Anaerobic membrane biotechnology for bioenergy and resources recovery from

wastewater: Current status, opportunities and perspectives

Abstract

Overall deficiencies of water, energy and climate change are receiving increased

attention for economical and sustainable wastewater treatment processes that may recover

those resources. A few systems have been recommended to give solution for the need.

Wastewater has been investigated as a source for nutrient, biogas, volatile fatty acids, and

biohydrogen recovery. Therefore, it is necessary to remove resources from wastewater.

Membrane biotechnology is found very promising method for resources recovery. Anaerobic

membrane bioreactor (AnMBR) technology holds great potential in waste treatment, and

energy consumption. Using AnMBR can decrease carbon footprint, sludge production,

increase sludge retention time quality of effluent and eliminates wastewater impact on

environment. This study aims to present analytical and complete review on recent advances

in anaerobic membrane biotechnology for resources and bioproduct recovery from waste

water along with challenges and opportunities.

Keywords: Anaerobic membrane bioreactor, nutrient recovery, biogas, biohydrogen, volatile

fatty acids, membrane fouling

Graphical abstract
1. Introduction

Overall deficiencies of water and energy are receiving increased attention for economical

wastewater treatment that may recover those resources. A few systems have been

recommended to give solution for the need (Chen et al., 2017a; McCarty et al., 2011).

Anaerobic membrane bioreactor (AnMBR) technology holds great potential in industrial

waste treatment. Compared to conventional aerobic process, it scales back sludge production

and energy consumption (McCarty et al., 2011). Over the past decade, there have been

several attempts to test AnMBR on lab scale. On lab scale AnMBR comparable effluent

quality is observed with conventional aerobic process (Lin et al., 2013; Skouteris et al., 2012;

Smith et al., 2012). Furthermore, AnMBR have been accounted to own environmental and

economic advantage over standard aerobic treatment processes (Pretel et al., 2016a; Smith et

al., 2014a). Over ten pilot-scale AnMBRs were studied after getting quality results on lab

scale. Pilot-scale AnMBR fed with real domestic wastewater, designed with industrial

membrane module and its results are sufficient for designing full-scale AnMBR. Only few

studies summarized results of pilot-scale AnMBRs. Fouling control demands high energy for

treatment of low strength wastewater (Skouteris et al., 2012; Smith et al., 2012).

Nutrients like phosphorus (P) and nitrogen (N) are vital for growth, survival and

reproduction of organisms. Overly enriched nutrients can cause eutrophication which include

excessive growth of organisms and may cause serious disorders (Gao et al., 2018). Therefore,

it is necessary to remove nutrients from wastewater and discharge of nutrients should be

analysed strictly. Nutrients must be discharged at concentration to be underneath 0.1 mg P/L

and 1-3 mg N/L, respectively (Fowler et al., 2013). N and P are mainly present as ammonium

and phosphate ions in wastewater. In earlier studies these ions were removed by nitrification-

denitrification and ammonia stripping, current studies show the removal of ions is carried out
by biological uptake and chemical precipitation (Liu et al., 2017a; Ye et al., 2017; Yin et al.,

2018). Although a large amount of chemicals and energy are not required for the removal of

nutrients from wastewater. Excess 4% power is required in United States for removal of N in

wastewater treatment plants (McCarty et al., 2011; Svardal & Kroiss, 2011). As a result of

Nutrient removal 0.9 kg CO2/m3 is emitted which cause global warming (Hall et al., 2011;

Svardal & Kroiss, 2011).

Nutrient based fertilizers demand increased nearly 1.8% per year for food production,

as world population is growing exponentially (Ledezma et al., 2015). However, there are

many difficulties in production of fertilizers. For food production demand approximately

90% of phosphate is consumed (Schroder et al., 2010), but in 30 to 300 years the remaining

phosphate rocks will be consumed completely (Elser & Bennett, 2011). Phosphate in

fertilizer cannot be substituted with other nutrients (Ichihashi & Hirooka, 2012). However,

ammonia is produced by Haber-Bosch process for fertilizer production, NH3-N is made by

utilizing atmospheric N (Fowler et al., 2013). The N-cycle is disturbed, and environment is at

risk by anthropogenic production of NH3-N, which is more than natural converted NH3-N

(Fowler et al., 2013). Moreover, huge amount of energy 35-50 MJ/kg N is depleted as a result

of generation of ammonia from atmospheric air, which comprises of 2% of global energy

(Desloover et al., 2012).

Membrane biotechnology is found very promising method for nutrients recovery (Qiu

& Ting, 2014). Removal of organic causes low membrane fouling in bioreactor. AnMBR can

decrease carbon footprint, sludge production and size of equipment as well Increase sludge

retention time and quality of effluent. Ina addition, no biological sedimentation unit ensure

safety. Table1 explains many configurations of membrane hybrid systems for recovery of

nutrients. Many studies have been done to recover resources from wastewater and use them

as fertilizer for food security and to eliminate wastewater impact on environment (Ichihashi
& Hirooka, 2012; Qiu & Ting, 2014). Membrane hybrid system concentrates nutrients with

low foreign matter. But technical and economic feasibility of membrane hybrid systems are

not discussed properly. This paper aims to present analytical and complete review on recent

advances in anaerobic membrane biotechnology for resources recovery from waste water

along with challenges and opportunities.

Figure 1.Flow chart of AnMBR system for resources recovery.

2. Mechanism and reactor configuration

According to the today’s scenario, natural resources are going decline day by day. So,

there come need to recover resources and energy. For this the waste and wastewater becomes

valuable for the researchers. According to the studies the waste and wastewater produces

biogas, biohydrogen, VFA etc. by anaerobic process which will used as a fuel and as a
fertilizer and produces carbon dioxide by aerobic process (Falahti-Marvast & Karimi-Jashni,

2015; Ma et al., 2016). Among them the anaerobic process is more preferable then aerobic

process and in anaerobic the AnMBR technology is preferred due to its economical and

environmentally friendly advantage as compared to conventional technology (Pretel et al.,

2016a; Smith et al., 2014a). It is observed that this technology become very promising, due to

its low consumption of energy and sludge generation as compared to other technologies

(McCarty et al., 2011). The requirement of anaerobic process from conventional aerobic

process is because of its major drawback that is aerobic process produces greenhouse gases

(Xie et al., 2014b).

The anaerobic process is the biological reduction procedure in the absence of oxygen

in which the biodegradable solid decompose with the help of microorganism (Adekunle &

Okolie, 2015). This procedure consists of four major steps hydrolysis, acidogenesis,

acetogenesis, and methanogenesis (Adekunle & Okolie, 2015; Deublein, 2008; Passos et al.,

2014) as shown in Fig. It starts with the hydrolysis of insoluble organic solid for example

protein etc. into soluble organic solid like sugar etc. these monomers are then converted into

intermediate products like VFA, Carbon dioxide etc. due to bacterial reaction in acidogenesis

(Kim et al., 2010; Wei et al., 2015; Zhao et al., 2016). These intermediates are not in the

stage of converted to methane so, to convert into stable intermediate like acetate, carbon

dioxide, hydrogen etc. is done by acetogenesis bacterial reaction (Li et al., 2015a; Li et al.,

2015b; Ozgun et al., 2013) and then these stable intermediates are finally converted to

methane under methanogenesis bacterial reaction (Lv et al., 2016; Passos et al., 2014).
 Fig. 2 steps involve in anaerobic processes

Among them the hydrolysis step is consider as a rate controlling step (Aquino &

Stuckey, 2008; Vavilin et al., 2003) and the slowest rate of biological reaction among all the

step is methanogenesis (Lv et al., 2016; Passos et al., 2014). The microorganism growth rate

of each step fluctuates due to the temperature, pH, physiology, and nutritional requirement.

So, to maintain balance between them become a major challenge (Adekunle & Okolie, 2015).

For an effective working of anaerobic process there is need to be optimization in the rate of

hydrolysis and methanogenesis (Fezzani & Cheikh, 2010; Xu et al., 2014).

