Register      Login
Environmental Chemistry Environmental Chemistry Society
Environmental problems - Chemical approaches
RESEARCH ARTICLE

Probing molecular interactions between humic acid and surface-grafted polyacrylamide using quartz crystal microbalance with dissipation and atomic force microscopy: implications for environmental remediation

Omar Maan A C , Jun Huang B C , Hongbo Zeng B and Qingye Lu https://orcid.org/0000-0002-4157-7602 A D
+ Author Affiliations
- Author Affiliations

A Department of Chemical and Petroleum Engineering, University of Calgary, Calgary, AB, T2N 1N4, Canada.

B Department of Chemical and Materials Engineering, University of Alberta, Edmonton, AB, T6G 2V4, Canada.

C These authors contributed equally to this work.

D Corresponding author. Email: qingye.lu@ucalgary.ca

Environmental Chemistry 15(6) 336-350 https://doi.org/10.1071/EN18079
Submitted: 10 April 2018  Accepted: 3 July 2018   Published: 20 August 2018

Environmental context. Polyacrylamide and its derivatives may enter the natural environment as a consequence of their wide use in various industrial applications. This study demonstrates the application of a quartz crystal microbalance and atomic force microscopy to study the molecular interactions between polyacrylamides and humic acids under various solution chemistries. The knowledge obtained can be used to understand and predict the environmental behaviour of polyacrylamides.

Abstract. A fundamental understanding of the environmental behaviour of polyacrylamide (PAM) is of importance for guiding environmental remediation. We create a framework for understanding the molecular interactions between PAM and a major constituent present in all natural waters and soil, humic acid (HA), using a quartz crystal microbalance with dissipation (QCM-D) and an atomic force microscope (AFM). A thin film of PAM was grafted on a silica surface silanised with 3-(trimethoxysilyl)propyl methacrylate and the resulting surface was characterised by X-ray photoelectron spectroscopy for the chemical bonds and composition, secondary ion mass spectrometry for the composition and molecular weight, water contact angle measurements for the hydrophilicity, AFM for the morphology, and ellipsometry for the thickness. Surface-grafted PAM was used to study its interactions with HA in aqueous solutions at different pH (2, 7, and 10) and NaCl salt concentrations (1, 10, and 100 mM, within the range of salt concentrations of fresh water) using QCM-D. QCM-D measurements showed that compared with bare silica, the adsorption of HA by PAM-coated silica was greatly reduced at all pHs and salt concentrations, and the adsorption of HA on PAM-coated silica depended on the solution chemistry including solution pH and salt concentration. Hydrogen bonding between PAM and HA is the major driving force for HA to adsorb on PAM. AFM force measurements showed that adhesion between PAM and HA was observed only at acidic conditions. The knowledge obtained from this study will benefit the prediction of the environmental behaviour of PAMs under different conditions in natural/engineered environments and provide guidance for the design of remediation technologies for water and soil.


References

Alagha L, Wang S, Xu Z, Masliyah J (2011). Adsorption kinetics of a novel organic-inorganic hybrid polymer on silica and alumina studied by quartz crystal microbalance. The Journal of Physical Chemistry C 115, 15390–15402.
Adsorption kinetics of a novel organic-inorganic hybrid polymer on silica and alumina studied by quartz crystal microbalanceCrossref | GoogleScholarGoogle Scholar |

Benninghoven A (1994). Chemical analysis of inorganic and organic surfaces and thin films by static time-of-flight secondary ion mass spectrometry (TOF-SIMS). Angewandte Chemie International Edition 33, 1023–1043.
Chemical analysis of inorganic and organic surfaces and thin films by static time-of-flight secondary ion mass spectrometry (TOF-SIMS)Crossref | GoogleScholarGoogle Scholar |

Bodnar J, Hajba L, Guttman A (2016). A fully automated linear polyacrylamide coating and regeneration method for capillary electrophoresis of proteins. Electrophoresis 37, 3154–3159.
A fully automated linear polyacrylamide coating and regeneration method for capillary electrophoresis of proteinsCrossref | GoogleScholarGoogle Scholar |

