Destabilization and Removal of Mixed Organic-Chromium Complexes from Leather Wastewater by Ultrasonic-Assisted Precipitation
Publication: Journal of Environmental Engineering
Volume 149, Issue 4
Abstract
During the leather tanning process, chromium (Cr) can interact with different macromolecular organics to generate mixed ligand complexes. The removal of organochromium complexes is one of the main difficulties in the treatment of tannery wastewater. In this study, a gelatin-gallic ac-id-Cr(III) (G-GA-Cr) mixed ligand complex was used to examine the effects of ultrasonic on chromium destabilization and removal from the dissolved complexes. To investigate organic destruction and chromium liberation, alkali precipitation or chelating precipitation assisted with ultrasound were conducted, respectively. The findings demonstrate that ultrasonic-assisted alkali precipitation and chelating precipitation, respectively, removed over 50% and 93% of Cr from the complexes. According to the data, ultrasonication weakened the bonds that bound macromolecular ligands together, and depolymerization took place to the point where Cr could interact directly with hydroxide ions or chelating agents. In addition, by applying ultrasonic-assisted chelating precipitation, the chromium concentration could meet the discharge standard and the amount of precipitation was also noticeably decreased.
Get full access to this article
View all available purchase options and get full access to this article.
Data Availability Statement
All data, models, or code that support the findings of this study are available from the corresponding author upon reasonable request.
Acknowledgments
Financial support for this research was issued by the National Natural Science Foundation of China (No. 22076113). The authors also thank the editor(s) and anonymous reviewer(s) for their constructive comments and suggestions.
References
Ayoub, G. M., A. Hamzeh, and L. Semerjian. 2011. “Post treatment of tannery wastewater using lime/bittern coagulation and activated carbon adsorption.” Desalination 273 (2–3): 359–365. https://doi.org/10.1016/j.desal.2011.01.045.
Bhunia, P., S. Chatterjee, P. Rudra, and S. De. 2018. “Chelating polyacrylonitrile beads for removal of lead and cadmium from wastewater.” Sep. Purif. Technol. 193 (Mar): 202–213. https://doi.org/10.1016/j.seppur.2017.11.001.
Bizzi, C. A., R. C. Zanatta, D. Santos, and S. De. 2020. “Ultrasound-assisted extraction of chromium from residual tanned leather: An innovative strategy for the reuse of waste in tanning industry.” Ultrason. Sonochem. 64 (Jun): 104682. https://doi.org/10.1016/j.ultsonch.2019.104682.
Cai, L., and H.-X. Zhou. 2011. “Theory and simulation on the kinetics of protein–ligand binding coupled to conformational change.” J. Chem. Phys. 134 (10): 105101. https://doi.org/10.1063/1.3561694.
Diehl, L. O., T. L. Gatiboni, P. A. Mello, E. I. Muller, F. A. Duarte, and E. M. Flores. 2018. “Ultrasound-assisted extraction of rare-earth elements from carbonatite rocks.” Ultrason. Sonochem. 40 (Part B): 24–29. https://doi.org/10.1016/j.ultsonch.2017.04.012.
Fukushima, M., K. Nakayasu, S. Tanaka, and H. Nakamura. 1995. “Chromium(III) binding abilities of humic acids.” Anal. Chim. Acta 317 (1–3): 195–206. https://doi.org/10.1016/0003-2670(95)00410-6.
Gao, X., C. Liu, C. Xiang, L. Yujie, D. Hongyu, and Y. Zhuowen. 2021. “Treatment of metals processing wastewater using pretreatment, Fenton oxidation, coagulation sedimentation and sand filtration process.” Chin. Technol. Water Treat. 47 (1): 130–133. https://doi.org/10.16796/j.cnki.1000-3770.2021.01.026.
Gustafsson, J. P., I. Persson, A. G. Oromieh, J. W. van Schaik, C. Sjöstedt, and D. B. Kleja. 2014. “Chromium (III) complexation to natural organic matter: Mechanisms and modeling.” Environ. Sci. Technol. 48 (3): 1753–1761. https://doi.org/10.1021/es404557e.
