Home Alkali lignin as a pH response bifunctional material with both adsorption and flocculation for wastewater treatment
Article
Licensed
Unlicensed Requires Authentication

Alkali lignin as a pH response bifunctional material with both adsorption and flocculation for wastewater treatment

  • Junjie Qi , Yahui Hou , Jiaying Liu , Ze Yuan , Jing Fang EMAIL logo , Zhiqiang Fang and Hao Li ORCID logo EMAIL logo
Published/Copyright: October 19, 2022
Become an author with De Gruyter Brill

Abstract

Alkali lignin (AL) has attracted great attention as a material for treating dye wastewater due to its low cost and environmental friendliness. However, the unique structure and aggregation characteristics of AL regarding the dye wastewater removal mechanism have not been systematically revealed. Here, the removal process of typical cationic dye contaminants (methylene blue, MB) from dye wastewater by AL at different pH was explored and the unique synergistic effect mechanism of adsorption and flocculation was revealed. With increasing pH, the removal rate initially increased and then decrease. With increasing MB concentration, the optimal pH value corresponding to the maximum adsorption rate increased regularly. Zeta potential and Fourier transform infrared spectroscopy (FTIR) showed that electrostatic and π–π interactions and hydrogen bonding consisted push-pull balance under the influence of pH. In addition, scanning electron microscopy (SEM), ultraviolet and visible spectrum (UV) and particle size analysis showed that the aggregate structure and synergistic mechanism changed with the solution pH and concentration. In the low concentration solution, adsorption dominated. While in the high concentration solution, flocculation dominated. The removal mechanism consisted of the synergy of adsorption and flocculation laying the foundation for the efficient and environmentally friendly treatment of dye wastewater by AL.


Corresponding authors: Jing Fang and Hao Li, National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300401, China; and State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou 510640, China, E-mail: ,

Award Identifier / Grant number: B2021202012

Award Identifier / Grant number: 22272043

Award Identifier / Grant number: 22278110

Award Identifier / Grant number: 202210

Funding source: Tianjin Technical Innovation Guidance Special Project

Award Identifier / Grant number: 20YDTPJC00630

  1. Author contributions: All the authors have accepted responsibility for the entire content of this submitted manuscript and approved submission.

  2. Research funding: The work was supported by the National Natural Science Foundation of China (22278110, 22272043), Hebei Province Natural Science Foundation (B2021202012), Tianjin Technical Innovation Guidance Special Project (No. 20YDTPJC00630), State Key Laboratory of Pulp and Paper Engineering (202210).

  3. Conflict of interest statement: The authors declare that they have no conflicts of interest regarding this article.

References

Ai, Y., Liu, Y., Lan, W., Jin, J., Xing, J., Zou, Y., Zhao, C., and Wang, X. (2018). The effect of pH on the U (VI) sorption on graphene oxide (GO): a theoretical study. Chem. Eng. J. 343: 460–466, https://doi.org/10.1016/j.cej.2018.03.027.Search in Google Scholar

Al-Ghouti, M.A. and Da’ana, D.A. (2020). Guidelines for the use and interpretation of adsorption isotherm models: a review. J. Hazard Mater. 393: 122383, https://doi.org/10.1016/j.jhazmat.2020.122383.Search in Google Scholar PubMed

Alver, E., Metin, A.U., and Brouers, F. (2020). Methylene blue adsorption on magnetic alginate/rice husk bio-composite. Int. J. Biol. Macromol. 154: 104–113, https://doi.org/10.1016/j.ijbiomac.2020.02.330.Search in Google Scholar PubMed

Ando, D., Nakatsubo, F., and Yano, H. (2019). Thermal stability of lignin in ground pulp (GP) and the effect of lignin modification on GP’s thermal stability: TGA experiments with dimeric lignin model compounds and milled wood lignins. Holzforschung 73: 493–499, https://doi.org/10.1515/hf-2018-0137.Search in Google Scholar

