Multi-interface interaction mechanism of pulp reject-based flocculants for the removal of antibiotics and its combined pollutants.

The efficient removal of antibiotics and its combined pollutants is essential for aquatic environment and human health. In this study, a lignin-based organic flocculant named PRL-VAc-DMC was synthesized using pulp reject as the raw material, with vinyl acetate (VAc) and methacryloxyethyltrimethyl ammonium chloride (DMC) as the grafting monomers. A series of modern characterization methods were used to confirm the successful preparation of PRL-VAc-DMC and elucidate its polymerization mechanism. It was found that the Ph-OH group and its contiguous carbon atoms of lignin served as the primary active sites to react with grafting monomers. Flocculation experiments revealed that PRL-VAc-DMC could react with tetracycline (TC) through π-π* interaction, hydrophobic interaction, hydrogen bonding, and electrostatic attraction. With the coexistence of humic acid (HA) and Kaolin, the aromatic ring, hydroxyl, and amide group of TC could react with the benzene ring, hydroxyl group, and carboxyl group of HA, forming TC@HA@Kaolin complexes with Kaolin particles acting as the hydrophilic shell. The increase in particle size, electronegativity, and hydrophily of TC@HA@Kaolin complexes facilitated their interaction with PRL-VAc-DMC through strong interfacial interactions. Consequently, the presence of HA and Kaolin promoted the removal of TC. The synergistic removal mechanism of TC, HA, and Kaolin by PRL-VAc-DMC was systematically analyzed from the perspective of muti-interface interactions. This paper is of great significance for the comprehensive utilization of pulp reject and provides new insights into the flocculation mechanism at the molecular scale.

Coagulation performance and mechanism of different hydrolyzed aluminum species for the removal of composite pollutants of polyethylene and humic acid.

Microplastics (MPs) and natural organic matter (NOM) composite pollutants have become emerging contaminants with potential threats. Coagulation has been widely used to remove MPs and NOM, but the underlying mechanisms for the removal of MPs-NOM composite pollutants by hydrolyzed Al species remain unclear. Therefore, the coagulation performance and mechanism of AlCl3, polyaluminum chloride with basicity of 2.2 (PAC22), and PAC25 in treating polyethylene (PE), humic acid (HA), and PE-HA composite systems were systematically investigated. The results showed that in the single PE system, PAC25 with hexagonal clusters achieved the maximum removal (68.09 %) (pH: 5, dosage: 0.5 mM) since adsorption bridging and sweeping effect were the main mechanisms for PE removal. The adsorption of HA on the PE surface enhanced its hydrophilicity and electrostatic repulsion, resulting in decreased PE removal. In the AlCl3-PE-HA system, the oligomeric Al first interacted with the -COOH and C-OH of HA through complexation, followed by the meso- and polymers of Al interacted with PE by electrostatic adsorption. The pre-formed medium polymeric Al species (Alb) and colloidal or solid Al species (Alc) in PAC22 and PAC25 formed complexes with the -OH and -COOH groups of HA, respectively, and then removed PE by adsorption bridging and sweeping effect.

Intrinsic mechanism for the removal of antibiotic pollution by a dual coagulation process from the perspective of the interaction between NOM and antibiotic.

Antibiotics bring potential risks to human health and ecosystem, and their coexistence with natural organic matters (NOMs) could have harmful impacts on the environment. Herein, a polyaluminium chloride (PAC)-polydimethyl diallyl ammonium chloride (PDMDAAC) dual coagulation process was designed to remove the co-pollutants of chlortetracycline (CTC) and humic acid (HA), representing antibiotics and NOMs, respectively. The main research strength was given to understand molecular interactions and their mechanisms associated with the coagulation and flocculation. We found that the co-existing HA and CTC increased the hydrophily and stability of contaminants, and generated HA@CTC complexes with large particles size. The interaction mechanism between CTC and HA was mainly hydrogen bonding, hydrophobic association action, n-π* electron donor-acceptor interaction, and π-π* conjugation. Lewis acid-base interaction was the main force between HA and CTC. The bonding energies of OH…N, OH…O, and hydrophobic association were -12.2 kcal/mol, -13.1 kcal/mol, and -11.4 kcal/mol, respectively, indicating that hydrogen bonding was stronger than hydrophobic association. The interactions between HA and CTC could improve their removal efficiency in the coagulation process. This is due to that the functional groups (COOH and OH) in the HA@CTC could be adsorbed by Al based hydrolysates. Polar interaction dominated the CTC and HA removal, and PAC was more efficient than PDMDAAC to remove HA@CTC complexes due to its higher complexing capacity. Thanks to the low concentration of residual contaminants and the formation of large and loose flocs, the interaction of HA and CTC could alleviate membrane fouling during ultrafiltration process. This study will provide new insight into the efficient removal of combined pollution and membrane fouling control.