Configurations of bioreactor play a major role in production of biohydrogen as it

affects the microenvironment of a reactor (Ntaikou et al., 2010). The significant

improvement is shown in the production of hydrogen and methane by using multiple stage

arrangements. Different designs, configurations and materials are available (Bundhoo &

Mohee, 2016; Jung et al., 2011). There were mainly three configurations used which are: the

external cross-flow Fig. 1a (Saddoud & Sayadi, 2007), the submerged membrane with

external membrane tank Fig. 1b (Lee et al., 2008), and the submerged membrane Fig. 1c

(Bohdziewicz et al., 2008). In external cross-flow membrane trans-membrane pressure is

required in circulation of pump. As a result, the formation of filtration cake unsettles on the

membrane surface by the cross-flow velocity (Bornare et al., 2014). Submerged membrane
with external membrane tank formation of filtration cake is disturbed with an external stirrer

in the tank (Aslan et al., 2014). In submerged membrane bioreactor membrane is operated at

vacuum instead of direct pressure and the module of membrane is directly adjusted in liquid

(Liao et al., 2006).

Fig. 3 anaerobic membrane configurations (a) external cross- flow configuration (b)
Submerged membrane with external membrane tank configuration (c) Submerged membrane
without external membrane tank configuration.

3. Opportunities for bioenergy and resources recovery

3.1. Biogas production

The first attempt on anaerobic membrane bioreactor (AnMBR) model was performed

by Grethlein in 1978 and research on model then started and detailed study on AnMBR was

represented in 2006 (Liao et al., 2006). Thus, AnMBR are verifying that this technology is

more valuable for waste water treatment because they avoid wastage of biomass from

bioreactor and generate excellent quality of effluent (Gao et al., 2010) and consume small

amount of energy as compared to aerobic process for treatment. It also generates biogas,

which is normally belongs to a combination of gases generated due to biological reaction of

organic substance in the deficient of oxygen. Combination normally contains hydrogen,

methane, nitrogen and carbon dioxide. But the larger fraction of biogas usually 70 to 90%

consists of methane (Chen et al., 2017b; Dolejs et al., 2017; Gouveia et al., 2015; Lin et al.,

2013) that is used to produce electricity by combusting biogas, that energy is utilize for the

wastewater treatment system (Kanai et al., 2010; Xie et al., 2010).

Methane becomes renewable fossil fuels which is generate from anaerobic digestion

system (Lehtomäki et al., 2008). Many biomass sources such as waste water and waste solid

as a feed for AnMBR, converted to methane. The AnMBR system has reliable temperature

flexibility with outstanding operation, conveyed under psychrophilic (Trzcinski & Stuckey,

2010), thermophilic (Gao et al., 2010) and mesophilic (Xie et al., 2010) situation. According

to (Gao et al., 2010) studies, greater than 90% of COD removed when organic loading rates

(OLR’s) was in the rage of 0.23 to 24 kg COD/m³/d. during pilot scale plant operation, biogas

generation rate fluctuates between from 0 to 220 L/d, while at full size plant operation it

could be great enough as 800Nm³/d. This generated gas had 60% methane and with two stage

it extended to 90% (Gao et al., 2010; Saddoud et al., 2009). The data are extracted from

different studies in Table which show different trend of biogas production and present

methane content on different operating conditions.

There are some factors which effect the methane generation, some of them is OLR,

as OLR high in influent the rate of generation is high (Chen et al., 2017b). The pH of the

system also takes part in methane generation. For the accurate completion of methanogen

reaction, the pH of system should be in limit of 6.6 to 7.6 (McCarty, 1964). If the pH of

system decreases from 6.2 the methanogen reaction will not able to be processed

(Switzenbaum et al., 1990). The Fig describes other factors on which whole system depend

and produce products.

 Fig. 4. Factors effecting AnMBR system

The most important part of a study on anaerobic process has some main goal, which

of them is the enhancement of energy transformation and effluent quality (Hu et al., 2018) by

improving the anaerobic process for methane generation (Abdelsalam et al., 2016; Huang et

al., 2016; Intanoo et al., 2016). The biogas yield can be enhanced by increase in accessible

carbon abundance (Di Maria et al., 2016) and this rise is due to co-digestion of the sludge

with rich organic waste (e.g. food) (Wickham et al., 2016). The enhancement of effluent

quality through anaerobic process, highly depend upon the reactor type. According to (Hu et

al., 2018) comparison between HF-AnMBR, continuous stirrer tank reactor (CSTR), and self-

agitated reactor (SAR) He realized that membrane reactor gives higher COD removal

efficiency then others reactor that is 80% and its effluent quality is 100 times better then SAR

The anaerobic process which is perform presently for the enhancement of methane

production is by headspace flushing with nitrogen and carbon dioxide where the enhanced

carbon dioxide solubilization reduces the oxygen stress on methanogenesis that’s result

greater yield (Koch et al., 2015). Some researcher has proved that the production of methane

can be increase by removing intermediate products (VFAs and biohydrogen) from anaerobic
process (Intanoo et al., 2016; Peces et al., 2016). The methane yield can be increased by

recovering dissolved methane which can do by degasification of membrane contactors and

non-spongy membrane (Cookney et al., 2016). The generation of methane can also be

increase by recycling anaerobic digester effluent (Li et al., 2015a; Li et al., 2015b).

According to newly concept, the rate can be increases as process transfer from single to two

stage anaerobic digestion system by implementing alternate working condition for hydrolysis

and methanogenesis (Intanoo et al., 2016).

The methane generation increases due to steadiness of An-digester below maximum

working condition. For example, greater OLR (up to 40kgCOD m-3d-1) greater abundance of

salt (up to 15 g/L Na and 152 mg/L Ca abundance) and a large span of pH (6.2 to 8.5) (Xing

et al., 2015; Yu et al., 2016). The membrane type also takes part in enhancement of methane

generation and COD removal efficiency. So, by using dynamic membrane instead of simple

membrane remove COD up to 98% and methane up to 60% (Joo et al., 2016). The methane

generation can be increase by enhance two-phase anaerobic digestion (TPAD) system by

converting volatile fatty acid (VFA) into acidogenic effluent that convert into methane at a

typical generation rate of 0.28 m³/m³/d with hydrolytic retention time (HRT) of 14 days. By

inserting cellulose hydrolysers, the substrate dosing frequently increased, and by feeding 1-20

mg/L nanoparticles (Fe, Ni, Co or Fe3O4) etc. results in 1.8 time rises in methane production

(Abdelsalam et al., 2016; Manser et al., 2015; Martin-Ryals et al., 2015).

The research success in methane generation show lot of potential but financial

possibility calculation for different techniques is more important to judge which techniques in

process will be less amount then other technique. There is 20% reduction in working cost

while using dynamic anaerobic membrane bioreactor then simple AnMBR (Joo et al., 2016).

The importance of AnMBR is due to maximum biogas and its main component, methane.

The amount of methane which is generated is the main part of anaerobic digestion process.
By comparing with others anaerobic digestion system, methane has many benefits; firstly, it

can be used as a fuel with or without purification. Secondly, consume low energy during

generation process (Kleerebezem et al., 2015). The financial possibility of AnMBR can be

increased by recovering the dissolve methane, when particularly system run at low

temperature and low HRT (Cookney et al., 2016). But the major problem of AnMBR is the

steady methane generation rate because low substrate in feed give low yield (Pretel et al.,

2015), which effect the financial possibility.

According to (Pretel et al., 2015), the estimated design conditions for submerged

AnMBR below various solid retention time (13 – 41 days), OLR (10 – 15 g/L MLSS) and

working temperature (15 - 30˚C). Further, the installation cost (reactor construction,

membrane and pumps) and working cost (sparging of gas, working of pumps and filtration)

of overall recovery of methane were computed against the generated revenue from methane.

As per outcome, revenue from overall recovery of methane obligated negative value

fluctuating from (-0.005 t0 -0.002 Euro/m3) beside of overall cost ranging from (0.130 to

0.079 euro/m3). This shows that profit earned from methane generation could not cross the

installation and working cost of an AnMBR.

Though, AnMBR technology effectively treats waste water and waste material and

give us useful products but have bad impact on environment. As its main product contains

methane, which is a greenhouse gas and having world-wide warming potential 28 to 36 times

greater than CO2 (Smith et al., 2014b). The dissolve methane in effluent also have bad impact

on environmental which make the effluent non-feasible to use so, to reduce bad impact there

are various models which explain the method to remove dissolve methane from effluent

(Cookney et al., 2016). The methane when combusted give carbon dioxide due to which the

environmental regulatory bodies have identified the harmful effect of climate changing due to

CO2 emissions and all world present political parties are completely focus on to reduce CO2
emissions by combusting fossil fuel (Cucchiella & D’Adamo, 2013). So, there comes up to

develop a renewable source to overcome the environmental issue and reduces use of fossil

fuels, as their reserves left finite currently (Wei et al., 2013).