Cao, K.L.A., Rahmatika, A.M., Kitamoto, Y., Nguyen, M.T.T., and Ogi, T. (2021). Controllable synthesis of spherical carbon particles transition from dense to hollow structure derived from kraft lignin. J. Colloid Interface Sci. 589: 252–263, https://doi.org/10.1016/j.jcis.2020.12.077.Search in Google Scholar PubMed

Chen, J., Kazzaz, A.E., Mazandarani, N.A., Feizi, Z.H., and Fatehi, P. (2018). Production of flocculants, adsorbents, and dispersants from lignin. Molecules 23: 868, https://doi.org/10.3390/molecules23040868.Search in Google Scholar PubMed PubMed Central

Kazzaz, A.E. and Fatehi, P. (2020). Fabrication of amphoteric lignin and its hydrophilicity/oleophilicity at oil/water interface. J. Colloid Interface Sci. 561: 231–243, https://doi.org/10.1016/j.jcis.2019.11.111.Search in Google Scholar PubMed

Florence, N. and Naorem, H. (2014). Dimerization of methylene blue in aqueous and mixed aqueous organic solvent: a spectroscopic study. J. Mol. Liq. 198: 255–258, https://doi.org/10.1016/j.molliq.2014.06.030.Search in Google Scholar

Fu, Y., Qian, Y., Zhang, A., Lou, H., Ouyang, X., Yang, D., and Qiu, X. (2022). Long-acting ultraviolet-blocking mechanism of lignin: generation and transformation of semiquinone radicals. ACS Sustain. Chem. Eng. 10: 5421–5429, https://doi.org/10.1021/acssuschemeng.1c08051.Search in Google Scholar

Gao, P., Chen, D., Chen, W., Sun, J., Wang, G., and Zhou, L. (2021). Facile synthesis of amine-crosslinked starch as an efficient biosorbent for adsorptive removal of anionic organic pollutants from water. Int. J. Biol. Macromol. 191: 1240–1248, https://doi.org/10.1016/j.ijbiomac.2021.09.206.Search in Google Scholar PubMed

Gonzales, R.R., Zhang, L., Sasaki, Y., Kushida, W., Matsuyama, H., and Shon, H.K. (2021). Facile development of comprehensively fouling-resistant reduced polyketone-based thin film composite forward osmosis membrane for treatment of oily wastewater. J. Membr. Sci. 626: 119185, https://doi.org/10.1016/j.memsci.2021.119185.Search in Google Scholar

Han, W., Rao, D., Gao, H., Yang, X., Fan, H., Li, C., Dong, L., and Meng, H. (2022). Green-solvent-processable biodegradable poly (lactic acid) nanofibrous membranes with bead-on-string structure for effective air filtration: “Kill two birds with one stone”. Nano Energy 97: 107237, https://doi.org/10.1016/j.nanoen.2022.107237.Search in Google Scholar

Hasan, A. and Fatehi, P. (2019). Flocculation of kaolin particles with cationic lignin polymers. Sci. Rep. 9: 2672, https://doi.org/10.1038/s41598-019-39135-z.Search in Google Scholar PubMed PubMed Central

He, W., Zhang, Y., and Fatehi, P. (2016). Sulfomethylated kraft lignin as a flocculant for cationic dye. Colloids Surf. A Physicochem. Eng. Asp. 503: 19–27, https://doi.org/10.1016/j.colsurfa.2016.05.009.Search in Google Scholar

Imam, S.S., Adnan, R., and Mohd Kaus, N.H. (2021). The photocatalytic potential of BiOBr for wastewater treatment: a mini-review. J. Environ. Eng. 9: 105404, https://doi.org/10.1016/j.jece.2021.105404.Search in Google Scholar

Jiang, M., Niu, N., and Chen, L. (2022). A template synthesized strategy on bentonite-doped lignin hydrogel spheres for organic dyes removal. Separ. Purif. Technol. 285: 120376, https://doi.org/10.1016/j.seppur.2021.120376.Search in Google Scholar