Microcosmic mechanism analysis of the combined pollution of aged polystyrene with humic acid and its efficient removal by a composite coagulant.

The composite pollutants formed by aged polystyrene (APS) and natural organic matter are complex and harmful, which lead to the deterioration of water quality. In this work, the interaction mechanism between humic acid (HA) and APS was discussed by investigating the changes in their functional groups. Besides, a novel polyaluminum-titanium chloride composite coagulant (PATC) was prepared, and its binding behaviors with HA@APS under different pH conditions were analyzed from a microscopic perspective. It was found that at pH 4, π-π conjugation was the dominant interaction between HA and APS. And the main removal mechanism of HA@APS by PATC was surface complexation. With the increase of pH, π-π conjugation, n-π electron donor-acceptor interaction (EDA), and hydrogen bonding gradually dominated the interaction between APS and HA. At pH 7, PATC hydrolyzed to form various polynuclear Al-Ti species, which could meet the demand for different binding sites of HA@APS. Under alkaline conditions, HB and n-π EDA in HA@APS were weakened, while π-π conjugation held a dominant position again. At this time, the main coagulation mechanism of PATC changed from charge neutralization to sweeping action, accompanied by hydrogen bonding. ENVIRONMENTAL IMPLICATION: Microplastics (MPs) have attracted the public's attention due to their potential toxicity to humans. The combined pollution of aged microplastics and humic acid (HA) will bring great harm to aquatic environment. The development of novel composite coagulants is hopeful to efficiently remove MPs and their combined pollutants. Elucidating the interactions between HA and aged MPs is helpful to understand the transformation and fate of MPs in actual environments, and to reveal the removal mechanism of composite pollutants by coagulation. The findings presented here will provide theoretical guidance for addressing the challenges of coagulation technology in treating new pollutants in practice.

The suitability and mechanism of polyaluminum-titanium chloride composite coagulant (PATC) for polystyrene microplastic removal: Structural characterization and theoretical calculation.

Microplastics (MPs) particles bring potential threats to the aqueous environment, and the coexistence of natural organic matter (NOM) enhances their toxicity. Coagulation is an efficient method for particle removal and exploring the binding sites and modes of the coagulant hydrolysates with MPs in the presence of NOM is essential to understand the coagulation mechanism. In this study, a novel polymerized polyaluminum-titanium chloride composite coagulant (PATC) was prepared and used to remove polystyrene (PS). It was found that PATC could compress or even destroy the surface layer of the negatively charged PS. In comparison to PAC and PTC, PATC was more efficient in decreasing the energy barrier of the PS particles and increasing their aggregation rate over a wider pH range. The results of the Extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) calculation revealed that the interaction between the hydrolysates of PATC and PS was mainly polar interaction (VAB), such as hydrogen bonding. The peak intensity and peak shift in Fourier-transformed infrared (FTIR) and X-ray photoelectron spectra (XPS) were analyzed to further explore the interaction between the hydrolysates of PATC and PS. It was found that hydrogen bonding existed between the -OH group of PATC and the aliphatic C-H and C=O groups of PS. And the main interaction between HA and PS was the π-π* conjugation and hydrogen bonding between the -COOH, -OH, and C=O groups of HA and the C=O and aliphatic C-H groups of PS. Therefore, in the HA@PS system, the active sites of HA (e.g. -COOH and -OH) and PS (e.g., C=O and aliphatic C-H) binding with the coagulants were occupied, which accordingly led to the dramatic decline in the removal efficiency of both HA and PS. In actual lake water treatment, although the removal efficiency of PS was significantly poor, PATC performed better for PS removal than PAC and PTC. Besides, the effluent pH was maintained at 6.81±0.08, which met the requirements of the subsequent water treatment process. This study provides systematic knowledge for understanding the interaction between PS, NOM, and coagulant hydrolysates, and further confirms the application potential of PATC for MPs removal.

Pilot-scale advanced treatment of actual high-salt textile wastewater by a UV/O3 pressurization process: Evaluation of removal kinetics and reverse osmosis desalination process.

