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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

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Front. Environ. Sci. Eng.    2021, Vol. 15 Issue (1) : 9    https://doi.org/10.1007/s11783-020-1301-6
RESEARCH ARTICLE
Forward osmosis coupled with lime-soda ash softening for volume minimization of reverse osmosis concentrate and CaCO3 recovery: A case study on the coal chemical industry
Jiandong Lu, Shijie You, Xiuheng Wang()
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
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Abstract

• Forward osmosis (FO) coupled with chemical softening for CCI ROC minimization

• Effective removal of scale precursor ions by lime-soda ash softening

• Enhanced water recovery from 54% to 86% by mitigation of FO membrane scaling

• High-purity CaCO3 was recovered from the softening sludge

• Membrane cleaning efficiency of 88.5% was obtained by EDTA for softened ROC

Reverse osmosis (RO) is frequently used for water reclamation from treated wastewater or desalination plants. The RO concentrate (ROC) produced from the coal chemical industry (CCI) generally contains refractory organic pollutants and extremely high-concentration inorganic salts with a dissolved solids content of more than 20 g/L contributed by inorganic ions, such as Na+, Ca2+, Mg2+, Cl−, and SO42−. To address this issue, in this study, we focused on coupling forward osmosis (FO) with chemical softening (FO-CS) for the volume minimization of CCI ROC and the recovery of valuable resources in the form of CaCO3. In the case of the real raw CCI ROC, softening treatment by lime-soda ash was shown to effectively remove Ca2+/Ba2+ (>98.5%) and Mg2+/Sr2+/Si (>80%), as well as significantly mitigate membrane scaling during FO. The softened ROC and raw ROC corresponded to a maximum water recovery of 86% and 54%, respectively. During cyclic FO tests (4 × 10 h), a 27% decline in the water flux was observed for raw ROC, whereas only 4% was observed for softened ROC. The cleaning efficiency using EDTA was also found to be considerably higher for softened ROC (88.5%) than that for raw ROC (49.0%). In addition, CaCO3 (92.2% purity) was recovered from the softening sludge with an average yield of 5.6 kg/m3 treated ROC. This study provides a proof-of-concept demonstration of the FO-CS coupling process for ROC volume minimization and valuable resources recovery, which makes the treatment of CCI ROC more efficient and more economical.
Keywords Coal chemical industry      Forward osmosis      Chemical softening      Reverse osmosis concentrate     
Corresponding Author(s): Xiuheng Wang   
Issue Date: 30 July 2020
 Cite this article:   
Jiandong Lu,Shijie You,Xiuheng Wang. Forward osmosis coupled with lime-soda ash softening for volume minimization of reverse osmosis concentrate and CaCO3 recovery: A case study on the coal chemical industry[J]. Front. Environ. Sci. Eng., 2021, 15(1): 9.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1301-6
https://academic.hep.com.cn/fese/EN/Y2021/V15/I1/9
Fig.1  (a) Conventional and (b) proposed treatment for the CCI wastewaters (mixed wastewater and saline wastewater). Normally, CCI ROC goes through a concentrator, a crystallizer and then a disposal process or a salt recovery process. Alternatively, the volume of CCI ROC could first be reduced by the FO-CS hybrid process, and the concentrated FS exiting FO will then go to (I) a compressed concentrator or directly to (II) a crystallizer or (III) the final disposal depending on the recovery rate of the FO process.
Parameter Value
pH 7.18
Alkalinity as CaCO3 (mg/L) 421
TOC (mg/L) 59.35
TDS (mg/L) 20800
Na+ (mg/L) 4895
Ca2+ (mg/L) 1430
Mg2+ (mg/L) 181.4
K+ (mg/L) 40.81
Sr2+ (mg/L) 10.63
Ba2+ (mg/L) 1.19
Fe2+/Fe3+ (mg/L) 0.345
Al3+ (mg/L) 0.21
Cl− (mg/L) 9184
SO42− (mg/L) 1758
NO3− (mg/L) 70.67
SiO2 (mg/L) 54.3
Osmotic pressure (bar) 4.8
Tab.1  Major water quality parameters of CCI ROC
Fig.2  Comparison of the FO performance between softened and raw ROC. (a) Maximum recovery experiments and (b) cyclic experiments. NaCl solution (1000 mL, 4 mol/L) and raw/softened ROC (500 mL) were used as DS and FS, respectively.
Major species Mean (mg/L) Standard deviation (mg/L) Removal rate (%)
Ca2+ 16.20 3.40 98.9
Mg2+ 27.88 0.85 84.6
Si 3.50 0.26 86.2
Sr2+ 1.98 0.21 81.3
Ba2+ 0.015 0.004 98.7
TOC 51.48 1.44 13.3
Tab.2  Concentration and removal rate of the major scale precursor ions after the chemical softening process
Fig.3  Saturation index (SI) of (a) barite (Ba) and calcite (Ca), (b) celestite (Ce), gypsum (Gy) and amorphous silica (Si). R and S represent raw ROC and softened ROC, respectively. The dash lines are the saturation lines with the SI value of 1. pKsp (25°C) of barite, calcite, celestite, gypsum and amorphous silica are 9.98, 8.48, 6.62, 4.61, and 2.71, respectively, which are obtained from the Visual MINTEQ software.
Fig.4  Comparison of (a) FTIR spectra and (b) XRD pattern between the pure CaCO3 and the chemical sludge obtained after the lime-soda ash softening of ROC. The blue square highlights the absorbance bands of the chemical sludge ranging from 1000 to 1100 cm-1.
Fig.5  (a-c) SEM images and EDS results of the chemical sludge after the lime-soda ash softening (samples taken from three independent softening processes).
Fig.6  SEM images of (a) the new membrane, (b) the membrane after FO using raw ROC, (c) the relatively fouled part and (d) the relatively clean part of the membrane after FO using softened ROC. The insets show the corresponding membrane images and the atomic percentages (At%).
Fig.7  FTIR spectra of the new membrane and the membranes after FO using softened/raw ROC as FS. The FTIR results with softened ROC include both the relatively clean (c) part and the relatively fouled (f) part.
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