Li, H., Yuan, Z., Shang, X., Shang, H., Liu, J., Darwesh, O.M., Li, C., and Fang, J. (2021). Application of gradient acid fractionation protocol to improve decolorization technology by lignin-based adsorbent. Int. J. Biol. Macromol. 172: 10–18, https://doi.org/10.1016/j.ijbiomac.2020.12.206.Search in Google Scholar PubMed

Liu, X.J., Li, M.F., and Singh, S.K. (2021). Manganese-modified lignin biochar as adsorbent for removal of methylene blue. J. Mater. Res. Technol. 12: 1434–1445, https://doi.org/10.1016/j.jmrt.2021.03.076.Search in Google Scholar

Melro, E., Alves, L., Antunes, F.E., and Medronho, B. (2018). A brief overview on lignin dissolution. J. Mol. Liq. 265: 578–584, https://doi.org/10.1016/j.molliq.2018.06.021.Search in Google Scholar

Mimini, V., Kabrelian, V., Fackler, K., Hettegger, H., Potthast, A., and Rosenau, T. (2018). Lignin-based foams as insulation materials: a review. Holzforschung 73: 117–130, https://doi.org/10.1515/hf-2018-0111.Search in Google Scholar

Mimini, V., Amer, H., Hettegger, H., Bacher, M., Gebauer, I., Bischof, R., Fackler, K., Potthast, A., and Rosenau, T. (2020). Lignosulfonate-based polyurethane materials via cyclic carbonates: preparation and characterization. Holzforschung 74: 203–211, https://doi.org/10.1515/hf-2018-0298.Search in Google Scholar

Qiao, J., Jiao, W., and Liu, Y. (2021). Degradation of nitrobenzene-containing wastewater by sequential nanoscale zero valent iron-persulfate process. Green Energy Environ 6: 910–919, https://doi.org/10.1016/j.gee.2020.07.018.Search in Google Scholar

Rezakazemi, M. and Shirazian, S. (2019). Lignin-chitosan blend for methylene blue removal: adsorption modeling. J. Mol. Liq. 274: 778–791, https://doi.org/10.1016/j.molliq.2018.11.043.Search in Google Scholar

Shakoor, S. and Nasar, A. (2016). Removal of methylene blue dye from artificially contaminated water using citrus limetta peel waste as a very low cost adsorbent. J. Taiwan Inst. Chem. Eng. 66: 154–163, https://doi.org/10.1016/j.jtice.2016.06.009.Search in Google Scholar

Sherko Omer, N., Jamal Salih, S., and Sadiq Hawezy, H.J. (2019). Adsorptive behavior of medicinal product based activated carbon for pharmaceutical active compounds in aqueous solution. Redlich–Peterson studies. Orient. J. Chem. 35: 813–821, https://doi.org/10.13005/ojc/350244.Search in Google Scholar

Shi, Y., Song, G., Li, A., Wang, J., Wang, H., Sun, Y., and Ding, G. (2022). Graphene oxide-chitosan composite aerogel for adsorption of methyl orange and methylene blue: effect of pH in single and binary systems. Colloid. Surface. 641: 128595, https://doi.org/10.1016/j.colsurfa.2022.128595.Search in Google Scholar

Sun, Y., Liu, X., Lv, X., Wang, T., and Xue, B. (2021). Synthesis of novel lignosulfonate-modified graphene hydrogel for ultrahigh adsorption capacity of Cr (VI) from wastewater. J. Clean. Prod. 295: 126406, https://doi.org/10.1016/j.jclepro.2021.126406.Search in Google Scholar

Swenson, H. and Stadie, N.P. (2019). Langmuir’s theory of adsorption: a centennial review. Langmuir 35: 5409–5426, https://doi.org/10.1021/acs.langmuir.9b00154.Search in Google Scholar PubMed