Advanced oxidation processes (AOPs) such as ozonation and Fenton processes are widely used in the treatment of high-salt wastewater. The UV/O3 pressurization process was designed and applied at the pilot-scale for treatment of actual high-salt textile wastewater. The UV/O3 pressurization process achieved the highest decolorization (85 %) and chemical oxygen demand (CODCr, 43.2 %) removal efficiency at an O3 dosage of 200 g·t-1 and a pressure of 0.2 MPa. Compared to ordinary ozonation, the UV/O3 pressurization process improved the solubility and gas-liquid mass transfer efficiency of O3 in wastewater and generated a large number of O3 microbubbles. Hydroxyl radical (·OH), superoxide radicals (O2·-) and single oxygen (1O2) all played a significant role on the removal of pollutants in wastewater during the UV/O3 pressurization process. The reverse osmosis (RO) process was used to evaluate the effect of UV/O3 pressurization and Fenton pre-oxidation processes on the desalination process as the last process in treating high-salt organic wastewater. The pre-oxidation processes improved the initial RO water flux. Compared with the Fenton process, the UV/O3 pressurization process had less membrane fouling (thin fouling layer vs thick fouling layer), and final water flux (59.4 LMH) was higher than that of Fenton process (34.9 LHM). The total dissolved solids (TDS), Cl- and SO42- of the effluent from UV/O3 pressurization process (37.2, 7.6 and 3.0 mg·L-1) were better than that of Fenton process (65.7, 13.9 and 7.1 mg·L-1). Therefore, the UV/O3 pressurization process without secondary pollution is more suitable for the advanced treatment of high-salt organic wastewater than the Fenton process.

Highly efficient Al-Ti gel as a coagulant for surface water treatment: Insights into the hydrolysate transformation and coagulation mechanism.

In view of the insufficient coagulation efficiency of traditional inorganic coagulants, a series of Al-Ti gels with different Ti/triethanolamine (TEA), Ti/H2O, and Ti/Al molar ratios were prepared by sol-gel process in this study. Fourier transform infrared (FTIR) spectra of the Al-Ti gels preliminarily confirmed the interaction between Al and Ti by detecting the appearance of the Al-O-Ti bond. The peak shift of the chemical bonds in X-ray photoelectron spectra (XPS) and the transformation of the hydrolysate species in the Al-Ti gels were analyzed to further explore the interaction mechanism between Al and Ti. It was found that moderate TEA could inhibit the hydrolysis of Ti precursors by taking up the coordination sites of H2O to form a CO-Ti bond. Density functional theory (DFT) calculation results showed that Ti could be incorporated into the framework of aluminum hydrolysates to form an Al-O-Ti bond, and [Al2Ti2(OH)x(TEA)y(H2O)8-x-y]14-x was the most possible copolymerization hydrolysate. Based on the above research results, the most efficient Al-Ti gel was selected and applied to the actual lake water treatment. The highest UV254 removal efficiency with the addition of Al-Ti gel was > 60%, nearly 25% higher than that of Ti gel. The hydrolysates of Al-Ti gel, such as TiO(OH)2(am), Al(OH)3(am), and [Al2Ti2(OH)x(TEA)y(H2O)8-x-y]14-x, could remove organic matters through the incorporation of charge neutralization, adsorption, complexation, and sweeping effects. These results provide a new idea for studying the interaction mechanism between Al and Ti in composite coagulants, and have theoretical guiding significance to actual water treatment.

Coagulation behavior of polyaluminum-titanium chloride composite coagulant with humic acid: A mechanism analysis.

The hydrolysate species of metal-based coagulants and the binding sites of humic acid (HA) are highly dependent on the pH conditions. Exploring the binding sites and modes between coagulant hydrolysates and HA molecules is critical to understanding the coagulation mechanism. In this paper, the binding behavior between HA molecules and the hydrolysates of a polyaluminum-titanium chloride composite coagulant (PATC) was investigated under different pH conditions by semi-quantitative FTIR and XPS. It was found that oligomeric and mesopolymeric hydrolysates were the dominant species under acid conditions, which could complex with the hydroxyl and carboxyl groups of HA by forming COAl/Ti coordinate bonds. However, large amounts of H+ could compete with Al3+ and weaken the removal efficiency of HA. With the increase of pH, the hydrolysis process of the PATC and the deprotonation of HA were simultaneously underway. Under weakly acid conditions, the complexation of the aluminum hydrolysates with carboxyl groups was improved due to the gradually diminishing competition of H+ and the enhanced charge neutralization of the further polymerized hydrolysates. Consequently, the maximum UV254 removal by adding PATC was observed at pH 6. Under alkaline conditions, the sweeping effect of amorphous hydroxide dominated the HA removals, which was accompanied by the surface complexation of Al/Ti nuclear with carboxyl groups as well as the hydrogen bonds between hydroxyl and hydroxide. This study provides a new clue for the interaction mechanisms between the hydrolysates of composite coagulants and the dominant functional groups of HA at various pH conditions.