Bolto B, Dixon D, Eldridge R, King S (2001). Cationic polymer and clay or metal oxide combinations for natural organic matter removal. Water Research 35, 2669–2676.
Cationic polymer and clay or metal oxide combinations for natural organic matter removalCrossref | GoogleScholarGoogle Scholar |

Bressy C, Ngo VG, Ziarelli F, Margaillan A (2012). New insights into the adsorption of 3-(trimethoxysilyl)propylmethacrylate on hydroxylated ZnO nanopowders. Langmuir 28, 3290–3297.
New insights into the adsorption of 3-(trimethoxysilyl)propylmethacrylate on hydroxylated ZnO nanopowdersCrossref | GoogleScholarGoogle Scholar |

Buleva M, Petkanchin I (1999). Interaction of humic substances with silica and alumina colloids: adsorption and stability: electro-optical study. Colloids and Surfaces A: Physicochemical and Engineering Aspects 151, 225–231.
Interaction of humic substances with silica and alumina colloids: adsorption and stability: electro-optical studyCrossref | GoogleScholarGoogle Scholar |

Caulfield MJ, Qiao GG, Solomon DH (2002). Some aspects of the properties and degradation of polyacrylamides. Chemical Reviews 102, 3067–3084.
Some aspects of the properties and degradation of polyacrylamidesCrossref | GoogleScholarGoogle Scholar |

Colombo C, Palumbo G, Angelico R, Cho HG, Francioso O, Ertani A, Nardi S (2015). Spontaneous aggregation of humic acid observed with AFM at different pH. Chemosphere 138, 821–828.
Spontaneous aggregation of humic acid observed with AFM at different pHCrossref | GoogleScholarGoogle Scholar |

Cringus-Fundeanu I, Luijten J, van der Mei HC, Busscher HJ, Schouten AJ (2007). Synthesis and characterization of surface-grafted polyacrylamide brushes and their inhibition of microbial adhesion. Langmuir 23, 5120–5126.
Synthesis and characterization of surface-grafted polyacrylamide brushes and their inhibition of microbial adhesionCrossref | GoogleScholarGoogle Scholar |

Dixon MC (2008). Quartz crystal microbalance with dissipation monitoring: enabling real-time characterization of biological materials and their interactions. Journal of Biomolecular Techniques 19, 151–158.

Eita M (2011). In situ study of the adsorption of humic acid on the surface of aluminum oxide by QCM-D reveals novel features. Soft Matter 7, 709–715.
In situ study of the adsorption of humic acid on the surface of aluminum oxide by QCM-D reveals novel featuresCrossref | GoogleScholarGoogle Scholar |

Ekholm P, Blomberg E, Claesson P, Auflem IH, Sjoblom J, Kornfeldt A (2002). A quartz crystal microbalance study of the adsorption of asphaltenes and resins onto a hydrophilic surface. Journal of Colloid and Interface Science 247, 342–350.
A quartz crystal microbalance study of the adsorption of asphaltenes and resins onto a hydrophilic surfaceCrossref | GoogleScholarGoogle Scholar |

Elsner M, Hoelzer K (2016). Quantitative survey and structural classification of hydraulic fracturing chemicals reported in unconventional gas production. Environmental Science & Technology 50, 3290–3314.
Quantitative survey and structural classification of hydraulic fracturing chemicals reported in unconventional gas productionCrossref | GoogleScholarGoogle Scholar |

Ghosh K, Schnitzer M (1980). Macromolecular structures of humic substances. Soil Science 129, 266–276.
Macromolecular structures of humic substancesCrossref | GoogleScholarGoogle Scholar |

Guezennec AG, Michel C, Bru K, Touze S, Desroche N, Mnif I, Motelica-Heino M (2015). Transfer and degradation of polyacrylamide-based flocculants in hydrosystems: a review. Environmental Science and Pollution Research International 22, 6390–6406.
Transfer and degradation of polyacrylamide-based flocculants in hydrosystems: a reviewCrossref | GoogleScholarGoogle Scholar |

