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Inhibitory Effects of Appropriate Addition of Zero-Valent Iron on NH3 and H2S Emissions during Sewage Sludge Composting

by 1,2, 1,2,3, 1,2,*, 1,2 and 1,2
Institute of Geographic Sciences and Natural Resources Research, Chinese Academy of Sciences, Beijing 100101, China
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
Guoneng Longyuan Environmental Co., Ltd., Beijing 100039, China
Author to whom correspondence should be addressed.
Agriculture 2022, 12(12), 2002;
Received: 22 October 2022 / Revised: 19 November 2022 / Accepted: 22 November 2022 / Published: 24 November 2022
(This article belongs to the Section Agricultural Technology)


Large amounts of NH3 and H2S are emitted during sewage sludge composting, resulting in odor pollution. This composting experiment was carried out using sewage sludge mixed with sawdust, and different amounts of zero-valent iron (ZVI) were added to investigate the effect on volatile gases, such as NH3 and H2S, and to analyze the effect on the available sulfur, total sulfur, moisture content, and germination index of the compost. The results showed that the addition of ZVI during the composting process had noticeable effects on the emission of NH3 and H2S. ZVI could also increase the heating rate and peak temperature of the pile, reduce the available sulfur loss, and promote the dewatering and decomposition of the compost pile. The addition of 3% ZVI had the best effect on NH3 emissions; it reduced the peak concentration of NH3 release during composting by 21.0% compared to the blank group. However, the addition of 2% ZVI was the most effective for H2S emissions; it reduced the peak release concentration of H2S by 20.0%. A higher addition of ZVI was more effective in reducing the moisture content and increasing the germination index of the compost.

1. Introduction

With the rapid development of urbanization, the amount of urban wastewater treatment is increasing, and the amount of sewage sludge is also increasing year by year. Composting is a common method of treating sewage sludge [1]. After the composting process, the biodegradable organic matter and water content of the sludge are reduced, and pathogens are inactivated [2]. However, some odorous gases are released during the composting process, which not only contributes to odor pollution but also causes nutrient loss from composted products [3,4]. Odor pollution has become an important restriction for the development of the compost industry in China [5]. Among the odorous gases, much attention has been focused on NH3 and H2S because of their high emissions and low olfactory threshold [6,7]. Currently, there are three main types of methods to control odor contamination in composting [8]: controlling the C/N ratio, moisture content, and pH of the compost raw materials [9,10]; selecting suitable exogenous additives such as sucrose and phosphate buffer [2,11]; and controlling composting process factors, such as temperature, oxygen content, and ventilation [12,13]. Exogenous additives have been widely used in many composting facilities because of their low investment costs and ease of application. However, there are still problems of limited variety and mediocre results; therefore, new additives need to be explored to achieve effective control of odor emissions during the composting process.
Many studies have been conducted on zero-valent iron (ZVI) for controlling H2S emissions during anaerobic digestion. The main mechanism is that under anaerobic conditions, ZVI is oxidized, thus releasing Fe2+, which generates FeS precipitation with a very small Ksp with S2− [14]. Furthermore, high-valent iron can reduce the conversion of sulfate to H2S by inhibiting the activity of sulfate-reducing bacteria (SRB), resulting in reduced H2S emissions [15,16]. In other words, the control of H2S by ZVI during anaerobic digestion is achieved by conversion to the higher-valent iron. Theoretically, the conversion of ZVI to higher-valent iron is more likely to occur in the aerobic composting processes than in the anaerobic digestion; therefore, it may also be able to control H2S. However, it is worth pointing out that the addition of ZVI, a reducing substance, may exacerbate the anaerobic environment in some areas within the composting system and increase the production of malodorous gases. Moreover, the addition of iron salts reduces nitrogen loss during composting [17,18]. If ZVI has the same effect, it may be a more suitable additive because it is cheaper and more easily available than iron salts. Furthermore, the addition of ZVI increases the iron content in the product, allowing for the use of compost products to increase soil fertility [19], resulting in increased environmental benefits.
According to relevant studies, we explored the addition of ZVI and analyzed its effects on NH3 and H2S emissions during the sewage sludge composting process, and we investigated its effect on the nutrient content of the compost, dewatering effectiveness, and product maturation. The results of the study can provide a new approach to controlling odor pollution and improving product quality in actual sewage sludge composting.