Insights into selective adsorption mechanism of copper and zinc ions onto biogas residue-based adsorbent: Theoretical calculation and electronegativity difference.

Modified biomass-based adsorption technique has attracted much attention in heavy metal ions removal, but selective adsorption behavior and mechanism of heavy metal ions adsorption onto biosorbent still need to be further clarified. Herein, a carboxylated biogas residue (BR-COOH) was prepared to remove the Cu2+ and Zn2+ from single/binary heavy metal ions solution and explore selective adsorption mechanism. The results exhibited that the adsorption capacities of BR-COOH for Cu2+ was higher than that for Zn2+ obviously, whether in the single or binary heavy metal ions solution. Meanwhile, the introduced carboxy groups were identified as the main sites for metal ions adsorption. Density functional theory (DFT) calculation results exhibited that the adsorption energy of Cu2+ (-0.51 eV) onto BR-COOH was lower than that of Zn2+ (-0.47 eV), indicating that the Cu2+ adsorbed on BR-COOH was more stable than Zn2+. Moreover, the metal ions adsorption capacity of BR-COOH was positively correlated with their electronegativity, which was due to that the metal ions with stronger electronegativity was more easily interacted with the negatively charged oxygen in carboxyl groups. The same results were also verified in the control experiment conducted with two other biosorbents. Therefore, the work provided a new and in-depth insight into selective adsorption of metal ions onto carboxylated biosorbent.

Enhanced removal of phosphate using pomegranate peel-modified nickel­lanthanum hydroxide.

In this work, a bimetallic Ni/La nanoparticle-laded biosorbent was fabricated from pomegranate fibers by solvothermal synthesis method. The material exhibited a high-efficient phosphate removal capability. The results of the characterization analysis showed that the surface of pomegranate fibers was rough and evenly coated with Ni and La after modification, and the specific surface area of Ni-La@Peel increased to 50.20 m2/g, providing a large number of adsorption sites for phosphate removal. The maximum phosphate removal rate of adsorbent was higher than 97% in a wide pH range (3.7-10.8). The maximum adsorption capacities of Ni-La@Peel were 226.55 mg-P/g and 220.31 mg-P/g under alkaline and acidic conditions, respectively, as calculated using the Langmuir model. Meanwhile, all the results were consistent with the Langmuir isothermal (R2 = 0.99) and kinetic pseudo-second order models (R2 = 0.99), indicating that the phosphate removal mechanism of Ni-La@Peel was mainly related to homogeneous chemisorption. Experimental results showed that in the presence of other anions, such as chloride, sulfate, nitrate, bromide and fluoride, the adsorption capacity of phosphate was only reduced by about 10% compared to the blank sample individually. In addition, the phosphate removal efficiency of Ni-La@Peel remained 82.05% at 7th adsorption-desorption cycle. These findings show that Ni-La@Peel is a promising material for purification of phosphate-containing wastewater.

Coagulation-ultrafiltration integrated process for membrane fouling control: Influence of Al species and SUVA values of water.

Natural organic matter (NOM) pollution is a great challenge for the ultrafiltration (UF) process owing to the inevitable membrane fouling. In this study, three Al species coagulants (Ala/Alb/Alc) and their composites in combination with Poly dimethyl ammonium chloride (PolyDMDAAC) were used as a pretreatment strategy for the UF process. Then, test waters with different NOM fractions (i.e., humic acid, fulvic acid, protein, and polysaccharide) were prepared to analyze the effects of NOM characteristics on membrane fouling behaviors. The results indicated that compared with Alb and Alc, Ala showed higher removal efficiencies for hydrophobic NOM, aromatic organic matters, and suspended particles, but a limited effect on removing dissolved organic carbon (DOC). Ala or Ala-PolyDMDAAC effectively mitigated membrane fouling by removing the hydrophobic NOM in the coagulation process and forming the porous cake layer in the UF process. The test waters with higher specific ultraviolet absorbance (SUVA) resulted in more severe total and reversible membrane fouling but lighter irreversible fouling. After pretreatment by Ala or Ala-PolyDMDAAC, water samples with the medium SUVA value exhibited remarkable alleviation of membrane fouling due to the formation of large, compact, and robust flocs, as well as the construction of loose and poriferous cake layer on the membrane surface. Although hydrophilic NOM was challenging to be removed by coagulation, the interception and re-adsorption of porous cake layers contributed to the alleviation of irreversible fouling.