Harewood K, Wolff JS (1973). A rapid electrophoretic procedure for the detection of SDS-released oncorna-viral RNA using polyacrylamide-agarose gels. Analytical Biochemistry 55, 573–581.
A rapid electrophoretic procedure for the detection of SDS-released oncorna-viral RNA using polyacrylamide-agarose gelsCrossref | GoogleScholarGoogle Scholar |

Harkema S, Schäffer E, Morariu MD, Steiner U (2003). Pattern replication by confined dewetting. Langmuir 19, 9714–9718.
Pattern replication by confined dewettingCrossref | GoogleScholarGoogle Scholar |

Huang J, Liu X, Qiu X, Xie L, Yan B, Wang X, Huang Q, Zeng H (2017). Octadecyltrichlorosilane deposition on mica surfaces: insights into the interface interaction mechanism. The Journal of Physical Chemistry B 121, 3151–3161.
Octadecyltrichlorosilane deposition on mica surfaces: insights into the interface interaction mechanismCrossref | GoogleScholarGoogle Scholar |

Junqua G, Spinelli S, Gonzalez C (2015). Occurrence and fate of acrylamide in water-recycling systems and sludge in aggregate industries. Environmental Science and Pollution Research International 22, 6452–6460.
Occurrence and fate of acrylamide in water-recycling systems and sludge in aggregate industriesCrossref | GoogleScholarGoogle Scholar |

Laird DA (1997). Bonding between polyacrylamide and clay mineral surfaces. Soil Science 162, 826–832.
Bonding between polyacrylamide and clay mineral surfacesCrossref | GoogleScholarGoogle Scholar |

Lipczynska-Kochany E (2018). Humic substances, their microbial interactions and effects on biological transformations of organic pollutants in water and soil: A review. Chemosphere 202, 420–437.
Humic substances, their microbial interactions and effects on biological transformations of organic pollutants in water and soil: A reviewCrossref | GoogleScholarGoogle Scholar |

Liu Q, Singh A, Lalani R, Liu L (2012). Ultralow fouling polyacrylamide on gold surfaces via surface-initiated atom transfer radical polymerization. Biomacromolecules 13, 1086–1092.
Ultralow fouling polyacrylamide on gold surfaces via surface-initiated atom transfer radical polymerizationCrossref | GoogleScholarGoogle Scholar |

Lu Q, Hwang DS, Liu Y, Zeng H (2012). Molecular interactions of mussel protective coating protein, mcfp-1, from Mytilus californianus.. Biomaterials 33, 1903–1911.
Molecular interactions of mussel protective coating protein, mcfp-1, from Mytilus californianus.Crossref | GoogleScholarGoogle Scholar |

Lu Q, Huang J, Maan O, Liu Y, Zeng H (2017). Probing molecular interaction mechanisms of organic fouling on polyamide membrane using a surface forces apparatus: implication for wastewater treatment. The Science of the Total Environment 622–623, 644–654.

Lub J, Benninghoven A (1989). On the mechanism of secondary ion formation from poly(methylmethacrylate) under static secondary ion mass spectrometry conditions. Organic Mass Spectrometry 24, 164–168.
On the mechanism of secondary ion formation from poly(methylmethacrylate) under static secondary ion mass spectrometry conditionsCrossref | GoogleScholarGoogle Scholar |

Ma J, Fu K, Jiang L, Ding L, Guan Q, Zhang S, Zhang H, Shi J, Fu X (2017). Flocculation performance of cationic polyacrylamide with high cationic degree in humic acid synthetic water treatment and effect of kaolin particles. Separation and Purification Technology 181, 201–212.
Flocculation performance of cationic polyacrylamide with high cationic degree in humic acid synthetic water treatment and effect of kaolin particlesCrossref | GoogleScholarGoogle Scholar |

Munro JC, Frank CW (2004). Polyacrylamide adsorption from aqueous solutions on gold and silver surfaces monitored by the quartz crystal microbalance. Macromolecules 37, 925–938.
Polyacrylamide adsorption from aqueous solutions on gold and silver surfaces monitored by the quartz crystal microbalanceCrossref | GoogleScholarGoogle Scholar |