Table 1 Summary of methane production and system performance of AnMBRs

Scale Wastewater configuration Reactor Membrane Temperature HRT Influent Methane yield Methane COD Reference
source capacity characteristics (˚C) (h) COD (LCH4/gCODremoved) content/ removal
(L) (mg/L) conversion (%)
rate
Pilot SMWa External 72 Silver coated 35-37 30 2400 0.31 70 – 75% 82 Amouamouha
PVDF, PES and Gholikandi,
0.22 µm 2018
Lab SMW Submerged 6 FS 25 8 670 ± 0.326 93 - Chen et al.,
PVDF 100 2017e; Chen et
0.20 µm al 2017d
Lab CPW and Submerged 6 (13L FS 55 10 d 42.4 ± 0.28 60% 92 ± 3 Chen et al.,
WAS total vol) 0.20 µm 9.9 g/L 2018

Lab SFW Submerged 21.6 FS 35 ± 1 20- 3000- 5 – 50 L/d 49 - 67% 94 ± 8 Casu et al.,
0.4 µm 120 d 27000 2012
Lab Synthetic Submerged 24.5 HF, MFPF 37 ± 2 - 4600 - 79%-83% 90 Aslan et al.,
wastewater 0.1 µm 2014
Lab SW Submerged 4 FS, CTA 25 15 - 460 - 65 - 78% 96 Chen et al.,
0.025 m² 40 2013
Lab SW Submerged 6.8 FS, PP 35.7 ± 0.1 240 20100 3.25 L/d 64%-72% 99 Ersahin et al.,
10 µm ± 310 2014
Lab SW Submerged 0.6 HF, PP 35 14 d - 0.168 L/d - 99 Jeong et al.,
0.45 µm 2010
lab SMW External 4 HF, PVDF 20 ± 0.5 12 330- 0.16 ± 0.006 45.3% 91.9 ± Chen et al.,
0.22 µm 370 1.5 2017a
Lab PWLL Submerged 10 FS, PVDF 37 - 2.78- 68% 90 Gao et al., 2010
70 kDa 3.35 -
Lab FW External 15 HF, PTFE - 5-30 73610 58-61 80.4-92.9 Hui cheng et al.,
0.2 µm d ± 3100 - 2018
Pilot PW External 180 HF, PVDF 40 48 - 2700- 0.195±0.017 to 66% 94 Huang et al.,
0.02 µm 24 6760 0.291±0.032 2018
Lab SW Submerged 7.4 FS 35.7 10 d 20,100 2.4 L/d - 99.5 Ersahin et al.,
2017
 Lab SMW submerged 6 FS, PVC 25 ± 1 12 492 ± 0.30 86.9 97.07 Nie et al., 2017
0.2 µm 112 CEJ
Lab SW External 0.7 FS, Nylon 35 1-7 d 5000 01-09 L/d 50%-79% 64-94 Alibardi et al.,
mesh 2014
200 µm
Pilot MW External 310 HFM 6-30 10- 892 ± 0.235 67.1 - Gouveia et al.,
submerged 0.045 µm 13.4 271 2015 BITE
Lab LL Submerged 48 FS, 37 2.5 d 13000 0.34 - 62.2 Xie et al., 2014
Dacronmesh
40 µm
Lab FW Submerged 5 HF 24 ± 2 24 1463 2.8 ± 0.2 L/d 38.4 87.50 M. Galib et al.,
0.04 µm 2016
Pilot DW External 50 UF 37 15 - 685 30 L/d 70% 55-90 Saddou et al.,
100 kDa 60 2007
Lab DWP External 10 CF, PVDF 37 6 29.2 ± 0.28 Nm3 - 98 Dereli et al.,
0.03 µm 3.3 g/L CH4/gCODremoved 2018
Lab DW Submerged 3.6 FS, Ceramic 25-30 7.5 330.4 ± 0.3 ± 0.001 85.70% - Yue et al.,2015
0.2 µm 89.8
Lab SWa Submerged 6 FS, PE 20-25 6-48 492 ± 2.11-2.85 L/d 32-77 80-97 Nie et al., 2017
0.2 µm 112 Energy

Lab SW External 0.7+0.06 FS 20-24 0.25- 900 0-0.2 - >89 Alibardi et al.,
5.7 2016
Lab DW Submerged 6 FS, POMM - 12 121 ± - - 83 Achili et al.,
0.4 µm 34 2011

Lab SMSW Submerged 3 FS, PE 35 0.37 - 4000- - 1-71% 93-94.5 Trzcinski and
0.4 µm 5.7 26000 Stuckey, 2009

CF: Cross flow, CPW: coffee processing wastewater CTA: Cellulose triacetate, DW: Domestic wastewater, DWP: Dilutedwheypermeate FS: Flat Sheet, FW: Food waste, HF: Hollow fibre, HFM:
Hollow fibre membrane, LL: Landfill leachate, MFPF: micro filtration polyethylene fibre, MW: municipal wastewater, PE: Polyethylene, PES: Polyethylene sulfone, PET: Polyethylene
terephthalate, POMM: Polyolefin microfiltration membrane, PP: polypropylene, PTFE: Polytetrafluoroethylene, PVC: Polyvinyl chloride, PVDF: Polyvinylidene fluoride, PW: pharmaceutical
wastewater, PWLL: Pulping Whitewater landfill leachate, Synthetic food wastewater (SFW), synthetic municipal solid waste (SMSW), Synthetic molasses wastewater (SMW a), Synthetic
municipal wastewater (SMW), Synthetic wastewater (SW), Sewage wastewater (SWa), UF: Ultrafiltration, WAS: waste activated sludge
3.2. Biohydrogen production

Production of biohydrogen from anaerobic process in wastewater treatment showing

increasing trend due its reliability. According to some recent studies hydrogen is predicted as

very consistent energy carrier in future (Devabhaktuni et al., 2013). Hydrogen is recognised

as one of the most energy effective energy fuel in energy adaptation for transportation area

(Ciancia et al., 1996; Hajimiragha et al., 2011). Hydrogen is emitted through some

microorganisms either from organic source or from water in reaction catalysed by

hydrogenase enzymes (Benemann, 1998). Production of hydrogen through microbial sources

has various benefits and it could be considered as a low-cost alternative to the recent

industrial processes of production H2 (Cao et al., 2001). Production of H2 by using dark

fermentation process produces a mixture of gases containing hydrogen and carbon dioxide

and liquid effluent containing large quantity of VFA (Bakonyi et al., 2018; Boboescu et al.,

2016; Ghimire et al., 2017; Khan et al., 2016b). Production of hydrogen by fermentation

process is one of the easy routes for hydrogen process (Hallenbeck & Benemann, 2002).

Production of gaseous molecular hydrogen and carbon dioxide is also the part of the

production of VFA from second and third stages of anaerobic process also contain molecular

hydrogen and CO2. The gaseous mixture containing biohydrogen and carbon dioxide is

collected at the top of the reactor (Kumar et al., 2016). Although the hydrogen is not present

in in nature abundantly, but it is considered as emerging fuel of the next century. Hydrogen

gives the high energetic yield of 122 kJ/g that is 2.75 times greater than hydrocarbon fuels

(Kapdan & Kargi, 2006). It combusts to produce only H2O and has a large energy content

(Lee et al., 2009). The energy obtained from the combustion of hydrogen is on the mass basis

having lower heating value (LHV) that is 4, 2.4 and 2.8 times greater than that of coal,

gasoline and methane respectively (Abbas & Daud, 2010). Hydrogen is recognized as a best

16
energy fuel for transport sector, moreover due its specific weight (0.0899 kgNm-3 at 1 atm

and 0 ℃ ) H2 is 2.5 times more effective than gasoline(Bergamaschi et al., 2005).

Production of biological hydrogen by using fermentation process has acknowledged a

significant importance. However, it has a limitation of low hydrogen production yield

because of generation of reduced organic species (Lee et al., 2008) Typically the fermentative

hydrogen production is produced in stirred tank reactors (CSTR) by using renewable

resources like sugar or starch (Shen et al., 2009). The dark fermentation process normally

occurs along with methanogenesis in anaerobic digestion, as hydrogen and acetate generated

from dark fermentation used as substrates for methanogenic bacteria (Inloes et al., 1983).