Tafulo, P.A., Queiros, R.B., and Gonzalez-Aguilar, G. (2009). On the “concentration-driven” methylene blue dimerization. Spectrochim. Acta Mol. Biomol. Spectrosc. 73: 295–300, https://doi.org/10.1016/j.saa.2009.02.033.Search in Google Scholar PubMed

Uddin, M.K. (2017). A review on the adsorption of heavy metals by clay minerals, with special focus on the past decade. Chem. Eng. J. 308: 438–462, https://doi.org/10.1016/j.cej.2016.09.029.Search in Google Scholar

Wang, J., Qian, Y., Zhou, Y., Yang, D., and Qiu, X. (2021). Atomic force microscopy measurement in the lignosulfonate/inorganic silica system: from dispersion mechanism study to product design. Engineering 7: 1140–1148, https://doi.org/10.1016/j.eng.2021.07.004.Search in Google Scholar

Wu, F.C., Liu, B.L., Wu, K.T., and Tseng, R.L. (2010). A new linear form analysis of Redlich–Peterson isotherm equation for the adsorptions of dyes. Chem. Eng. J. 162: 21–27, https://doi.org/10.1016/j.cej.2010.03.006.Search in Google Scholar

Wurzer, G.K., Hettegger, H., Bischof, R.H., Fackler, K., Potthast, A., and Rosenau, T. (2022). Agricultural utilization of lignosulfonates. Holzforschung 76: 155–168, https://doi.org/10.1515/hf-2021-0114.Search in Google Scholar

Yadav, M. and Singh, N.K. (2017). Isotherm investigation for the sorption of fluoride onto bio-F: comparison of linear and non-linear regression method. Appl. Surf. Sci. 7: 4793–4800, https://doi.org/10.1007/s13201-017-0602-9.Search in Google Scholar

Yamauchi, F., Ito, T., Kawamoto, O., Komatsu, T., Akiyama, T., Yokoyama, T., and Matsumoto, Y. (2020). Effects of lignin structure and solvent on the formation rate of quinone methide under alkaline conditions. Holzforschung 74: 559–566, https://doi.org/10.1515/hf-2019-0269.Search in Google Scholar

Ying, T., Su, J., Jiang, Y., Ni, L., Jiang, X., Ke, Q., and Xu, H. (2022). Superhydrophobic MOFs decorated on hierarchically micro/nanofibrous membranes for high-performance emulsified oily wastewater separation and cationic dyes adsorption. J. Mater. Chem. A 10: 829–845, https://doi.org/10.1039/d1ta04982h.Search in Google Scholar

Zhang, A., Wu, X., Ouyang, X., Lou, H., Yang, D., Qian, Y., and Qiu, X. (2022). Preparation of light-colored lignosulfonate sunscreen microcapsules with strengthened UV-blocking and adhesion performance. ACS Sustain. Chem. Eng. 10: 9381–9388, https://doi.org/10.1021/acssuschemeng.2c01487.Search in Google Scholar

Zhou, Y., Yang, Z.H., Huang, J., Xu, R., Song, P.P., Zhang, Y.J., Li, J., and Aloun, M. (2017). Ni (II) removal from aqueous solution by biosorption and flocculation using microbial flocculant GA1. Res. Chem. Intermed. 43: 3939–3959, https://doi.org/10.1007/s11164-016-2845-8.Search in Google Scholar

Zhou, M., Xiong, Z., Yang, D., Pang, Y., Wang, D., and Qiu, X. (2018). Preparation of slow release nanopesticide microspheres from benzoyl lignin. Holzforschung 72: 599–607, https://doi.org/10.1515/hf-2017-0155.Search in Google Scholar


Supplementary Material

The online version of this article offers supplementary material (https://doi.org/10.1515/hf-2022-0117).


Received: 2022-07-11
Accepted: 2022-10-06
Published Online: 2022-10-19
Published in Print: 2022-12-16

© 2022 Walter de Gruyter GmbH, Berlin/Boston

Downloaded on 23.9.2025 from https://www.degruyterbrill.com/document/doi/10.1515/hf-2022-0117/html
Scroll to top button