2. Materials and Methods

2.1. Composting Materials

The sewage sludge was ex-factory sludge from a municipal wastewater treatment plant located in Zhengzhou, China, which was press-filtered and dewatered to a moisture content of approximately 80%. The compost conditioner was selected as loose sawdust with a low moisture content (approximately 10%). The mixing ratio of sewage sludge and sawdust was 10:3 (w/w). The ZVI powder (purity > 98%, 400 mesh) was obtained from Zhongyue Jiadun Industries Ltd. (China).

2.2. Composting Method and Device

The composting process was conducted using a small aerobic composting automatic control device as shown in Figure 1. In order to accurately describe the temperature of the composting process, the composting device was equipped with four temperature sensors at different depths. The effective volume of the device was 340 L. Intermittent ventilation was forced by fans with 20 min intervals per 1 min of operation. The ventilation rate was adjusted to 3 L/min. The composting process was as follows: sewage sludge, sawdust, and different amounts (1%, 2%, and 3%, based on the wet weight of the sewage sludge) of ZVI were mixed thoroughly and then added to the composting device. The pile without ZVI addition was used as a control group. The composting duration for this experiment was 15 days, and compost samples were sampled on days 0, 1, 2, 3, 4, 5, 7, 9, 11, 13, and 15, while H2S and NH3 were sampled and measured. Samples were obtained by mixing samples from the top, middle, and bottom of the composting tank.

2.3. Analytical Methods

The concentrations of NH3 and H2S were detected using a portable NH3 detector (B1010-NH3-SC, range 0–2000 ppm, accuracy 1 ppm) and a portable H2S detector (BW08-III, range 0–200 ppm, accuracy 0.1 ppm). The detectors for NH3 and H2S were calibrated with standard gases. The tests were carried out at 8:00 a.m. and 6:00 p.m., and at least one ventilation cycle was maintained at each test time. The moisture content was measured by drying fresh samples in an oven at 105 °C to a constant weight (approximately 8 h). Fresh samples were mixed with deionized water at a mass ratio of 1:10 (w/v) and then shaken completely for 2 h to obtain a water extract which was used to determine pH, electrical conductivity (EC), and seed germination index (GI). EC and pH were determined using an integrated pH–EC meter (Thermo Fisher Scientific, Waltham, MA, USA). The total sulfur content was measured by taking a dry sample, grinding it, and measuring it using an elemental analyzer (FLASH 2000, Thermo Fisher Scientific, USA). The available sulfur content was determined using a turbidimetric method [20]. The seed germination index (GI) was determined according to a previous study [21].

2.4. Statistical Analysis

All measurements were taken in triplicate. The mean and standard deviation of the experimental data were calculated using Microsoft Excel. The SPSS was used for statistical analyses, while the plots were prepared using OriginLab 2018. The results were tallied using a paired Student’s t-test when appropriate. The results are expressed as means, and differences of p < 0.05 were considered significant.