Organic compounds would be converted to methane, hydrogen of electrical energy after

fermentation process (Hallenbeck & Ghosh, 2009). The dark fermentation processes many

practical applications because it has ability to convert different wastes organic substances into

hydrogen (Das & Veziroǧlu, 2001; Levin et al., 2004). Acetic acid butyric acid can also give

hydrogen under fermentation process (Guwy et al., 2011; Hosseini & Wahid, 2016; Xia et al.,

2016).

Using of membrane technology in anaerobic process has shown benefits of low HRT,

SRT and sludge production and to enhance the quality of reactor effluent (Krzeminski et al.,

2017; Pretel et al., 2016b). In AnMBRs several membranes to minimize the disadvantages of

conventional anaerobic technologies e.g., high HRT and SRT have been used for the

treatment of various wastewater streams such as municipal wastewater(Grundestam &

Hellström, 2007). Production of hydrogen by using continuous cultures is normally carried

out in CSTRs in which microorganism proliferation is identified by the applied rate of

dilution showing a possible risk of biomass washout (Li & Fang, 2007; Show et al., 2008).

when the different bioreactor assemblies are compared in order to choose the best alternative

to increase hydrogen and methane production, results shows that Anaerobic membrane

17
bioreactor (AnMBR) provides vigorous and reliable operating possibilities, regardless of

threat of membrane fouling.

The performance of different AnMBRs for production of hydrogen is summarized in

Table 1. The entire studies were summarized at small-scale and 5 to 60 L/m2/h membrane

refluxes were obtained. Carbon was obtained from the sugars, and the AnMBR system were

operated at mesophilic temperatures, and operated at thermophilic temperatures apart from an

investigation that applied wastewater (Kim et al., 2011). The idea of linking a hydrogen

fermenter with a bioreactor is also found in different research models (Bakonyi et al., 2015).

For maximum production rates, Simultaneous production of hydrogen and methane from the

two-stage UASB reactors is the part of recently developed models (Intanoo et al., 2016;

Jariyaboon et al., 2015). Some combined approaches are now being established such as

multistage bioreactor, two-step hybrid fermentation process (Hwang et al., 2011; Show et al.,

2011), or the use of modified microbial fuel cells (De Mes et al., 2003; Ueno et al., 2007).

These types of systems are already being adapted at pilot-scale, for example the joining of

methane and hydrogen fermentation of kitchen waste has tend to remove 80% of COD and

produce 5.4 m3/m3 d of hydrogen and 6.1 m3/m3 d of methane (Ueno et al., 2007).

The suitable technology for hydrogen production is AnMBR process. Maximum

treatment efficiency, high stability of operation, and stable production of biogas in AnMBR

have already been shown in various studies (Dereli et al., 2012; Lin et al., 2013). AnMBRs

have ability to convert 98% of influent into biogas and to produce least amount of sludge as it

produces less growth yield of anaerobic micro-organisms (Skouteris et al., 2012; Van Zyl et

al., 2008). Using of AnMBR is an emerging technology to prevent VFAs accumulation

during managing of biomass in the medium. Different designs, configurations and materials

are available (Bundhoo & Mohee, 2016; Jung et al., 2011; Singhania et al., 2012). The

development of integrated systems is another way through which hydrogen is produced by

18
using fermentation process would be joined to the next process. Organic compounds would

be converted to methane, hydrogen of electrical energy after fermentation process

(Hallenbeck & Ghosh, 2009). However, to identify the advantages of AnMBR obtained from

the few lab-scale studies performed, there are more studies required at both experimental-

scale and pilot-scale.

Moreover, issues of membrane fouling must be identified, as the microorganisms that

produce hydrogen may contain different properties as compared to other membrane systems.

There are normally three processes (Pore narrowing, pore plugging, and cake layer

formation) which may cause membrane fouling (Metcalf, 2003). The behaviour of membrane

fouling is normally related to both blocking of pores and formation of cake, regardless of the

process whether it is anaerobic or aerobic. High capital cost for the membrane, fouling of

membrane, and high cost of operation due to energy required are the major drawbacks of this

technology (Al-Malack & Anderson, 1997). The two major barriers in the production of

biohydrogen are low yield and cost of production. Low yield of biohydrogen is the biggest

issue in anaerobic fermentation process on the basis of fermentation reaction maximum yield

of hydrogen is 4 mol H2/mol glucose and this can only be obtained when electron sinks are

acetate and hydrogen (Lee et al., 2008; Logan, 2004; Thauer et al., 1977).

One of the major challenges is to decrease the cost of production, storage, conversion,

delivery, and practical applications. Production of hydrogen using traditional industrial

processes is costly so, there is need to find ways through which hydrogen can produce at low

cost. Production cost of hydrogen from renewable biomass has been identified in various

studies (Sarkar & Kumar, 2007). Cost of producing hydrogen by using renewable biomass

ranges from US$10 to 14 GJ-1 having net higher heating value (HHV) energy efficiency of

56-64% (Hamelinck & Faaij, 2002) The modified process can be used to improve the

hydrogen yield, by effective bioreactor design, bacterial tension, genetic and molecular

19
engineering method metabolic pathway can be improved. A major part of hydrogen that is

being used is not produced from the renewable resources. To overcome the economic

limitations and to achieve the maximum energy requirements, the production of hydrogen

through renewable biomass such as molasses, bagasse, and agricultural wastes can be used

(Kivistö et al., 2010; Perera et al., 2010) under the dark fermentation process (Bharathiraja et

al., 2016; Hay et al., 2013).

The trend of biodiversity of the microbial community that produce hydrogen is still

being exposed. This multidirectional biodiversity will be selected by establishing

mechanisms for unified management and application of these microbial resources as the

maximum work is expected in coming era. Biomass resources are abundantly present in

Asian countries and they have ability to produce biohydrogen as a fuel by using biomass

resources (Pudukudy et al., 2014). The techniques and potential for connecting microbial

resources can highlight the further enhancement of yield and production rates of H2. The

hydrogen production technologies are not much developed that they can apply on large

industrial scale. Countries like Singapore, Pakistan, Philippines and Indonesia have biomass

resources in large quantity, but due to lack of effective policies they do not really show

interest to produce biohydrogen as a fuel by utilizing these resources (Haslam et al., 2012). In

order to promote the technology of hydrogen production the international incentives to

produce hydrogen economy (IPHE) taking initiatives to enhance hydrogen economy chain

worldwide and encouraging ongoing projects on advancement of biohydrogen technology

(Lube, 2012).

Production of hydrogen through anaerobic process involves negligible negative

effects on environment and also provides a good solution for energy crisis. Scientists,

engineers and researchers have promoted and encouraged the use of hydrogen as a fuel in

different areas (Pant & Gupta, 2009). The anaerobic process is the best way for hydrogen

20
production to overcome the problems associated with emissions of carbon (Intanoo et al.,

2016; Jariyaboon et al., 2015). Production of hydrogen through renewable energy resources

will remove the environmental problems (El-Osta & Zeghlam, 2000). Hydrogen can be

generated from carbon-free energy resources like wind, solar and electric energy, in this way

the harmful emissions could be eliminate by the application of hydrogen (Balat & Balat,

2009). Favourable raw materials for recent industrial generation of hydrogen includes natural

gas, coal and oil but all of the processes require greater energy and need massive amount of

fossil fuel (Hosseini & Wahid, 2016). Hydrogen has very good characteristics as green and

clean bio fuel the production of biohydrogen by using anaerobic fermentation process could

minimize the cost of production which sacrifice the efficiency of recent industrial methods; it

may signify maintainable and efficient energy in future because this is a renewable initiative

(Jung et al., 2011; Xia et al., 2015).

