Catalysis Today 193 (2012) 120–127
Contents lists available at SciVerse ScienceDirect
Catalysis Today
j ourna l ho me p ag e: www.elsevier.com/lo cate/cattod
Experiment and modeling of advanced ozone membrane reactor for treatment of
organic endocrine disrupting pollutants in water
Hung Lai Ho
a
, Wai Kit Chan
a
, Angelique Blondy
a
, King Lun Yeung
a,b,∗
, Jean-Christophe Schrotter
c
a
Department of Chemical and Biomolecular Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
b
Division of Environment, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
c
Water Research Center of Veolia, Anjou Recherche, Chemin de la Digue, BP 76. 78603, Maisons Laffitte, Cedex, France
a r t i c l e i n f o
Article history:
Received 19 October 2011
Received in revised form 15 February 2012
Accepted 28 March 2012
Available online 12 May 2012
Keywords:
Water and wastewater treatment
Ozonation reaction
Phthalate
Nanofiltration membrane
Zeolite membrane
a b s t r a c t
An advanced ozone membrane reactor that uses membranes for ozone distribution, reaction contact and
selective water separation was used for ozone treatment of a recalcitrant endocrine disrupting compound
in water. Experiments and model calculation were employed to examine the ozonation of phthalate
in the new reactor. Experimental results showed that fast ozone mass transfer rate is responsible for
membrane reactor’s superb performance compared with a semibatch reactor. Selective water removal
further enhanced phthalate conversion and TOC removal by concentrating the pollutants in the reaction
zone. Clean water was produced by membrane separation. Mathematical model was used to investigate
the effect of membranes, reactor design and reaction operation on pollutant conversion and removal.
© 2012 Elsevier B.V. All rights reserved.
1. Introduction
There is growing evidence that a large number of chemical
compounds found in common household products ranging from
medicines, cosmetics and personal care products, and household
cleansers, can survive state-of-the-art wastewater treatment pro-
cesses to contaminate surface and ground waters [1–10]. Many
of these compounds are endocrine disruptors and studies carried
out in 2001 [11] and 2003 [12] showed that a large numbers of
endocrine disrupting chemicals (EDCs) survive conventional drink-
ing water treatment processes to persist in finished, potable water.
Several of the compounds were even found in samples of human
blood, milk and urine [13]. Although health risk from chronic expo-
sure to EDCs in humans has not been adequately addressed, their
effects on normal hormonal processes is well documented and
there is extensive evidence of their adverse effects in wildlife [14].
It is particularly disturbing that most studies in animal models [15]
showed that early life stages are the most vulnerable to the actions
of EDCs, putting pregnant women and children at greater risk
[16].
∗
Corresponding author at: Department of Chemical and Biomolecular Engineer-
ing, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon,
Hong Kong. Tel.: +852 23587123; fax: +852 23580054.
E-mail address: kekyeung@ust.hk (K.L. Yeung).
Ozone and membrane processes are technologies that showed
the best promise for treatment of EDCs in water [17,18]. How-
ever, ozone treatment alone suffered from slow mineralization
rates [19] and the UV/O
3
and O
3
/H
2
O
2
used by various authors
[20–22] to remedy this shortcoming are often expensive and com-
plex. Nanofiltration and reverse osmosis membrane can remove
most EDCs [23,24], but the separated EDCs require further treat-
ment. In addition, membrane fouling is a concern [25]. Ozone has
been used in membrane to alleviate membrane fouling by organic
matters [26,27] and improves membrane filtration processes [28].
Shanbhag et al. [29] explored in their early work the use of a sil-
icone capillary membrane for ozone distributor for treatment of
chemical micropollutants in water. More recently Karnik et al.
[30] employed a catalytic membrane based on ultrafiltration and
ozonation for drinking water treatment. This work examines an
advanced ozone membrane reactor for treatment of recalcitrant
organic EDCs in water. The membrane reactor uses membranes
for ozone distribution, reaction contactor and water separation
in a compact unit that synergistically combines ozone oxidation
and membrane separation to achieve greater treatment efficiency.
The use of multi-functional membrane reactor was shown to
benefit gas-phase and liquid phase reactions [31–38]. Indeed,
prior works showed the new membrane reactor increased min-
eralization rate, improved ozone utilization, reduced membrane
fouling and enhanced clean water production [39,40]. This study
investigates the design of the reactor and membranes using a math-
ematical model to guide the optimization and scale-up the process
0920-5861/$ – see front matter © 2012 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.cattod.2012.03.059