Recycling exhausted magnetic biochar with adsorbed Cu2+ as a cost-effective permonosulfate activator for norfloxacin degradation: Cu contribution and mechanism.

Herein, we attempted to apply an exhausted magnetic biochar with adsorbed Cu2+ (Cu-Fe@BRC) directly as a PMS activator and explored the feasibility of this attempt. Density functional theory (DFT) and electrochemical analysis illuminated the adsorbed Cu2+ in Cu-Fe@BRC improved PMS activation and NOR degradation efficiency by elevating the adsorption capacity of PMS and performance of electron transfer. About 91.47% of norfloxacin (NOR) was rapidly degraded in Cu-Fe@BRC/PMS system with low Fe and Cu leaching. An in-depth mechanistic study was conducted with radical scavenging, radical capturing and solvent exchange, which demonstrated that the adsorbed Cu2+ could facilitate the formation of both different radicals and non-radical. Importantly, Cu-Fe@BRC can maintain a long-term stable operation and excellent catalytic performance in surface water treatment. The potential toxicity of by-product generated in the NOR degradation process was also predicated, and results suggested that most identified by-products were less toxic than NOR itself. Notably, the preparation cost of exhausted adsorbent-based catalysts could be negligible, so the expenditure of the corresponding oxidation process is reduced accordingly. Based on above, this work provides not only a low-cost exhausted biochar-based catalyst for water purification but also the insight into the PMS activation by adsorbed transition metal ions.

Flocculation performance of papermaking sludge-based flocculants in different dye wastewater treatment: Comparison with commercial lignin and coagulants.

In this study, papermaking sludge-based flocculant (PSBF) and commercial lignin-based flocculant (LBF) have been synthesized by the same graft copolymerization procedures. The structures of alkaline lignin (AL), commercial lignin and the two flocculants were characterized by the modern analytical methods, also, the molecular weights and charge properties were analyzed. The effects of coagulant/flocculant dosages, pH conditions and coexistent dye auxiliaries on flocculation efficiencies were studied in the treatment of reactive turquoise blue (RTB) and disperse red (DR) dye wastewater. The flocculation experiments indicated that PSBF and LBF performed better in the removals of RTB and DR than commercial PAC and PAM. PSBF and LBF were insensitive to pH variation due to their strong charge neutralizing abilities and bridging effects even with the pH changing. In the existence of dye auxiliaries, PSBF and LBF could also exhibit superior decolorization efficiencies by slightly enlarging their dosages. Furthermore, PSBF and LBF had similar flocculation behaviors under all measured experimental conditions, suggesting that PSBF also had excellent flocculation performances even if it was prepared from papermaking sludge.

Synthesis, characterization and flocculation performance of a novel sodium alginate-based flocculant.

In this study, a natural polymer-based organic flocculant (sodium alginate-methacrylatoethyl trimethyl ammonium chloride, SA-PDMC) was synthesized by graft copolymerization. The optimum preparation procedures were determined by single factor experiments. The flocculation behaviors of SA-PDMC were investigated in humic acid (HA) and kaolin suspension considering the effects of flocculant doses and initial pH. The results indicated that charge neutralization and bridging action played an important role in the removals of HA and kaolin. Also, SA-PDMC performed well in a wide pH range of 5.0-10.0. Besides, SA-PDMC, as polyaluminium (PAC) aid, was investigated in the lake water treatment. The ratio of PAC and SA-PDMC was optimized through response surface methodology based on a central composite design. Results showed that SA-PDMC and PAC have a strong synergy, under optimal conditions SA-PDMC can reduce the dose of PAC by 40 % while ensuring the water quality.

Waste-to-resources: Green preparation of magnetic biogas residues-based biochar for effective heavy metal removals.