21
Table 2 Summary of performance of AnMBR for production of hydrogen
Carbon
source Feed Hydrogen Yield Hydrogen
Type of Membrane Configura HRT SRT Temperature
Inoculum Scale Substrate utilization COD production L H2/ mol content Reference
reactor specifications tion (h) (d) (˚C)
efficiency (g/L) rate (L/h/L) substrate (wt.%)
(%)
Anaerobic Kubota Co., Double- (Bakonyi)
digester AnHPMBR L Japan pore membrane Glucose 12 10 37 _ 40 0.24 1.13 _ et al.,
sludge size:0.45 µm bioreactor 2014)
Up-flow
Anaerobic anaerobic (Hern and
4380
granular sludge L _ _ Glucose _ 37 _ 10.05 1.72 2.6 _ Mendoza,
7
sludge blanket 2014)
reactor
Up-flow
Anaerobic anaerobic
Cheese 4380 (Reyes et
granular sludge L _ _ _ 37 _ 13.4 0.31 N. A _
Whey 7 al., 2014)
sludge blanket
reactor
N.S, Hollow
Heat-treated fiber (Kim et
AnHPMBR L _ TPW 10' 90 25 _ 30 19.8 42.4 _
sludge microfiltratio al., 2011)
n
Kubota Co,
Domestic flat sheet, PO, Submerge (Lee et al.,
CSTR L Glucose 9 450 35 99.6 8.25l 2.45-2.56 _ 51
wastewater pore size:0.2 d 2008)
µm
Heat-treated pore
3.3- (oh et
soil AnHPMBR L diameter: 0.2- _ Glucose 3.3-5 25 _ _ 9.2 N. Sd _
48 al.,2004)
inoculates 1µm
Kubota Co,
2-
Domestic flat sheet, PE, Submerge 50.8- (Lee et al.,
CSTR L Glucose 9 12.5 35 55-94/98 16e 3.9-5.8/2.0f _
wastewater pore size:0.45 d 60/52 2010)
/90
µm

Anaerobic
Anaerobic
sequencing Food (Kim et
digester L _ _ 10 _ 37 _ 55 1.76 0.95 _
batch Waste al., 2012)
sludge
reactor

22
Acid-treated, pore
3 (Lee et
acclimated AnHPMBR L diameter: 0.2- _ 1–4 N.S. 25 _ _ 66* 39 _
Hexoses al.,2007)
sludge 1µm
(Collet et
_ AnMBR L _ _ Lactose _ _ _ _ _ 1.5 _
al., 2004)
Deposition
sciences Inc.,
Domestic 4349 (Lee et
CSTR L Hollow fibre, External Fructose _ 35 79.5/94.2 20 2.75/1.87 _ 40.4/45
wastewater 7 al.,2007)
MF pore size
0.2 µm
Anaerobic
mixed
microflora
(Wang et
acquired pig Batch L _ _ Glucose _ _ _ _ _ _ 1405.0mL _
al., 2011)
manure
treating
reactor
Screened
pore
anaerobic (Shen et
AnHPMBR L diameter: 0.2- _ Glucose 8 24h 25 _ _ 4.5 40.2 _
digester al.,2009)
1µm
sludge
Kubota Co,
Heat-treated,
flat sheet, PE, Submerge 2- (Lee et al.,
acclimated AnHPMBR L Glucose 9 25 _ 30 5.8 27 _
pore size:0.45 d 90' 2010)
sludge
µm
Clostridium 9.95 mmol/g (Chen et
Batch L _ _ Starch _ _ _ _ _ _ _
butyric COD al., 2007)
m CGS2

Domestic MF, Hollow Submerge Tofu 4367 (Kim et

CSTR L _ 60 _ 26.5h 12.81-19.86i _ _
wastewater fiber d waste 9 al., 2011)

Kubota Co,
Domestic flat sheet, PE, Submerge (Lee et al.,
CSTR L Glucose 12.5 _ 35 68-100 16J 0-42k _ 62.6
wastewater pore size:0.45 d 2009b)
µm

Municipal (Chen et
CSTR L _ _ Sucrose 4 _ 40 _ _ _ 4.7 _
sewage al., 2008)

23
 34 g (Chang
Anaerobic
UASBr L _ _ Sucrose 8 _ 35 _ COD 0.75 _ _ and Lin
digester
/L ,2004)
Household (Liu et al.,
CSTR L _ _ Sucrose 48 _ 37 1.61 43 _
solid waste 2006)
GE Water
and process (Shen et
Domestic technology. Submerge 1.3- m al.,
CSTR L Glucose 8 1 23 7-100 0.02-0.2 _ 52-57
wastewater ZW-1 Hollow d 10 2009,2010
fibre, pore )
size 0.04µm
Anaerobic
(Wu et al.,
digester FBR L _ _ Sucrose _ _ 35 _ 45 3.17 _ _
2006)
sludge
US Filter Co.,
Tubular 0.5/
Domestic 0.64/0.31- (oh et
CSTR L ceramic, pore External Glucose 3.3/5 0.5- N. A 98/-99.5 10 _ 57-60
wastewater 0.46l al.,2004)
size 0.2-0.8 2
µm
b CSTR= continuous stirred tank reactor
c AnMBRs= anaerobic hydrogen production membrane reactor
d N.S
-= not specified
e =glucose concentration
f Units are L/L/d
g biogas production rate (units are L/h)
h dissolved COD
I Units are L/L/d
j glucose concentration
l biogas production
m Unit is mole/L/d

24
2.3 Volatile fatty acids

Biohydrogen generation and VFA production are two important factors for recovery

option of cost for AnMBRs. In AnMBRs the process of anaerobic digestion is very best way

for energy sustainability control of pollution of waste management into the environment. The

final product from digestion process which is get is methane and also VFA and biohydrogen

are produced as intermediate products (Khan et al., 2016a). By anaerobic acidification

technique volatile fatty acids generation is greater as hydraulic retention time of wastewater

reduced and it also depend on the bacteriological communal, feed features and design of

bioreactor used for reaction (Kuruti et al., 2017). The initiative is to be taken for reduction in

continuously increasing energy crisis and it is to be determined that on greenhouse gas there

is too much effect of resultant products that produces after any experiment or reaction .The

extraction of intermediate products like VFA and biohydrogen by individual anaerobic

digestion process is already proved feasible by the experiments (Abdelsalam et al., 2016;

Guwy et al., 2011; Yuan & Zhu, 2016). Demand for high value chemicals is reduced due to

VFA production and also VFA recognize as best indicators for biopolymers(Scoma et al.,

2016).

In AD process which begin or initiate with bacteriological hydrolyse of organic

materials which cannot soluble and combinations of materials with larger molecular mass

such fats, proteins and carbohydrates are converted into soluble derivatives such as sugars,

fatty acids and amino acids (Adekunle & Okolie, 2015; Passos et al., 2014). It is noted that

for definite type of bioreactor the factors like pH , temperature , HRT ( hydraulic retention

time), pre-treatment method of sludge, chemical additives and organic loading rates (OLRs)

etc. for VFAs generation these factors are directly influences (Garcia-Aguirre et al., 2017;

Jankowska et al., 2018; Khan et al., 2016a; Peces et al., 2016). Monomer is generated as a

result which is hydrolysed and this monomer is than converted into the VFA, alcohol, the

25
carbon dioxide and hydrogen through the help of bacteria which is acid forming bacteria

(Khan et al., 2016a; Kim et al., 2010; Wei et al., 2015; Zhao et al., 2016).

Optimize rate is required to mutually the lastly methanogenesis process and at first hydrolysis

processes for efficient anaerobic digestion process, but due to higher the ratio of hydrolysis as

related to methanogenesis rate VFA which are produced into the reactor are accumulate in

system and the PH of reactor is decreasing as a result of this accumulation of VFA and due

to decrease in PH the methanogenesis process is inhibited and also the digester system maybe

failed or damage(Fezzani & Cheikh, 2010; Xu et al., 2014). Also too much Experiments are

performed by (Khan et al., 2019) to find the optimum relation between Hydraulic retention

time and organic loading rates for production of different volatile fatty acids during waste

water treatment in continuous anaerobic membrane bioreactor. VFAs primarily include

butyric acid, valeric acid, propanoic acid and acetic acid these are forerunners of

methanogenesis and are products from initial acidogenic phase (Khan et al., 2016a; Khan et

al., 2016b; Morgan-Sagastume et al., 2011). And during anaerobic process between these

volatile fatty acids the acids like butyric acid, acetic acid and propanoic acid are most leading

VFA elements during volatile fatty acids generation, through butyric and acetic acid the

production of methane in biogas is directly produces from 65%to 95%and this is prove from

documented work(Khan et al., 2016a; Khan et al., 2019; Mamimin et al., 2017; Morgan-

Sagastume et al., 2011).

