This research was supported by the JSPS KAKENHI Grant Number (26420764, JP17K06892). The contribution of Ministry of Land, Insfrastructure, Transport and Tourism (MLIT), Government of Japan under &#8216;Construction Technology Research and Development Subsidy Program&#8217; to this research is also recognized. &#160;We also acknowledge the contribution of Mr. Kiyotaka Senmoto to this research. Ms. Adele Pitkeathly, Senior Writing Advisor Fellow from Writing Center of Hiroshima University is also acknowledged for English corrections and suggestions. This research was selected for oral presentation in 7th IWA-Aspire Conference, 2017 and Water and Environment Technology Conference, 2018.

CAUTION: Arsenic is extremely toxic. Please use gloves, long sleeve clothing, and experimental goggles at all times during the experiment to prevent any contact of arsenic solution with the skin and eyes. If arsenic comes into contact with any part of your body, wash it immediately with soap. Additionally, please clean up the experimental surroundings regularly so that you and others do not come into contact with arsenic, even when the experiment is not being performed. The symptoms of arsenic exposure may appear after a long period of time. Prior to cleaning the equipment, first rinse it with clean water and dispose the water separately into an experimental waste container designated for arsenic. Then, clean the equipment well with detergent. To prevent arsenic contamination of the environment, take precautions while disposing of arsenic samples. Dispose of them separately into experimental waste containers designated for arsenic. After the adsorption or desorption experiment is performed, the gels contain a high amount of arsenic. Therefore, dispose of the gels separately to a designated experimental waste bin for only arsenic-containing gels.
1. Synthesis of the DMAPAAQ+FeOOH gel composite
<ol>
	<li>Dry two 20 mL measuring flasks and two 20 mL beakers equipped with magnetic stir bars.</li>
	<li>Transfer 2.07 g of DMAPAAQ (75%), 0.15 g of N,N&#8217;-methylene bisacrylamide (MBAA), 0.25 g of sodium sulfite and 1.68 g of NaOH to one 20 mL beaker.</li>
	<li>Dissolve the solution wholly in distilled water as &#8216;solvent&#8217; and stirring it for 30 min with a magnetic stir bar.</li>
	<li>Transfer the mixture from the beaker to one 20 mL measuring flask and add distilled water to generate a 20 mL solution. Label the solution as the &#8220;monomer solution&#8221;.</li>
	<li>Similarly, take 0.27 g of ammonium peroxodisulfate (APS) and 3.78 g of FeCl3 in another 20 mL beaker.</li>
	<li>Dissolve the solution completely in distilled water and stirring it for 30 min with a magnetic stir bar.</li>
	<li>Transfer the mixture from the beaker to another 20 mL measuring flask and add distilled water to compose a 20 mL solution. Label the solution as the &#8220;initiator solution&#8221;.</li>
	<li>Prepare the experimental setup as shown in Figure 1.</li>
	<li>Transfer the solutions into the respective 20 mL separating funnels.</li>
	<li>Purge the solutions with N2 gas for 10 min.</li>
	<li>Mix the solutions together, stir them in a 50 mL test tube with an electric stirrer, and then place the mixture into a chiller maintained at 10 &#176;C for 40 min.</li>
	<li>Take out the gel block from the test tube and place it on a flat cutting board.</li>
	<li>Cut the gel block into a cubic shape, 5 mm in length.</li>
	<li>Soak the gel slices with de-ionized water for 24 h to remove the impurities.</li>
	<li>After 12 h, replace the water and soak the gel slices again.</li>
	<li>Spread the gel slices onto a Petri dish and dry them at room temperature for 24 h.</li>
	<li>Place the Petri dish with the gel slices in the oven at 50 &#176;C for 24 h.</li>
</ol>
2. pH sensitivity analyses
<ol>
	<li>Dry nine 40 mL plastic containers.</li>
	<li>Measure nine 20 mg dried gel pieces and put each of them in a separate 40 mL plastic container.</li>
	<li>Add 20 mL of a 4 mM disodium hydrogenarsenate heptahydrate (Na2HAsO4&#183;7H2O) solution to each container.</li>
	<li>To control the pH levels, add 20 mL of NaOH solution or HCL solution with different concentrations (0.1, 0.01, 0.001, 0.0001 M) in the respective containers to maintain pH levels of 2, 6, 8, 10, 12, 13 and label them.</li>
	<li>Keep the containers in the stirrer at 20 &#176;C and 120 rpm for 24 h.</li>
	<li>Collect a 5 mL sample from each container and place each sample in a plastic tube using a micropipette.</li>
	<li>Measure the equilibrium pH for all the samples.</li>
	<li>Measure the remaining concentration of arsenic in the solution using a high performance liquid chromatography (HPLC). Use an analytical column (4 x 200 mm), a guard column (4 x 50 mm) and a 4 mm suppressor with the following conditions: 
	Flowrate: 1.5 mL/min; 
	Amount of injected sample: 10 &#956;L; 
	Column temperature: 30 &#176;C; 
	Eluent solution: 2.7 mM Na2CO3 and 0.3 mM NaHCO3; 
	Pump pressure: 2000 psi; 
	Electric conductivity detection: Suppressor method. 
