.128534.10.1016/j.seppur.2024.128534 ↗
34. 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.12.2.2690-2698.10.15376/biores.12.2.2690-2698 ↗
35. 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.2019.02.097.10.1016/j.jclepro.2019.02.097 ↗
36. 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.2020.109361.10.1016/j.matdes.2020.109361 ↗
37. 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.4c01643.10.1021/acsapm.4c01643 ↗
38. 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.
39. 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.2021.103232.10.1016/j.vibspec.2021.103232 ↗
40. 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.2022.12.54.6.163.10.7584/JKTAPPI.2022.12.54.6.163 ↗
41. 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.2017.9233.10.1166/asl.2017.9233 ↗
42. 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.4620.10.1002/jrs.4620 ↗
43. 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/pr11051465.10.3390/pr11051465 ↗
44. 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.2c04348.10.1021/acs.iecr.2c04348 ↗
45. 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/polym14163351.10.3390/polym14163351 ↗
46. 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.2025.140060.10.1016/j.ijbiomac.2025.140060 ↗
47. 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.2024.133576.10.1016/j.ijbiomac.2024.133576 ↗
48. 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/s11356-024-33780-2.10.1007/s11356-024-33780-2 ↗
49. 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.2008.06.008.10.1016/j.forsciint.2008.06.008 ↗
50. 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.2022.130778.10.1016/j.colsurfa.2022.130778 ↗
51. 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.10.1007/s12221-022-4470-z ↗
52. 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.2023.136445.10.1016/j.jclepro.2023.136445 ↗
53. 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.10.1039/C7RA09972J ↗
54. 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.10.1088/1361-6528/ad090c ↗
55. 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.