Through confirmed experimental results VAFs are recognize as probable bases of

medium length chain fatty acid, fatty alcohols and fatty acid methyl esters (FAMEs) (Elain et

al., 2016; Jung et al., 2016; Koutinas et al., 2014). Recovery of VFAs supports the

methanogenic activity and works against the production of organic acid, this is noticed during

AD process there are retardations in methanogenesis process and bacteriological stress due to

growth of high level of VFA (Fezzani & Cheikh, 2010; Huang et al., 2016; Khan et al.,

26
2016a; Xu et al., 2014). Recently created AnMBR reproductions designed for VFA

generations incorporates binary phase gathering , due to this model VFA is formed at initially

hydrolytic phase (Wijekoon et al., 2011). There is a basic challenge in which to remove the

water completely from VFA by conventional or membrane distillation process, as VFAs are

produced by hydrolysis method (Jung et al., 2016; Khan et al., 2016a).

The VFAs removal activity is mainly influenced by number of causes , these are like

washing of biomass by sudden flow rates changing, higher amount of water, due to impurities

presence and due to removed acids fractionations efficiencies (Huang et al., 2016; Khan et

al., 2016a; Scoma et al., 2016; Wijekoon et al., 2011). During anaerobic digestion up till now,

for VFA extraction, ammonia and electrodialysis are developed (Scoma et al., 2016). Identify

the difference for VFAs generation from binary stage AnMBR through GC through change

charging levels and temperatures (Wijekoon et al., 2011). And from different experiments

results shows that the organic loading rates are increases in the initial hydrolytic stage as the

production of VFAs are increases. And hence, the wastewater having higher concentration of

organic content is more favourable for VFA production which is more stable than the VFA

produces due to feed stock of municipal wastewater having low content of organic

compounds. For example, VFAs recovered by electrodialysis process from dephenolized

olive mill wastewater are cost effective (Khan et al., 2016a; Scoma et al., 2016).The VFAs

which produced at large scale or actually due to the chemical reactions which includes the

catalytic oxidation reaction between carbon monoxide and ethylene and also include

methanol carbonylation. To compare about financial aspects of anaerobic digestion process

and regular carbonylation process, the cost study is still not available. With methane the

removal of VFAs could be done or it is the aim of process for complete recovery of VFAs in

the AD process (Khan et al., 2016a; Peces et al., 2016).

27
 Through investigation of main slurry pre-fermentation in partial aerobic conditions

the results of experiment which are observed for both the VFA recovery and better methane

retrieval at 37 .C and 20 .C functional temperatures of experiment (Khan et al., 2016a; Peces

et al., 2016). VFA reduce the chemicals like alkanes, alcohols, aldehydes and ketones through

anaerobic digestion process at its initial hydrolysis stage. From permeate the volatile fatty

acids are recovered when using anaerobic membrane distillation bioreactor technology and

also VFA’s replaces different very costly chemicals like ketones, aldehyde, biofuels and

alcohols because they are initiators for different biopolymers (Khan et al., 2016a; Yao et al.,

2019).

`From VFAs which enhance Or upgrade the PMC (photosynthetic mixed culture) are

preferable as compare to the pure culture system used by commercial industries, because the

bio polymer like poly hydroxy alkenoate (PHA) which is produced is cost effective and also

use for manufacturing of plastics which are biodegradable (Fradinho et al., 2014; Khan et al.,

2016a). When AnMBR is used to produce VFA then main economic room motivate to do

more detailed research work on the estimation of economic practicality . Also anaerobic

membrane bioreactors have more capabilities for treatment of wastewater as related to

aerobic bioreactors (Goh et al., 2015; Jeison & Van Lier, 2008; Xia et al., 2016; Yao et al.,

2019).

The lessor the PH in the reactor can cause to inhibit or stop the methanogenic activity,

so the control is required for generation of VFA for prevention of reduction in PH and

maximum methane production (Yuan & Zhu, 2016). The production of volatile fatty acids are

reduced due to increases of temperature in membrane bioreactor because of the reason that

due to higher temperatures there is reduction in generation of VFAs because higher

temperature can encouraged the actions of thermophilic methanogens (Lettinga, 1995;

Puchongkawarin et al., 2015; Yao et al., 2019). Due to methanogenic inhibition hence VFA

28
and methane are produced, but also there is reduction in cost of installation and little amount

of energy is consumed and in the activity of AnMBR we also get extension in operating

conditions for use(Khan et al., 2016a; Kleerebezem et al., 2015). And in Table 3 from some

resources there is brief summary present which describe about the production of volatile fatty

acids at different operating conditions and also percentage of acetic and butyric acid is given,

and also how much of the COD removal efficiencies are documented into the paper.

Through potential solution the production of VFA and biohydrogen may be improve

economical or cost effective in AnMBR. The product fatty acid methyl esters (FAMEs)

Which is getting from conversion of VFAs are less toxic and highly biodegradable and

therefore used as a green solvent (Jung et al., 2016). The greenhouse emissions are also

reduces because of reasons that VFA’s are also used as green fuel (Khan et al., 2016a; Yao et

al., 2019).

Also VFA recovery can change the parts of organic carbon in the anaerobic digestion

and hence the methane production is lower and through this there is decrement in greenhouse

gas emissions and environmental impacts is reduced due to product(Khan et al., 2016a;

Puchongkawarin et al., 2015). So, the design of AnMBR is selected in which there is

maximum production of VFAs involve. At pilot scale attempts or to be made to produce or to

get the maximum production of VFA for AD process (Huang et al., 2016; Xia et al., 2016;

Yin et al., 2016). On the other hand, bacteriological actions are strongly effected undesirably

due to build-up of salinity and also through extensive period processes membrane fouling and

membrane saturating happened (Goh et al., 2013; Wijekoon et al., 2014; Yao et al., 2019). As

the biogas generation was reduce, it is because of reason that while VFAs are collected then

there is increase in soluble COD in both the reactor and effluent (Khan et al., 2016a)

Volatile fatty acids production from wastewater have also too many advantages when

using AnMBR technology like economic profits and also VFAs are higher inhibitors in

29
AnMBR technology so while separate these VFAs from bioreactors can cause increases in

production of microorganism’s (Gryta et al., 2013; Yao et al., 2019). The quick growth of

VFAs are due to lowering of Fe and Ni for the duration of anaerobic digestion of wheat

stillage. The microbial activities are stuck because of reason that the anaerobic membrane

bioreactor reactors with more initial salinity have lower total organic carbon in pass through

of membrane reactor and therefore the volatile fatty acids production are also reduce due to

higher the mass transfer resistance by cake layer increases (Luo et al., 2016; Yao et al.,

2019).

30
 Table 3 Summary of methane production and system performance of AnMBRs
Scale Wastewater configuratio Reactor Membrane Temperatur HRT Influent VFA Acetic acid Butyri COD Reference
n capacity characteristi e (˚C) (h) COD (mg/L) concentration c acid remov
(L) cs (mg/L) concen al (%)
tration
Lab Synthetic External 6 (t.v 9) MF, tubular 55 32 7500 – 2700 43.2% - 41.2% 74 Kaushalya et
molasses ceramic 18000 42.2% - 48% al., 2011
wastewater membrane
0.1 µm
Lab Synthetic External 6 (t.v 9) IF, tubular 55 32 16400 ± 3500 (under 47% 39% 80 Chaikasem et
municipal ceramic 800 PVA-gel) al., 2014
wastewater membrane
0.1 µm
Lab Synthetic External 6 (t.v 9) IF, tubular 55 32 16400 ± 2600 (without 57% 27% 90 Chaikasem et
municipal ceramic 800 PVA-gel) al., 2014
wastewater membrane
0.1 µm
Lab Municipal External 1.9 CF, PVDF 15 ± 1 10.4 610 ± 215 48 ± 38- - - 77 ± Zamanfar et al.,
wastewater 30 nm ± 4.7 10 2016
Lab Municipal Submerged 3.9 FM, PVDF 22 ± 1 48 – 6 550 ± 10 0.9869 ± 0.0403 49% - 55% 0.85% 70 Khan et al.,
wastewater 0.07 – 0.1 - 2019
µm 1.8344 ± 0.0875
milli-mole/L
CF: cross flow, IF: intermittent filtration, MF: micro filtration, PVA: polyvinyl alcohol, PVDF: Polyvinylidene fluoride

31
3.3. Nutrients

Nutrient based fertilizers demand increased nearly 1.8% per year for food production,

as world population is growing exponentially (Ledezma et al., 2015). However, there are

many difficulties in production of fertilizers. For food production demand approximately

90% of phosphate is consumed as fertilizer (Schroder et al., 2010), but in 30-300 years the

remaining phosphate rocks will be consumed completely (Elser & Bennett, 2011). Phosphate

in fertilizer cannot be substituted with other nutrients (Ichihashi & Hirooka, 2012). However,

ammonia is produced by Haber-Bosch process for fertilizer production, NH3-N is made by

utilizing atmospheric N (Fowler et al., 2013). The N-cycle is disturbed, and environment is at

risk by anthropogenic production of NH3-N, which is more than natural converted NH3-N

(Fowler et al., 2013).

