Ozonation as an efficient pretreatment method to alleviate reverse osmosis membrane fouling caused by complexes of humic acid and calcium ion

doi:10.1007/s11783-019-1139-y

Front. Environ. Sci. Eng.

2019, Vol. 13

Issue (4) : 55 https://doi.org/10.1007/s11783-019-1139-y

RESEARCH ARTICLE

Ozonation as an efficient pretreatment method to alleviate reverse osmosis membrane fouling caused by complexes of humic acid and calcium ion

Xuehao Zhao¹, Yinhu Wu¹(

), Xue Zhang², Xin Tong¹, Tong Yu¹, Yunhong Wang¹, Nozomu Ikuno³, Kazuki Ishii³, Hongying Hu^1,⁴(

)

¹. Environmental Simulation and Pollution Control State Key Joint Laboratory, State Environmental Protection Key Laboratory of Microorganism Application and Risk Control (SMARC), School of Environment, Tsinghua University, Beijing 100084, China
². Collaborative Innovation Center for Advanced Nuclear Energy Technology, Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China
³. Kurita Water Industries Ltd., Nakano-ku, Tokyo 164-0001, Japan
⁴. Shenzhen Environmental Science and New Energy Technology Engineering Laboratory, Tsinghua-Berkeley Shenzhen Institute, Shenzhen 518055, China

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Abstract

Humic acids (HA) didn’t cause obvious reverse osmosis (RO) membrane fouling in 45 h.

Osmotic pressure (NaCl) affected slightly the RO membrane fouling behavior of HA.

Ca²⁺ promoted aggregation of HA molecules and thus aggravated RO membrane fouling.

Ozonation eliminated the effect of Ca²⁺ on the RO membrane fouling behavior of HA.

The change of the structure of HA was related to its membrane fouling behavior.

Humic acid has been considered as one of the most significant sources in feed water causing organic fouling of reverse osmosis (RO) membranes, but the relationship between the fouling behavior of humic acid and the change of its molecular structure has not been well developed yet. In this study, the RO membrane fouling behavior of humic acid was studied systematically with ozonation as a pretreatment method to control RO membrane fouling. Furthermore, the effect of ozone on the structure of humic acid was also explored to reveal the mechanisms. Humic acid alone (10–90 mg/L, in deionized water) was found not to cause obvious RO membrane fouling in 45-h operation. However, the presence of Ca²⁺ aggravated significantly the RO membrane fouling caused by humic acid, with significant flux reduction and denser fouling layer on RO membrane, as it was observed by scanning electron microscope (SEM) and atomic force microscope (AFM). However, after the pretreatment by ozone, the influence of Ca²⁺ was almost eliminated. Further analysis revealed that the addition of Ca²⁺ increased the particle size of humic acid solution significantly, while ozonation reduced the SUVA₂₅₄, particle size and molecular weight of the complexes of humic acid and Ca²⁺ (HA-Ca²⁺ complexes). According to these results and literature, the bridge effect of Ca²⁺ aggregating humic acid molecules and the cleavage effect of ozone breaking HA-Ca²⁺ complexes were summarized. The change of the structure of humic acid under the effect of Ca²⁺ and ozone is closely related to the change of its membrane fouling behavior.

Keywords Reverse osmosis Membrane fouling Humic acid Ca²⁺ Ozone

Corresponding Author(s): Yinhu Wu,Hongying Hu

Issue Date: 15 May 2019

Cite this article:

Xuehao Zhao,Yinhu Wu,Xue Zhang, et al. Ozonation as an efficient pretreatment method to alleviate reverse osmosis membrane fouling caused by complexes of humic acid and calcium ion[J]. Front. Environ. Sci. Eng., 2019, 13(4): 55.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-019-1139-y
https://academic.hep.com.cn/fese/EN/Y2019/V13/I4/55

Fig.1 Schematic diagram of the RO cross-flow apparatus.

Fig.2 (a) RO flux change with different humic acid concentrations. Experimental conditions: DI water. (b1) RO flux profiles at the initial first hour of the experiment; (b2) Flux change during the whole experimental period. Experimental conditions: ionic strength of 30 mmol/L. (c) RO flux change at the initial first hour with/without 10 mg/L humic acid at different ionic strengths; (d) RO flux variation during the whole experimental period. Experimental conditions: NaCl solutions with the ionic strength of 10, 30 and 50 mmol/L. (e) System filtration resistance at different humic acid concentration under ionic strength of 30 mmol/L. (f) System filtration resistance of 10 mg/L humic acid at different ionic strength.

Fig.3 (a) RO flux change with humic acid and different Ca²⁺ concentration. Experimental conditions: 10 mg/L humic acid with total ionic strength 30 mmol/L. (b) System filtration resistance at different Ca²⁺ concentration. (c) Original flux profiles of the RO membrane with 10 mg/L humic acid and 1,3, 5 mmol/L Ca²⁺; —: fitting lines of the intermediate blocking model.

Tab.1 Model fitting results of J_pss and k

Fig.4 (a) RO flux change with humic acid (10 mg/L) and different concentrations of Ca²⁺ treated by ozone (10 mg/L). Experimental conditions: ionic strength 30 mmol/L. (b) System filtration resistance of humic acid with different concentrations of Ca²⁺ treated by ozone.

Fig.5 Original and SEM images of RO membrane. (a) clean membrane. (b) to (d) membranes fouled by 10 mg/L humic acid solutions without Ca²⁺, with 1 mmol/L Ca²⁺ and 5 mmol/L Ca²⁺. (e) to (f) membranes fouled by 10 mg/L humic acid solutions with 1 mmol/L Ca²⁺ and 5 mmol/L Ca²⁺ after pretreatment by ozone.

Fig.6 AFM images of RO membrane. (a) clean membrane. (b) to (d) membranes fouled by 10 mg/L humic acid solutions without Ca²⁺, with 1 mmol/L Ca²⁺ and 5 mmol/L Ca²⁺. (e) to (f) membranes fouled by 10 mg/L humic acid solutions with 1 mmol/L Ca²⁺ and 5 mmol/L Ca²⁺ after ozone pretreatment.

Tab.2 Roughness and hydrophilicity of clean and fouled RO membranes

Fig.7 The effects of Ca²⁺ and ozone on the (a) SUVA₂₅₄, (b) particle size and (c) molecular weight distribution of humic acid solution.

Fig.8 Proposed mechanism of the influence of Ca²⁺ and ozone on the structure of humic acid (modified from ^{Matilainen et al. (2010)}; ^{Kalinichev et al. (2011)}; ^{Wenk et al. (2013})).

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