3. Results and Discussion

3.1. Effect of ZVI on the Temperature of the Composting Pile

Temperature directly impacts the microorganisms in the pile and microbial community structure, and it further affects the decomposition and decay process of organic matter [22]. The composting process must reach a relatively high temperature and last for a certain duration to ensure that pathogenic bacteria are destroyed. The temperature changes inside the piles with different amounts of ZVI are shown in Figure 2. The control group, as well as the groups with 1%, 2%, and 3% ZVI additions, all entered the high-temperature phase (above 55 °C) on day one. Their high-temperature stages were 4, 6, 6, and 7 days, respectively, all of which met the requirement of at least three days for the high-temperature stage of sludge composting according to the Standard for Stabilization of Municipal Wastewater Treatment Plant Sludge (CJ/T 510-2017). Compared to the control group, the piles with the addition of ZVI all demonstrated an increase in peak temperature and a prolongation of the high-temperature phase. The addition of an iron source accelerates the maturation of the compost and improves the quality of compost by forming the “acid–Fe–P” complex with the phosphate and the humic acid produced during the composting process [23]. The possible reasons for this are that iron oxides act as electron acceptors or donors to promote microbial growth and metabolism [24], as well as electron conductors to mediate electron transfer between microorganisms [24,25], increasing the rate of microbial metabolism of organic waste and promoting heat generation [26]. Consistent with the results of studies on similar composting with the addition of FeCl3 [27] and Fe(NO3)3 [18], the addition of ZVI was also able to increase the peak temperature of the compost. The addition of 2% ZVI resulted in the fastest warming of the pile and the highest peak temperature, indicating that this treatment was the most favorable for microbial metabolism. Although iron enhances the metabolic capacity of microorganisms, when the concentration is too high, it has an inhibitory effect on the activity of microorganisms [28,29], which may be why the temperature of the pile with 3% ZVI addition was not as high as that with 2% ZVI. Furthermore, the experimental results showed that the addition of ZVI increased the composting temperature on days 5–12, which was very beneficial to the composting process.

3.2. Effect of ZVI on NH3 Emission during the Composting Process

Figure 3 shows the variation of the NH3 concentrations emitted from the piles with different ZVI additions. Throughout the composting process, NH3 concentrations increased and then decreased, with the peak concentration occurring in the high-temperature phase of the compost. The NH3 released during this phase was also the main cause of nitrogen loss during composting, accounting for approximately 20–60% of the total nitrogen [30]. In the control group, as well as the groups with 1%, 2%, and 3% ZVI additions, the peak time of NH3 emission was observed on days 4, 7, 4, and 5, with peak concentrations of 827.0, 1408.4, 936.8, and 653.7 mg·m−3, respectively. The peak concentrations of NH3 emitted with the addition of 1% and 2% ZVI increased by 70.3% and 13.3%, respectively, whereas that of NH3 with the addition of 3% ZVI decreased by 21%, compared to the control group. Under the treatment of low (1% and 2%) ZVI addition, iron acted as a trace element to increase microbial activity, enhance pile temperature, promote organic matter degradation, and eventually increase the emission of NH3. In addition, the emission of NH3 is not only related to biological influences but also influenced by chemical factors [31], such as NH4+ concentration and pH value. NH3 (liquid) is continuously transferred to the phase interface of water and gas and evaporates as NH3 (gas) once the pKa of NH3/NH4+ exceeds 9.25 [32,33]. When 3% ZVI was added, the excess ZVI may have resulted in the inhibition of microbial activity, resulting in the pile temperature being not as high as that in the groups with 1% and 2% ZVI addition, thus reducing the emission of NH3 during the high-temperature phase. Meanwhile, a large amount of iron may undergo anaerobic ammonium oxidation coupled with iron reduction, termed Feammox [34] (6Fe(OH)3 + 2NH4+ + 10H+ → 6Fe2+ + 18H2O + N2), converting NH3 into high-valent-state nitrogen (N2, NO2, and NO3), which may be another reason for the reduction in NH3 emissions [35]. Of course, there needs to be further evidence as to whether this reaction or mechanism actually occurs.
The cumulative amounts of NH3 in the control group, as well as the groups with 1%, 2%, and 3% ZVI additions, were 641.5, 815.0, 1039.4, and 581.3 mg, respectively (Figure 3b). The cumulative emission of NH3 from the pile with 3% ZVI addition decreased by 9.4%, whereas that from the piles with 1% and 2% ZVI additions increased by 27% and 62%, respectively, compared with the control group. Although the mechanism via which ZVI controls NH3 emissions during composting was quite complex when combining the concentration and cumulative emission of NH3, it was still evident that the addition of 3% ZVI could inhibit NH3 emission.