The agricultural wastes disposal and polluted water purification are always the key issues of environmental restoration. In this work, a magnetic biogas residue-based biochar (mBR-C) by direct pyrolysis and sonochemical method was prepared from biogas residue (BR). Response design methodology based on Box-Behnken design was used for the preparation parameters optimization. The characterization results identified that mBR-C had well-developed pore structure and surface area, which was beneficial to diffuse and capture heavy metal ions. Traces of toxic heavy metal in mBR-C was leached (˂0.04 mg/L) through TCLP method, indicating the environmental safety of the magnetic biochar. Meanwhile, the mBR-C exhibited excellent solid-liquid separation efficiency because of its strong magnetism. The series of adsorption experiments indicated that mBR-C could capture Cu2+ and Pb2+ rapidly, and the maximum adsorption capacity for Cu2+ and Pb2+ was 75.76 and 181.82 mg/g, respectively, which was higher than some other biochars previously reported. mBR-C was further applied in the synthetic wastewater treatment, which could effectively purify at least 600 mL (150 BV) to meet emission standards. After several column adsorption-desorption cycles, the adsorption capacity could still reach 85%, implying that mBR-C has good reusability and stability. Overall, the mBR-C can be used as an eco-friendly, desirable, economic and recyclable biosorbent in heavy metal polluted water treatment, providing a new idea for a combination of biogas residue recycle and wastewater treatment.

Effects of charge density and molecular weight of papermaking sludge-based flocculant on its decolorization efficiencies.

The charge densities (CD) and molecular weights (MW) of the flocculants are closely related to their application performances, but seldom researches focus on the effects of flocculant CD and MW on decolorization efficiencies. Herein, a series of flocculants with various CD and MW levels, named as PBF1-9, were designed and synthesized from papermaking sludge. The physicochemical characteristics of the PBF1-9 were measured by fourier transform infrared spectroscopy (FTIR), gel permeation chromatography (GPC), X-ray photoelectron spectroscopy (XPS) and particle charge density analyzer (PCD). The efficiencies of PBF1-9 were studied in the reactive blue (RB) dye removals by flocculation under different process conditions. The operation costs of the flocculants were evaluated at their optimal dosages. Also, the pH-independences and ion-tolerances of the aforementioned flocculants were studied in terms of the molecular levels. The experimental results exhibited that the flocculants CD or MW values were relevant to their flocculation behaviors and operation costs. CD values played a dominant role in color removal efficiencies and the costs, whereas MW values were critical to the floc structure. The pH or ion-independences of the flocculants were significantly dependent on the CD and MW values. However, some conclusions, conflicted with prior studies, were observed in this work. For instance, flocculant with the highest CD and MW levels was not the most effective one in enduring pH variation and the coexisting ions. The floc properties, including floc size, resistance and recovery ability, were relatively insensitive to flocculant intrinsic CD and MW levels when the flocculants were used at their optimal dosages. Furthermore, the possible relevance between CD or MW levels and the flocculation mechanisms have been proposed in this work. Exploring the effects of flocculants CD and MW levels could precisely control the flocculant characteristics to achieve satisfactory decontamination efficiencies with low costs.

Characterization and influence of floc under different coagulation systems on ultrafiltration membrane fouling.

A hybrid system was developed in this study consisting of different coagulation systems and ultrafiltration (UF). Property and effect of flocs formed in different coagulation systems on ultrafiltration membrane fouling control were investigated. All three coagulation systems, as pretreatment of UF, were effective in improving membrane flux and reducing membrane resistance within an appropriate range of natural organic matters (NOM) concentration. At high initial NOM concentration, the performance of polyaluminum chloride (PAC) on NOM removal and fouling control was severely limited. For PAC-poly dimethyl diallyl ammonium chloride (PAC-PolyDMDAAC) coagulation system, the limitation of initial NOM concentration on removing NOM and alleviating membrane fouling was slightly weakened, indicating composite flocculant PAC-PolyDMDAAC produced larger flocs through combined action of charge neutralization and adsorption bridging. In PAC + PolyDMDAAC dual coagulation system, the combined action of adsorption-bridging effect, sweeping effect, and charge neutralization were the mechanisms under both low and high initial NOM concentration. Although the flocs formed in PAC + PolyDMDAAC dual coagulation system had poor recovery ability compared with those formed in PAC and PAC-PolyDMDAAC coagulation system, flocs formed through adsorption-bridging and sweeping had large size and higher ability to resist shear force, resulting in the formation of cake layer with porous and fluffy structure and less blockage in membrane pore in PAC + PolyDMDAAC dual coagulation system. These results demonstrated that dual coagulation system combined PAC coagulation and PolyDMDAAC flocculation as a pretreatment of UF process can improve the characteristics of flocs and structure of cake layer for improving NOM removal and controlling membrane fouling.