Naderi A, Claesson PM (2006). Adsorption properties of polyelectrolyte-surfactant complexes on hydrophobic surfaces studied by QCM-D. Langmuir 22, 7639–7645.
Adsorption properties of polyelectrolyte-surfactant complexes on hydrophobic surfaces studied by QCM-DCrossref | GoogleScholarGoogle Scholar |

Nagy G, Lu P, Walker AV (2008). An investigation of secondary ion yield enhancement using Bin2+ (n=1,3,5) primary ions. Journal of the American Society for Mass Spectrometry 19, 33–45.
An investigation of secondary ion yield enhancement using Bin2+ (n=1,3,5) primary ionsCrossref | GoogleScholarGoogle Scholar |

Parks GA (1965). The isoelectric points of solid oxides, solid hydroxides, and aqueous hydroxo complex systems. Chemical Reviews 65, 177–198.
The isoelectric points of solid oxides, solid hydroxides, and aqueous hydroxo complex systemsCrossref | GoogleScholarGoogle Scholar |

Penfold J, Staples E, Tucker I, Thomas RK (2002). Adsorption of mixed anionic and nonionic surfactants at the hydrophilic silicon surface. Langmuir 18, 5755–5760.
Adsorption of mixed anionic and nonionic surfactants at the hydrophilic silicon surfaceCrossref | GoogleScholarGoogle Scholar |

Penta NK, Dandu Veera PR, Babu SV (2011). Role of poly(diallyldimethylammonium chloride) in selective polishing of polysilicon over silicon dioxide and silicon nitride films. Langmuir 27, 3502–3510.
Role of poly(diallyldimethylammonium chloride) in selective polishing of polysilicon over silicon dioxide and silicon nitride filmsCrossref | GoogleScholarGoogle Scholar |

Penta NK, Amanapu HP, Peethala BC, Babu SV (2013). Use of anionic surfactants for selective polishing of silicon dioxide over silicon nitride films using colloidal silica-based slurries. Applied Surface Science 283, 986–992.
Use of anionic surfactants for selective polishing of silicon dioxide over silicon nitride films using colloidal silica-based slurriesCrossref | GoogleScholarGoogle Scholar |

Plaschke M, Römer J, Klenze R, Kim JI (1999). In situ AFM study of sorbed humic acid colloids at different pH. Colloids and Surfaces A: Physicochemical and Engineering Aspects 160, 269–279.
In situ AFM study of sorbed humic acid colloids at different pHCrossref | GoogleScholarGoogle Scholar |

Plaza I, Ontiveros-Ortega A, Calero J, Aranda V (2015). Implication of zeta potential and surface free energy in the description of agricultural soil quality: Effect of different cations and humic acids on degraded soils. Soil & Tillage Research 146, 148–158.
Implication of zeta potential and surface free energy in the description of agricultural soil quality: Effect of different cations and humic acids on degraded soilsCrossref | GoogleScholarGoogle Scholar |

Prado AGS, Pertusatti J, Nunes AR (2011). Aspects of protonation and deprotonation of humic acid surface on molecular conformation. Journal of the Brazilian Chemical Society 22, 1478–1483.
Aspects of protonation and deprotonation of humic acid surface on molecular conformationCrossref | GoogleScholarGoogle Scholar |

Ramazan KA, Wingen LM, Miller Y, Chaban GM, Gerber RB, Xantheas SS, Finlayson-Pitts BJ (2006). New experimental and theoretical approach to the heterogeneous hydrolysis of NO2: key role of molecular nitric acid and its complexes. The Journal of Physical Chemistry A 110, 6886–6897.
New experimental and theoretical approach to the heterogeneous hydrolysis of NO2: key role of molecular nitric acid and its complexesCrossref | GoogleScholarGoogle Scholar |

Steiner U (2005). Force measurements using capillary instabilities. Journal of Polymer Science. Part B, Polymer Physics 43, 3395–3405.
Force measurements using capillary instabilitiesCrossref | GoogleScholarGoogle Scholar |