3.3. Effect of ZVI on H2S Emission during the Composting Process

The variation in the H2S emission concentration under different ZVI additions is shown in Figure 3b. H2S is the most abundant sulfur-containing gas released during the sewage sludge composting process [36], and its release not only brings malodor but also causes the loss of elemental sulfur from the compost. The trend in H2S concentrations was similar, with peak concentrations at the beginning of the composting period and H2S emissions almost ceasing after 3 days. In the control group, the peak H2S emission occurred on day 1 with a concentration of 105.3 mg·m−3. In the group treated with 1% ZVI, the peak H2S emission occurred on day 2 with a concentration of 98.7 mg·m−3. In the group treated with 2% ZVI, the peak H2S emission occurred on day 1 with a concentration of 79.0 mg·m−3. In the group treated with 3% ZVI, the peak H2S emission occurred on day 1 with a concentration of 227.8 mg·m−3. Compared to the control group, the peak H2S concentration released from the piles with 1% and 2% ZVI addition decreased by 6.3% and 19.9%, respectively, while the peak H2S concentration released from the piles with 3% ZVI increased by 188.3%. In other studies [37], nitrates were used to reduce the release of hydrogen sulfide from sewage sludge composts, with the effect of reducing it by 20%. During the composting process, H2S is mainly generated through the reduction of sulfate by microorganisms and the decomposition of sulfur-containing substrates under anaerobic conditions. [38]. Sulfate-reducing bacteria (SRB) play a key role in this process, and their activity is influenced by the substrate (SO42−) concentration [39], product (reduced sulfides) concentration, and abundance of electron donors (organic carbon or H2) [40]. The concentration of H2S with 3% ZVI addition increased significantly compared with that from the control group, which may be attributed to the fact that excess ZVI greatly increases the biological activity of SRB and promotes the formation of reduced sulfides (H2S, HS, and S2−) [14,41]. However, the reduced sulfides failed to precipitate with Fe2+ or Fe3+, resulting in increased emission of H2S from the piles. The 1% and 2% ZVI additions were not effective in promoting SRB activity, and the H2S produced locally anaerobically could precipitate with sufficient Fe2+/Fe3+ in the piles, thereby not increasing H2S emission [42]. Moreover, the effect of ZVI on H2S removal is influenced by temperature and pH [43], which may be another reason for the significantly different effect of 3% ZVI addition on H2S emission compared to the 1% and 2% ZVI additions.
The cumulative amounts of H2S in the control group, as well as the groups with 1%, 2%, and 3% ZVI additions, were 28.5, 21.2, 24.4, and 56.4 mg, respectively (Figure 3d). Compared to the accumulation of H2S in the control group, the accumulation of H2S with 2% addition was reduced by 9.0%, while the accumulation of H2S with 1% and 3% addition was increased by 9% and 93%, respectively. Combining the H2S concentration and cumulative emissions, the appropriate (2%) addition of ZVI had a certain inhibitory effect on H2S emissions.