PAC-PDMDAAC pretreatment of typical natural organic matter mixtures: Ultrafiltration membrane fouling control and mechanisms.

Precoagulation by polyaluminum chloride-poly dimethyl diallyl ammonium chloride (PAC-PDMDAAC) prior to ultrafiltration (UF) was conducted to evaluate the influence of PAC-PDMDAAC on controlling membrane fouling from typical natural organic matter (NOM) mixtures of humic acid (HA), bovine serum albumin (BSA) and sodium alginate (SA). Membrane flux decline and flux recovery after backwashing were investigated to evaluate the membrane fouling. The fouling mechanisms were determined from the floc size, floc structure and membrane resistance. PAC-PDMDAAC effectively alleviated membrane fouling caused by the HA, HA-BSA, HA-SA and HA-BSA-SA mixtures; furthermore, membrane fouling was better mitigated in the HA-SA and HA-BSA-SA mixtures. The untreated HA-SA and HA-BSA-SA mixtures caused much more serious total membrane resistance and fouling due to blocking and adsorption in the membrane pores by particles with sizes similar to those of the pores. The increased membrane flux and decreased irreversible resistance after the PAC-PDMDAAC pretreatment were attributed to the formation of flocs with a large size and small fractal dimension, which mainly formed a cake layer on the membrane surface. However, PAC-PDMDAAC was not particularly effective in reducing the irreversible membrane fouling originating from the HA and HA-BSA mixtures due to the formation of aggregates and pore blocking by microflocs.

Synthesis of polyaluminium chloride/papermaking sludge-based organic polymer composites for removal of disperse yellow and reactive blue by flocculation.

In this study, a series of polyaluminium chloride/papermaking sludge-based organic polymer (PAC-PSBF) composites with different PAC basicity and PAC/PSBF mass ratios were prepared from papermaking sludge. The basic properties of the aforementioned composites were characterized, and their flocculation efficiencies were studied in the disperse yellow (DY) and reactive blue (RB) dye removals. The results of the flocculation experiments demonstrated that PAC-PSBF composites performed better than PAC regardless of the PAC basicity or PAC/PSBF mass ratios. The composites with low PAC basicity were effective in DY and RB dye removals. PAC-PSBF composites with the same PAC basicity but higher PAC/PSBF mass ratios exerted more satisfactory color removals and floc properties in both DY and RB dye removals. PAC-PSBF composites were more pH-independent than PAC, and the excellent flocculation efficiencies of the composites was achieved at pH 4.0 to 8.0 in DY/RB dye removals. In brief, desirable flocculation efficiencies of the PAC-PSBF composites were obtained when PAC and PSBF were appropriately combined together.

Evaluation of molecular weight, chain architectures and charge densities of various lignin-based flocculants for dye wastewater treatment.

In this work, four alkaline lignin (AL) based flocculants with distinct molecular weight, chain architectures and charge densities (denoted as AL-g-DMC1, AL-g-DMC2, AL-GTA1 and AL-GTA2) were prepared from paper mill sludge, which were designed via graft copolymerization of dimethyl diallyl ammonium chloride (DMC) or etherification of 2, 3-epoxypropyl trimethyl ammonium chloride (GTA). The characteristics of the aforementioned flocculants were evaluated by a series of analysis technologies, which essentially confirmed the successful introduction of quaternary ammonium groups onto the AL. The flocculation performances of the four synthesized lignin-based polymers as the coagulant aids for PAC were investigated in disperse dye (DY) wastewater treatment, and the effects of dosages, initial pH, coexisting ions, humic acid (HA) or kaolin particles were also studied. The results indicated that branched copolymers with high molecular weight like AL-g-DMC1 and AL-g-DMC2 exerted excellent color removals and satisfactory floc properties in comparison with linear polymers with low molecular weight (AL-GTA1 and AL-GTA2). Furthermore, AL-g-DMC1 and AL-g-DMC2 exhibited remarkable tolerance on pH alteration and coexisting ions owing to their strong bridging action.