Hao, Y.-Y., H.-R. Ma, Q. Wang, C. Zhu, and A. He. 2022. “Complexation behaviour and removal of organic-Cr (III) complexes from the environment: A review.” Ecotoxicol. Environ. Saf. 240 (Jul): 113676. https://doi.org/10.1016/j.ecoenv.2022.113676.
He, L., C. Mu, J. Shi, Q. Zhang, B. Shi, and W. Lin. 2011. “Modification of collagen with a natural cross-linker, procyanidin.” Int. J. Biol. Macromol. 48 (2): 354–359. https://doi.org/10.1016/j.ijbiomac.2010.12.012.
Jaikumar, D., B. Baskaran, and V. G. Vaidyanathan. 2017. “Effect of chromium (III) gallate complex on stabilization of collagen.” Int. J. Biol. Macromol. 96 (Mar): 429–435. https://doi.org/10.1016/j.ijbiomac.2016.12.049.
Jaisson, S., C. Pietrement, and P. Gillery. 2018. “Protein carbamylation: Chemistry, pathophysiological involvement, and biomarkers.” Adv. Clin. Chem. 84 (Feb): 1–38. https://doi.org/10.1016/bs.acc.2017.12.001.
Kantar, C., H. Demiray, N. M. Dogan, and C. J. Dodge. 2011. “Role of microbial exopolymeric substances (EPS) on chromium sorption and transport in heterogeneous subsurface soils: I. Cr (III) complexation with EPS in aqueous solution.” Chemosphere 82 (10): 1489–1495. https://doi.org/10.1016/j.chemosphere.2011.01.009.
Khandegar, V., and A. K. Saroha. 2013. “Electrocoagulation for the treatment of textile industry effluent: A review.” J. Environ. Manage. 128 (Oct): 949–963. https://doi.org/10.1016/j.jenvman.2013.06.043.
Kurt, U., O. Apaydin, and M. T. Gonullu. 2007. “Reduction of COD in wastewater from an organized tannery industrial region by Electro-Fenton process.” J. Hazard. Mater. 143 (1–2): 33–40. https://doi.org/10.1016/j.jhazmat.2006.08.065.
Li, Q., G. Ji, Y. Tang, X. D. Gu, J. J. Fei, and H. Q. Jiang. 2012. “Ultrasound-assisted compatible in situ hydrolysis of sugarcane bagasse in cellulase-aqueouseN-methylmorpholine-N-oxide system for improved saccharification.” Bioresour. Technol. 107 (Mar): 251–257. https://doi.org/10.1016/j.biortech.2011.12.068.
Li, X. H., T. Guo, Y. Yu, and Y. Zhang. 2019. “Effects of ultrasound treatment on properties of gelatin from porcine skin.” Chin. Food Fermentat. Ind. 45 (6): 153–158. https://doi.org/10.13995/j.cnki.11-1802/ts.018211.
Liu, W., and Y. Yu. 2021. “Removal of recalcitrant trivalent chromium complexes from industrial wastewater under strict discharge standards.” Environ. Technol. Innovation 23 (Jul): 101644. https://doi.org/10.1016/j.eti.2021.101644.
Lofrano, G., S. Meriç, G. E. Zengin, and D. Orhon. 2013. “Chemical and biological treatment technologies for leather tannery chemicals and wastewaters: A review.” Sci. Total Environ. 461–462 (Sep): 265–281. https://doi.org/10.1016/j.scitotenv.2013.05.004.
Ma, H.-R., X.-J. Li, C. Zhu, F. Chen, Y. Yang, and X. Chen. 2020a. “Liberation and recovery of Cr from real tannery sludge by ultrasound-assisted supercritical water oxidation treatment.” J. Cleaner Prod. 267 (Sep): 122064. https://doi.org/10.1016/j.jclepro.2020.122064.