3.4. Effects of Adding ZVI on Total Sulfur and Available Sulfur Content

The total sulfur content continued to decrease throughout the composting cycle with the emission of volatile sulfides (Figure 4a). The total sulfur content of the compost decreased from 3.27, 3.43, 3.44, and 3.43 g/kg at the beginning to 2.60, 2.76, 2.82, and 2.69 g/kg at the end, respectively, for the control group, as well as the groups with 1%, 2%, and 3% ZVI additions. The total sulfur content decreased by 20.6%, 19.5%, 18.1%, and 21.5%, respectively. The results showed that the addition of 1% and 2% ZVI reduced the total sulfur loss from the compost. The reason for this result was related to the reduction of sulfide emissions. Furthermore, the migration and fraction changes of sulfur are influenced by the quantity and properties of the electron donor or acceptor in the composting process [44,45]. The addition of ZVI inevitably affects these processes, but the mechanism of action still needs to be explored in subsequent studies.
The available sulfur in compost is a direct reflection of the plant’s ability to supply sulfur. In all treatments, the available sulfur content of the pile showed a smooth increase, as shown in Figure 4b. In the control group, as well as the groups with 1%, 2%, and 3% ZVI additions, the available sulfur content increased from 1.21, 1.23, 1.46, and 1.42 g/kg at the beginning to 1.50, 1.73, 1.74, and 1.63 g/kg at the end, respectively, increasing by 23.7%, 40.7%, 19.5%, and 15.0%. The experimental results showed that the addition of 1% ZVI effectively increased the available sulfur content in the compost products, which coincided with the result that the treatment was optimal for reducing H2S emissions. In terms of available sulfur in the compost product, the addition of ZVI resulted in a higher concentration than the blank, indicating that the ZVI increased the concentration of available sulfur in the compost product.

3.5. Effect of Adding ZVI on Dewatering

Moisture content is one of the most important parameters in the composting process because it is critical to the physiological and metabolic activities of microorganisms [46,47]. Furthermore, the moisture content directly determines the speed of the aerobic composting reaction and the quality of compost products [48]. The moisture content of the control group, as well as the groups with 1%, 2%, and 3% ZVI additions, decreased from 64.4%, 63.3%, 62.3%, and 65.6% at the beginning to 63.7%, 57.0%, 60.6%, and 54.5% on day 15 (Figure 5), decreasing by 1.1%, 10.0%, 2.7%, and 16.9%, respectively. The reduction in the moisture content of the blank compost should not have been so low, and it is possible that other factors interfered with the sampling process at the end of the experiment. The results indicate that the addition of ZVI promoted the dewatering of the pile, and the addition of 3% ZVI had the best dewatering effect.

3.6. Effect of Adding ZVI on Maturity

The maturity of compost is the degree to which the organic matter in the compost is finally stabilized through the process of mineralization and decay. This evaluation is important for safe agricultural use, with common indicators such as GI, pH, and EC. GI is an index that assesses the phytotoxicity and stability of the compost by measuring relative germination and relative root growth rates. It is also considered to be the most sensitive and effective indicator for assessing compost decay [49]. In general, compost products are considered mature and stable when the GI exceeds 90% [50]. The GI values of the composts were all increased by the composting treatment, as shown in Figure 6. At the end of composting, the GI of the control group, as well as the groups with 1%, 2%, and 3% ZVI additions, were 96%, 119%, 120%, and 139%, respectively. The results showed that in terms of promoting seed germination, a higher addition of ZVI led to a more effective compost.
The pH and EC are also often used as indicators to assess the degree of decomposition. The pH is also an important factor in monitoring the composting process and is closely related to changes in compost composition [51]. Relevant research and industry standards suggest that a mature compost product should have a pH between 8 and 9 [51]. EC reflects the total ionic concentration of the composting leachate, i.e., the soluble salt content, thus characterizing the potential ionic toxicity to the crop [52]. During the composting process, microorganisms break down organic matter into small inorganic molecules which are soluble in water, thus increasing the EC of the compost. According to the relevant industry standards, mature compost products have an EC of no more than 4000 mS/cm. In the control group, as well as the groups with 1%, 2%, and 3% ZVI additions, the EC of the compost increased from 741, 734, 750, and 668 mS/cm at the beginning to 1295, 1252, 1287, and 1324 mS/cm on day 15, respectively (Figure 7b). Statistical analysis showed that there was no significant effect of zero-valent iron addition on material conductivity (p < 0.01). The results showed that the addition of ZVI had no significant effect on the pH and EC of the pile.

