By mimicking iron(Fe)-based phosphorus
(P) immobilization in natural
environments, an Fe-retrofitted UCT-MBR involving in situ vivianite
crystallization for removing and recovering P from sewage was developed,
and its performance was examined in this work. We show that dosing
of ferrihydrite, once biological P uptake reached its limit, enabled
effective ongoing P removal; whereas conventional conditions in the
anaerobic chamber of the University of Cape Town (UCT) system (i.e.,
a sludge retention time of hours and a completely mixed sludge phase)
was insufficient for a satisfactory Fe(III) bioreduction, with the
overaccumulation of Fe(III) as fine particles finally resulting in
severe membrane fouling and collapse in P removal. The enhancement
of reductive conditions in the anaerobic chamber by lowering agitation
and adding biocarriers to favor Fe(III) reduction was found to be
effective in enabling ongoing P removal and recovery. The average
level of effluent P was as low as 0.18 mg/L for a period of 258 d
under this condition. Using chemical and spectroscopic methods, the
P product was identified as primarily vivianite: Fe3(PO4)2·8H2O. The in situ crystallization of vivianite as a sink for P enabled the UCT-MBR
to continuously remove and recover sewage P with no need for sludge
discharge.
The formation of
vivianite (Fe3(PO4)2·8H2O) in iron (Fe)-dosed wastewater treatment
facilities has the potential to develop into an economically feasible
method of phosphorus (P) recovery. In this work, a long-term steady
FeIII-dosed University of Cape Town process-membrane bioreactor
(UCT-MBR) system was investigated to evaluate the role of Fe transformations
in immobilizing P via vivianite crystallization. The highest fraction
of FeII, to total Fe (Fetot), was observed in
the anaerobic chamber, revealing that a redox condition suitable for
FeIII reduction was established by improving operational
and configurational conditions. The supersaturation index for vivianite
in the anaerobic chamber varied but averaged ∼4, which is within
the metastable zone and appropriate for its crystallization. Vivianite
accounted for over 50% of the Fetot in the anaerobic chamber,
and its oxidation as it passed through the aerobic chambers was slow,
even in the presence of high dissolved oxygen concentrations at circumneutral
pH. This study has shown that the high stability and growth of vivianite
crystals in oxygenated activated sludge can allow for the subsequent
separation of vivianite as a P recovery product.
Vivianite (Fe3(PO4)2·8H2O) crystallization has attracted increasing attention
as a
promising approach for removing and recovering P from wastewaters.
However, FeII is susceptible to oxygen with its oxidation
inevitably influencing the crystallization of vivianite. In this study,
the profile of vivianite crystallization in the presence of dissolved
oxygen (DO) was investigated at pHs 5–7 in a continuous stirred-tank
reactor. It is found that the influence of DO on vivianite crystallization
was highly pH-related. At pH 5, the low rate of FeII oxidation
at all of the investigated DO of 0–5 mg/L and the low degree
of vivianite supersaturation resulted in slow crystallization with
the product being highly crystalline vivianite, but the P removal
efficiency was only 30–40%. The removal of P from the solution
was substantially more effective (to >90%) in the DO-removed reactors
at pH 6 and 7, whereas the efficiencies of P removal and especially
recovery decreased by 10–20% when FeII oxidation
became more severe at DO concentrations >2.5 mg/L (except at pH
6
with 2.5 mg/L DO). The elevated degree of vivianite supersaturation
and enhanced rate and extent of FeII oxidation at the higher
pHs led to decreases in the size and homogeneity of the products.
At the same pH, amorphous ferric oxyhydroxide (AFO)the product
of FeII oxidation and FeIII hydrolysisinterferes
with vivianite crystallization with the induction of aggregation of
crystal fines by AFO, leading to increases in the size of the obtained
solids.
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