Ma, H.-R., Q. Wang, Y.-Y. Hao, C. Zhu, X. Chen, C. Wang, and Y. Yang. 2020b. “Fenton reaction induced in-situ redox and re-complexation of polyphenol-Cr complex and their products.” Chemosphere 250 (Jul): 126214. https://doi.org/10.1016/j.chemosphere.2020.126214.
Madhan, B., C. Muralidharan, and R. Jayakumar. 2002. “Study on the stabilisation of collagen with vegetable tannins in the presence of acrylic polymer.” Biomaterials 23 (14): 2841–2847. https://doi.org/10.1016/S0142-9612(01)00410-0.
Mohammadi, Z., S. Shangbin, C. Berkland, and J. T. Liang. 2017. “Chelator-mimetic multi-functionalized hydrogel: Highly efficient and reusable sorbent for Cd, Pb, and As removal from waste water.” Chem. Eng. J. 307 (Jan): 496–502. https://doi.org/10.1016/j.cej.2016.08.121.
Popiolski, A. S., R. M. Dallago, J. Steffens, M. L. Mignoni, L. D. Venquiaruto, D. Santos, and F. A. Duarte. 2018. “Ultrasound-assisted extraction of Cr from residual tannery leather: Feasibility of ethylenediaminetetraacetic acid as the extraction solution.” ACS Omega 3 (11): 16074–16080. https://doi.org/10.1021/acsomega.8b02241.
Puzon, G. J., A. G. Roberts, D. M. Kramer, and L. Xun. 2005. “Formation of soluble organo-chromium(III) complexes after chromate reduction in the presence of cellular organics.” Environ. Sci. Technol. 39 (8): 2811–2817. https://doi.org/10.1021/es048967g.
Qiang, T., L. Chen, Q. Zhang, and X. Liu. 2018. “A sustainable and cleaner speedy tanning system based on condensed tannins catalyzed by laccase.” J. Cleaner Prod. 197 (Part 1): 1117–1123. https://doi.org/10.1016/j.jclepro.2018.06.257.
Qiang, T.-T., Q. Bu, L. F. Ren, and X. Wang. 2014. “Adsorption behaviors of Cr (III) on carboxylated collagen fiber.” J. Appl. Polym. Sci. 131 (11): 40285. https://doi.org/10.1002/app.40285.
Rice, E. W. 2012. Standard methods for the examination of water and wastewater. Washington, DC: American Public Health Association.
Teh, C. Y., P. M. Budiman, K. P. Y. Shak, and T. Y. Wu. 2016. “Recent advancement of coagulation–flocculation and its application in wastewater treatment.” Ind. Eng. Chem. Res. 55 (16): 4363–4389. https://doi.org/10.1021/acs.iecr.5b04703.
Tyagi, V. K., S. L. Lo, L. Appels, and R. A. F. Dewil. 2014. “Ultrasonic treatment of waste sludge: A review on mechanisms and applications.” Crit. Rev. Environ. Sci. Technol. 44 (11): 1220–1288. https://doi.org/10.1080/10643389.2013.763587.
Vidal, C. M. P., W. Zhu, S. Manohar, B. Aydin, T. A. Keiderling, P. B. Messersmith, and A. K. Bedran-Russo. 2016. “Collagen-collagen interactions mediated by plant-derived proanthocyanidins: A spectroscopic and atomic force microscopy study.” Acta Biomater. 41 (Sep): 110–118. https://doi.org/10.1016/j.actbio.2016.05.026.
Wang, D.-D., S. He, C. Shan, Y. Ye, H. Ma, X. Zhang, W. Zhang, and B. Pan. 2016. “Chromium speciation in tannery effluent after alkaline precipitation: Isolation and characterization.” J. Hazard. Mater. 316 (Oct): 169–177. https://doi.org/10.1016/j.jhazmat.2016.05.021.
Wang, D.-D., Y.-X. Ye, H. Liu, H. Ma, and W. Zhang. 2018. “Effect of alkaline precipitation on Cr species of Cr (III)-bearing complexes typically used in the tannery industry.” Chemosphere 193 (Feb): 42–49. https://doi.org/10.1016/j.chemosphere.2017.11.006.