Stringfellow WT, Domen JK, Camarillo MK, Sandelin WL, Borglin S (2014). Physical, chemical and biological characteristics of compounds used in hydraulic fracturing. Journal of Hazardous Materials 275, 37–54.
Physical, chemical and biological characteristics of compounds used in hydraulic fracturingCrossref | GoogleScholarGoogle Scholar |

Sun M, Qiao MX, Wang J, Zhai LF (2017). Free-radical induced chain degradation of high-molecular-weight polyacrylamide in a heterogeneous electro-Fenton system. ACS Sustainable Chemistry & Engineering 5, 7832–7839.
Free-radical induced chain degradation of high-molecular-weight polyacrylamide in a heterogeneous electro-Fenton systemCrossref | GoogleScholarGoogle Scholar |

Teng F, Liu Q, Zeng H (2012). In situ kinetic study of zinc sulfide activation using a quartz crystal microbalance with dissipation (QCM-D). Journal of Colloid and Interface Science 368, 512–520.
In situ kinetic study of zinc sulfide activation using a quartz crystal microbalance with dissipation (QCM-D)Crossref | GoogleScholarGoogle Scholar |

Valle-Delgado JJ, Molina-Bolivar JA, Galisteo-Gonzalez F, Galvez-Ruiz MJ, Feiler A, Rutland MW (2005). Hydration forces between silica surfaces: experimental data and predictions from different theories. The Journal of Chemical Physics 123, 034708
Hydration forces between silica surfaces: experimental data and predictions from different theoriesCrossref | GoogleScholarGoogle Scholar |

Wang Z, Zhao Y, Wang J, Wang S (2005). Studies on nanofiltration membrane fouling in the treatment of water solutions containing humic acids. Desalination 178, 171–178.
Studies on nanofiltration membrane fouling in the treatment of water solutions containing humic acidsCrossref | GoogleScholarGoogle Scholar |

Yoon S-H, Lee C-H, Kim K-J, Fane AG (1998). Effect of calcium ion on the fouling of nanofilter by humic acid in drinking water production. Water Research 32, 2180–2186.
Effect of calcium ion on the fouling of nanofilter by humic acid in drinking water productionCrossref | GoogleScholarGoogle Scholar |

Yuan W, Zydney AL (2000). Humic acid fouling during ultrafiltration. Environmental Science & Technology 34, 5043–5050.
Humic acid fouling during ultrafiltrationCrossref | GoogleScholarGoogle Scholar |

Zeng H, Maeda N, Chen N, Tirrell M, Israelachvili JN (2006a). Adhesion and friction of polystyrene surfaces around Tg. Macromolecules 39, 2350–2363.
Adhesion and friction of polystyrene surfaces around TgCrossref | GoogleScholarGoogle Scholar |

Zeng H, Tirrell M, Israelachvili JN (2006b). Limit cycles in dynamic adhesion and friction processes: a discussion. The Journal of Adhesion 82, 933–943.
Limit cycles in dynamic adhesion and friction processes: a discussionCrossref | GoogleScholarGoogle Scholar |

Zeng H, Pesika N, Tian Y, Zhao B, Chen Y, Tirrell M, Turner KL, Israelachvili JN (2009). Frictional adhesion of patterned surfaces and implications for gecko and biomimetic systems. Langmuir 25, 7486–7495.
Frictional adhesion of patterned surfaces and implications for gecko and biomimetic systemsCrossref | GoogleScholarGoogle Scholar |

Zeng H, Hwang DS, Israelachvili JN, Waite JH (2010a). Strong reversible Fe3+-mediated bridging between dopa-containing protein films in water. Proceedings of the National Academy of Sciences of the United States of America 107, 12850–12853.
Strong reversible Fe3+-mediated bridging between dopa-containing protein films in waterCrossref | GoogleScholarGoogle Scholar |

Zeng H, Zhao B, Israelachvili JN, Tirrell M (2010b). Liquid- to solid-like failure mechanism of thin polymer films at micro- and nanoscales. Macromolecules 43, 538–542.
Liquid- to solid-like failure mechanism of thin polymer films at micro- and nanoscalesCrossref | GoogleScholarGoogle Scholar |