Nutrient recovery is more beneficial than nutrient elimination because: 1) nutrient-

based fertilizers are produced which food security. 2) It can reduce carbon footprints of

wastewater, sludge production and decrease eutrophication, disorder in living organisms. 3)

Natural resources consumed much less, and cost is saved along with N fixation. Although, for

nutrient recovery there are many methods, biological method is more effective as compared

to chemical precipitation method (Johansson et al., 2017; Ye et al., 2016). Phosphorus

concentration in wastewater is more than 100mg/L then chemical precipitation method is

found economically feasible (Pastor et al., 2010; Ronteltap et al., 2010). Chemical

precipitation needs a precipitator which reacts with specific nutrient for precipitate formation

at pH more than 8 (Romero-Güiza et al., 2015; Ye et al., 2016; Zeng et al., 2018). Most

commonly used precipitators are Ca and Mg to form NH₄MgPO₄·6H₂O (struvite mineral)

and Ca5(PO4)3OH (Hydroxyapatite), respectively. Furthermore, Al and Fe not found suitable

because phosphate ions tightly bounded by recovered product, making it difficult for plats to

consume phosphate (Petzet & Cornel, 2012). Enhanced biological phosphorus removal

32
(EBPR) process is most commonly used for recovery of P (Valverde-Pérez et al., 2016).

Phosphate recovery depends upon phosphate accumulating organisms (PAOs), in an aerobic

environment PAOs accumulates huge polyphosphate, but phosphate is released in anaerobic

state from cells to wastewater (Zhao et al., 2015). Huge amount of phosphorus containing

surplus sludge is produce in this case. However, Excess sludge cannot be used for fertilizer

application as it contains toxic matter, heavy metals, and pathogens (Schoumans et al., 2015).

For N recovery, after stripping of ammonia with air/N2 from wastewater, salts such as

(NH4)2SO4 ammonium sulphate and (NH4)2CO3 ammonium carbonate are formed by

adsorption (Iskander et al., 2016; Kelly & He, 2014; Wu & Modin, 2013). The quality of

nutrient is greatly affected by coexisting metals and harmful toxic elements. Harmful and

heavy metals found in crystals of struvite, Arsenic concentration is found greater than 570

mg/kg, such struvite is not used for agricultural application. To enhance quality of nutrient it

is required to purify nutrient from foreign matter. Therefore, membranes technology is found

promising technique to enrich nutrients and have high-rejection for ions. No additional

chemicals and energy are required for membrane technology it’s a simple physical process.

Therefore, membrane separation is more economical then above discussed processes because

of no additional maintenance and operational cost. To get improved technical and economic

feasibility many processes like biological processes and chemical precipitation are

incorporated with membrane technology to make membrane hybrid systems (Ahn et al.,

2011; Gerardo et al., 2013; Gong et al., 2017; Ichihashi & Hirooka, 2012; Qiu & Ting, 2014;

Xie et al., 2014b; Zhang et al., 2013). To concentrate nutrients using membrane technology

FO, MD and ED are mainly used (Ahn et al., 2011; Xie et al., 2014a). Membrane bioreactor

is considered very effective for nutrients recovery (Qiu & Ting, 2014). Removal of organic

cause low membrane fouling in bioreactor. Using bioreactor can 1) decrease carbon footprint,

sludge production and size of equipment. 2) Increase sludge retention time and quality of

33
effluent. 3) No biological sedimentation unit ensure safety. Commonly used hybrid systems

are discussed in Table 1. Many studies have been done to recover resources from wastewater

and use them as fertilizer for food security and to eliminate impact wastewater impact on

environment (Ichihashi & Hirooka, 2012; Qiu & Ting, 2014). Hybrid systems of membrane

found promising technique because it concentrates nutrients with low foreign matter. Many

studies have been done on different schemes of hybrid systems for potential nutrient recovery

(Ansari et al., 2017; Darestani et al., 2017; Iskander et al., 2016; Jadhav et al., 2017; Kelly &

He, 2014; Nancharaiah et al., 2016; Neoh et al., 2016; Quist-Jensen et al., 2015; Xie et al.,

2016). But technical and economic feasibility of membrane hybrid systems are not discussed

properly.

The membrane-based hybrid system removes organics from feed source and recovers

nutrients hence fouling of membrane also decreases; as a result, efficiency of nutrient

recovery is improved. OMBR is formed by conventional MBR by replacing FO by UF/MF

(Huang et al., 2015). OMBR have several advantages over traditional MBR: 1) higher

rejection rate for impurities like nutrients, minerals and microbes. 2) low energy consumption

and membrane fouling. 3) High quality of treated water (Achilli et al., 2009; Alturki et al.,

2012; Neoh et al., 2016). 90% of nutrient recovered as struvite precipitate using OMBR-

based hybrid system from municipal wastewater (Qiu & Ting, 2014). In this case, nutrients

and FO membrane have high rejection rate for calcium, magnesium, and potassium like

mineral salts. Therefore Ca2+ and Mg2+ are not required for chemical precipitation. After

rejection through FO membrane, precipitates formed after reaction of minerals with nutrients

at higher pH greater than eight. Except nutrients that are bio assimilated by microorganisms

all the nutrients are recovered.

Modified OMBR hybrid system is developed by several authors for nutrient recovery.

MF membrane is integrated with OMBR hybrid scheme for phosphate recovery from

34
wastewater (Qiu et al., 2015) in such system both FO and MF membrane operate in parallel

(see Fig. 9). In this system phosphate and mineral salts, rejected by bioreactor are extracted

by MF membrane. Therefore, recovery of phosphate is done by Ca3(PO4)2 precipitates;

addition of Ca2+ ions is not required. The outcomes demonstrate that up to 98% and 70 mg/L

of phosphate can be recycled and enriched respectively. High concentration of mineral salts

and nutrients in feed cause precipitation in bioreactor by the reaction of ammonium,

phosphate and mineral salts like Calcium and Magnesium ion. In such scenario recovery of

nutrient may decreased. Chances of spontaneous precipitation could lower by increasing MF

flow rate (Qiu et al., 2015). Economic feasibility of process for phosphate recovery would be

enhanced by if MF extraction is operated at low permeate flux along with reduction in

fouling potential and energy reduction of MF membrane (Luo et al., 2016).

AnMBR holds great potential for nutrient recovery. In past few years, AnMBR have

developed rapidly and have been the object of sound investigation due to some unique

advantages like most of the P and N can be discharged as phosphate and ammonium,

respectively (Jensen, 2015). Low biomass yield for anaerobic microbes results in partial

removal of Nitrogen and Phosphorus through biomass growth (Smith et al., 2012). Moreover,

Technical and economic feasibility of AnMBR increases because of reduction in organic

matter and production of energy for nutrient recovery (Ozgun et al., 2013). (Smith et al.,

2012) examined AnMBR-based hybrid scheme for nutrient recovery using red meat

processing water and reported that 80% of phosphate and 90% ammonia are recovered.

Additionally, feed pH should be maintained low because as a result of high pH nitrogen can

be converted to ammonia, nutrients may loss (Jensen, 2015). Rising temperature increases

biological activity, therefore rise in temperature results in enrichment of nutrient by

microorganisms (Ozgun et al., 2013). (Ozgun et al., 2013) reported that the efficiency of

AnMBR might stay balanced at shifting organic loading rate beginning from 0.5 to 12.5 kg

35
COD/m3/d. Therefore, nutrients can be concentrated over a wide range of organic loadings

from various wastewater sources.

Anaerobic digestion also considered as a promising waste biomass treatment process.