Wang, Q., J. Chen, A. Zheng, and L. Shi. 2019. “Dechelation of Cd-EDTA complex and recovery of EDTA from simulated soil-washing solution with sodium sulfide.” Chemosphere 220 (Apr): 1200–1207. https://doi.org/10.1016/j.chemosphere.2018.12.212.
Wang, Y., and L. Jin. 2018. “A reconsideration of the effect of procyanidin on the assembly of collagen type I.” BioRxiv 8 (Jul): 372847. https://doi.org/10.1101/372847.
Xiao, R., D. Diaz-Rivera, and L. K. Weavers. 2013. “Factors influencing pharmaceutical and personal care product degradation in aqueous solution using pulsed wave ultrasonic.” Ind. Eng. Chem. Res. 52 (8): 2824–2831. https://doi.org/10.1021/ie303052a.
Xiao, R., Z. Wei, D. Chen, and L. K. Weavers. 2014. “Kinetics and mechanism of sonochemical degradation of pharmaceuticals in municipal wastewater.” Environ. Sci. Technol. 48 (16): 9675–9683. https://doi.org/10.1021/es5016197.
Xie, Q., G. Liang, T. Lin, F. Chen, D. Wang, and B. Yang. 2020. “Selective chelating precipitation of palladium metal from electroplating wastewater using chitosan and its derivative.” Adsorpt. Sci. Technol. 38 (3–4): 113–126. https://doi.org/10.1177/0263617420918729.
Yang, L., J. F. Rathman, and L. K. Weavers. 2005. “Degradation of alkylbenzene sulfonate surfactants by pulsed ultrasonic.” J. Phys. Chem. B 109 (33): 16203–16209. https://doi.org/10.1021/jp0523221.
Yuan, H.-N., J.-M. Lv, J.-Y. Gong, G. Xiao, R. Zhu, L. Li, and J. Qiu. 2018. “Secondary structures and their effects on antioxidant capacity of antioxidant peptides in yogurt.” Int. J. Food Prop. 21 (1): 2167–2180. https://doi.org/10.1080/10942912.2018.1501700.
Yuan, Y., J. Li, L. Fu, and F. Liu. 2019. “Development and prospect of heavy metal-organic acid complex wastewater treatment technology.” Chin. Environ. Sci. Technol. 42 (8): 76–85. https://doi.org/10.19672/j.cnki.1003-6504.2019.08.012.
Zhang, Y., L. Ma, L. Cai, Y. Liu, and J. Li. 2017. “Effect of combined ultrasonic and alkali pretreatment on enzymatic preparation of angiotensin converting enzyme (ACE) inhibitory peptides from native collagenous materials.” Ultrason. Sonochem. 36 (May): 88–94. https://doi.org/10.1016/j.ultsonch.2016.11.008.
Zhu, C., H. Q. Wang, H.-R. Ma, Y. Yang, and F. Li. 2020. “Tanning process promotes abiotic humification: Separation and characterization of humic acid-like polymers complex.” Environ. Sci. Pollut. Res. 27 (33): 41437–41445. https://doi.org/10.1007/s11356-020-10111-9.
Information & Authors
Information
Published In
Journal of Environmental Engineering
Volume 149 • Issue 4 • April 2023
Copyright
© 2023 American Society of Civil Engineers.
History
Received: Sep 26, 2022
Accepted: Nov 30, 2022
Published online: Jan 24, 2023
Published in print: Apr 1, 2023
Discussion open until: Jun 24, 2023
ASCE Technical Topics:
- Alkalinity and acidity
- Chemical compounds
- Chemical elements
- Chemical properties
- Chemicals
- Chemistry
- Chromium
- Climates
- Engineering fundamentals
- Environmental engineering
- Field tests
- Heavy metals
- Industrial wastes
- Meteorology
- Nondestructive tests
- Pollutants
- Precipitation
- Solid wastes
- Tests (by type)
- Wastes
- Wastewater management
- Wastewater treatment
- Water treatment
Authors
Metrics & Citations
Metrics
Citations
Download citation
If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.