4. Conclusions

The addition of an appropriate amount of ZVI in the aerobic composting process of sewage sludge reduced the emissions of H2S and NH3. Furthermore, the addition of ZVI increased the available sulfur content of the compost product, reduced the loss of total sulfur, and promoted the maturation and dewatering of the compost. Under the ZVI addition conditions designed for this experiment, no negative effects of the ZVI addition on the composting process were observed. The experimental results showed that a greater addition of ZVI led to more favorable dewatering and decomposition in the aerobic composting process.

Author Contributions

Development and design of the methodology, G.Z.; data curation, Y.L., J.L. and Y.C.; writing—original draft preparation, Y.L., G.Z. and J.L.; writing—review and editing, Y.L., J.L., J.Y. and Y.C.; visualization, G.Z. and Y.L.; supervision, G.Z.; project administration, J.Y.; funding acquisition, G.Z. All authors have read and agreed to the published version of the manuscript.


This research was funded by the National Key Research and Development Program of China (2016YFC0401102).

Institutional Review Board Statement

Not applicable.

Data Availability Statement

Not applicable.


The authors are grateful for the financial support received from the National Key Research and Development Program of China (2016YFC0401102).

Conflicts of Interest

The authors declare no conflict of interest.


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Figure 1. Schematic of the aerobic composting automatic control device.
Figure 1. Schematic of the aerobic composting automatic control device.
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Figure 2. Changes in temperature of the composting pile with different ZVI additions. ZVI: zero-valent iron.
Figure 2. Changes in temperature of the composting pile with different ZVI additions. ZVI: zero-valent iron.
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Figure 3. Dynamics of NH3 (a) and H2S (c) emission and cumulative emission of NH3 (b) and H2S (d) from the composting pile under different ZVI additions. ZVI: zero-valent iron.
Figure 3. Dynamics of NH3 (a) and H2S (c) emission and cumulative emission of NH3 (b) and H2S (d) from the composting pile under different ZVI additions. ZVI: zero-valent iron.
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Figure 4. Changes in total sulfur (a) and available sulfur (b) content of the compost material under different ZVI additions. ZVI: zero-valent iron.
Figure 4. Changes in total sulfur (a) and available sulfur (b) content of the compost material under different ZVI additions. ZVI: zero-valent iron.
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Figure 5. Changes in moisture content of the compost material under different ZVI additions. ZVI: zero-valent iron.
Figure 5. Changes in moisture content of the compost material under different ZVI additions. ZVI: zero-valent iron.
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Figure 6. Germination index of sewage sludge compost under different ZVI additions. ZVI: zero-valent iron.
Figure 6. Germination index of sewage sludge compost under different ZVI additions. ZVI: zero-valent iron.
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Figure 7. Change in pH (a) and electrical conductivity (b) under different ZVI additions. ZVI: zero-valent iron.
Figure 7. Change in pH (a) and electrical conductivity (b) under different ZVI additions. ZVI: zero-valent iron.
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Liu, Y.; Liu, J.; Zheng, G.; Yang, J.; Cheng, Y. Inhibitory Effects of Appropriate Addition of Zero-Valent Iron on NH3 and H2S Emissions during Sewage Sludge Composting. Agriculture 2022, 12, 2002.

AMA Style

Liu Y, Liu J, Zheng G, Yang J, Cheng Y. Inhibitory Effects of Appropriate Addition of Zero-Valent Iron on NH3 and H2S Emissions during Sewage Sludge Composting. Agriculture. 2022; 12(12):2002.

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Liu, Yuan, Junwan Liu, Guodi Zheng, Junxing Yang, and Yuan Cheng. 2022. "Inhibitory Effects of Appropriate Addition of Zero-Valent Iron on NH3 and H2S Emissions during Sewage Sludge Composting" Agriculture 12, no. 12: 2002.

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