Biomass waste is found to be great renewable resource (Appels et al., 2011). (Kumar et al.,

2016) reported that nearly 3950 Ml of crude oil is generated by using municipal solid waste,

sewage sludge and livestock waste. Anaerobic digestion process has potential to convert

biomass to 60-70% biogas. Anaerobic digestion can be used for production of biogas from

biomass, but nitrogen is unaffected from this process. Nitrogen mainly exists in form of NH4+

-N found in digested liquid. Digested liquid fertilizer can be directly applied to land

(Kocatürk-Schumacher et al., 2018).

Furthermore, anaerobic OMBR (AnOMBR) found to have additional benefits than

conventional AnMBR (Chen et al., 2014), key advantages are: a) fouling potential is lower

because of FO membrane, water permeation decreases by the compaction of foulant layer

(Lay et al., 2010; Liu et al., 2017b), b) concentration of dissolved methane in effluent is

reduced; and c) More is the removal and recovery efficiency of N, P and carbon (Martinez-

Sosa et al., 2011; Smith et al., 2013; Smith et al., 2012). (Hou et al., 2017)formed a set up by

installing microbial electrochemical setup with AnOMBR for making microbial recovery cell

(MRC)-AnOMBR arrangement. In such arrangement, mineral salts nutrients and nutrients are

extracted through AnOMBR solution by electricity that is derived from MRC; afterword for

nutrient recovery drives them to a separate solution. The generation of methane was more

than 0.19 L CH4/g COD along with 45% ammonium and 65% phosphate ion removal with

removal of organic up to 93%.

The biggest challenge using MBR hybrid systems is membrane fouling. Fouling

causes poor membrane performance, reduction in economic feasibility and increase in energy

consumption. High fouling reversibility and easy membrane cleaning is observed in FO

36
system (Ansari et al., 2017). Furthermore, in membrane-based hybrid systems possibility of

membrane fouling is low by the removal of organics such as antibiotics (Karaolia et al., 2017;

Wang et al., 2018). Antibiotics are removed using OMBR-based hybrid system and 77.7-

99.8% removal of antibiotics is observed (Raghavan et al., 2018). Salinity is a huge challenge

while implementing membrane hybrid system for nutrient recovery, which may decrease

water flux and disturb biotic activities (Qiu & Ting, 2013; Yap et al., 2012). In an OMBR-

hybrid system salinity can be controlled as for precipitation nutrients and mineral salts were

depleted. In OMBR-based hybrid system membrane fouling can also be overcome by using

FO membrane which can cause low membrane propensity (Yap et al., 2012), while osmotic

backwashing can also be applied on membrane surface to remove foulants (Achilli et al.,

2009). The concentration of dissolved phosphate and magnesium can be increased by

anaerobic digestion and ammonium by protein degradation (Lin et al., 2014), in such case

nutrient recovery is done by chemical precipitation. Membrane fouling can be decreased by

removing organics, however membrane‘s sensitivity to toxicity make it difficult for the

application of commercial AnMBRs at plant-scale.

37
 Membrane
wastewater Membrane
Hybrid Performance Overall cost Advantages Disadvantages References
source fouling
systems
BES-based Domestic Surface Concentration factor: Energy neutral Positive energy balance, Accumulation of recovered Chen et al,
wastewater fouling and ammonium (1.5) & low chemical consumption. nutrient on the cathode 2017
scaling phosphate (4.9) Recover chemical energy
stored in organic matter
MBR-based MWW Insignificant >95% of phosphate Draw solution, Additional Low fouling Qiu and Ting,
recovered NaOH 2014
FO-based SWW Cake layer >93% of ammonium and Draw solution, Manpower Low fouling propensity, Reverse salt flux, organics Wu et al.,
Urine formation >99% of phosphate costs, Energy high fouling reversibility, accumulation, reconcentration of 2018
recovered consumption of pump and high rejection rate for the draw solution,
stirrer nutrient
MD-based Biogas slurry Biofouling >98% of ammonia Vacuum pressure: 10kPa, High membrane selectivity membrane wetting, organics He et al.,
Swine recovered in 1.0 mol. N/L Feed temperature: 75 C for ammonia possibility of accumulation 2018
manure the renewable energy
utilized, low operating
pressure. Separate gas from
liquid phase
ED-based Synthetic N/A 78% of ammonium and Energy consumption: 0.08 High efficiency for nutrient High energy consumption, Shi et al.,
manure 75% of phosphate kWh/L of hydrolysate enrichment irreversible membrane fouling, 2018
recovered treated organic accumulation
AD-map Sewage N/A 90-99% P removed Have heavy metals and organic Uysal et al.,
method sludge contaminants 2010

Dow-HFO- municipal N/A . 94% of the removed Nutrients were Exchange capacity decreases after Mullen
Cu resin ion wastewater phosphate was concentrated in the initial regeneration
exchange recovered during regenerants and
media for regeneration recovered as
AnMBR precipitated struvite.
permeate highest phosphate
exchange capacity and
phosphate recovery

38
4. Challenges and future perspectives

In long term the present methods used have not many useful or fruitful results as

compared to the proposed method. It has some intermediate products biopolymer,

medium chain fatty acid, biohydrogen and some other valued product. COD removal and

methane conversion are one the biggest challenges and this method is very efficient and

promising for this purpose also being economical. However, some challenges are also

related to this process at this stage, the first one is the high energy demand from

membrane fouling, methane recovery and low COD/sulphate ratio (Aslam et al., 2018).

Methane recovery and control of membrane fouling should be studied and improved to

reduce energy consumption and process efficiency. Organics can be removed from the

membrane by biological activity with some biological processes such as BES and OMBR

based hydrogen system. With the basic advantage of reduced fouling in BES system some

other benefits are also present such as the pH elevation of nutrients recovery do not need

alkaline chemicals but in that place the cathode reaction can be used. One of the other

great advantage is positive energy balance. OMBR-based hybrid system also have some

of its benefits such as low membrane fouling and less energy consumption and high

rejection rate of minerals and salts (Visvanathan & Abeynayaka, 2012). In future to make

this process useable at plant and pilot scale the economical factor should be should be

studied along with nutrient recovery and some technical support. In overall review this

process is more energy efficient with less steps but membrane fouling and nutrients

recovery is a challenge which should be studied to make this process practically useable

and industrial level.

A large amount of gasses are produced from water treatment which become a part of

greenhouse gas. Methane is one of the major gas productions along with CO2 and N2O.

CO2 production is significantly lower in AnMBR than aerobic process. The methane is

39
produced in high amount and its solubility will increase as the temperature will decrease

(Cakir & Stenstrom, 2005). Therefore, more methane could leave the reactor in the form

of dissolved gas in the effluent. Thermo- dynamic gas–liquid equilibrium as defined by

Henry’s law. So, the methane gets dissolved with effluent and it is discharged in air

which causes global warming and it is one of the biggest issues to be studied regarding

AnMBR systems.

Low temperature is caused by the membrane fouling and it is one pf the biggest issue

to carry out the reaction properly. The basic solution to this can be the waste heat

recovery. Low bio gas production and membrane fouling is also an issue leading to the

salinity built and to distract the reaction for this sufficient organic supply and pre-treated

water should be used. Biochemical degradation and chemical degradation is also an issue

which can be solved by the membrane surface modification(Martinez-Sosa et al., 2011).

Figure 5.Membrane challenges and solutions.

40
5. Conclusions

Nutrients, organic loadings and mineral salts show enormous energy potential in domestic

wastewater and considered sustainable energy resource as well. Anaerobic membrane

biotechnology found to be promising technology and sustainable solution for bioenergy

production and resources recovery from wastewater. Nutrients like N and P have been shown

to be effectively recovered and concentrated and provide food security as a supplementary

source for fertilizer production. Membrane technology found potentially useful for

production of bioenergy and high concentration and productivity of nutrients can be achieved

by using this technology.

However, membrane fouling is the main challenge to make membrane process viable.

Membrane fouling can be potentially minimized by development of hybrid membrane

systems, fouling mechanisms, fouling control strategies and by formation of different

membrane configurations. Membrane hybrid systems in combination with low energy

resources recovery processes, offer an exciting opportunity to utilize wastewater sustainably.

Though, many of these hybrids systems are still immature and need further advancement to

make them economically efficient, reliable, technically feasible, scalable, and they must also

have minimal impact on the environment. Improvements in nutrient recovery efficiency,

separation of dissolved biohydrogen and biogas from effluent are the main issues requiring

further attention to for pilot scale application in future research.

41
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