	NOTE: We procured 1 mL of the sample into a 1 mL single-use syringe. The syringe was coupled with a syringe membrane filter (pore size: 0.22 &#956;m, diameter: 13 mm) to discrete the microscopic fragments of the gel from the sample. About 0.7 mL of sample was instilled into the column. Distilled water was infused before the inception of injecting the samples as blank sample. Peaks denoting the existence of arsenic in the sample was detected at 13 min. 
	CAUTION: After injecting the sample, please leave the syringe into the suction head of HPLC for nearly 2 min with roughly 0.2-0.3 mL of sample remaining in it. Because the dust and air could penetrate the column and alter its adeptness, which possibly will result in erroneous outcome.</li>
</ol>
3. Arsenic adsorption experiment
<ol>
	<li>Dry five 40 mL plastic containers.</li>
	<li>Measure and place 20 mg of dried gel in each 40 mL plastic container.</li>
	<li>Add 40 mL of disodium hydrogenarsenate heptahydrate (Na2HAsO4&#183;7H2O) solution to each container at the following concentrations: 0.1, 0.2, 0.5, 1, 2 mM.</li>
	<li>Keep the containers in the stirrer at 20 &#176;C and 120 rpm for 24 h.</li>
	<li>Collect a 5 mL sample from each container and place in a plastic tube using a micropipette.</li>
	<li>Follow step 2.8 to assess the equilibrium arsenic levels in the solutions using HPLC.</li>
</ol>
4. Selectivity analyses of the DMAPAAQ+FeOOH gel
<ol>
	<li>Dry five 40 mL plastic containers.</li>
	<li>Place 20 mg of dried gel in each of the five 40 mL plastic containers.</li>
	<li>Add 20 mL of a 0.4 mM disodium hydrogenarsenate heptahydrate (Na2HAsO4&#183;7H2O) solution to each container.</li>
	<li>Add 20 mL at concentrations of 0.5, 1, 2, 5, 10 mM Na2SO4 to the five containers.</li>
	<li>Keep the containers in the stirrer at 20 &#176;C and 120 rpm for 24 h.</li>
	<li>Collect a 5 mL sample from each container and place into separate plastic tubes using micropipettes.</li>
	<li>Follow step 2.8 to quantify the remaining concentration of arsenic in the solution using HPLC.</li>
</ol>
5. Equilibrium rate analyses
<ol>
	<li>Dry seven 40 mL plastic containers.</li>
	<li>Place 20 mg of dried gel in each of the 40 mL plastic containers.</li>
	<li>Add 40 mL of a 0.2 mM disodium hydrogenarsenate heptahydrate (Na2HAsO4&#183;7H2O) solution to each of the containers.</li>
	<li>Keep the containers in the stirrer at 20 &#176;C at 120 rpm for the duration of their designated times.</li>
	<li>Collect 5 mL samples in plastic tubes using micropipettes after 0.5, 1, 3, 7, 11, 24, and 48 h.</li>
	<li>Follow step 2.8 to determine the equilibrium arsenic level in each solution using HPLC.</li>
</ol>
6. Regeneration analysis
<ol>
	<li>Adsorption analysis
	<ol>
		<li>Dry a 40 mL plastic container.</li>
		<li>Take 20 mg of dried gel and place it in the 40 mL plastic container.</li>
		<li>Add 40 mL of a 0.2 mM disodium hydrogenarsenate heptahydrate (Na2HAsO4&#183;7H2O) solution to the container.</li>
		<li>Keep the container in the stirrer at 20 &#176;C and 120 rpm for 24 h.</li>
		<li>Collect a 5 mL sample in a plastic tube using a micropipette.</li>
		<li>Refer to step 2.8 to evaluate the equilibrium arsenic level in the solution using HPLC.</li>
	</ol>
	</li>
	<li>Cleaning the gel
	<ol>
		<li>Obtain a mesh sieve.</li>
		<li>Carefully collect the gel pieces one at a time so that they do not break and place them in the mesh sieve.</li>
		<li>Wash the gel several times (minimum five times) using de-ionized water so that any remaining arsenic on the surface of the gel is washed away. 
		CAUTION: The gel pieces are fragile. Handle them with care while washing and transferring them from the arsenic solution to the NaCl solution.</li>
	</ol>
	</li>
	<li>Desorption analyses
	<ol>
		<li>Dry a 40 mL plastic container.</li>
		<li>Put the gel pieces from step 6.2 into a 40 mL plastic container.</li>
		<li>Add 40 mL of a 0.5 M NaCl solution to the container.</li>
		<li>Keep the container in the stirrer at 20 &#176;C and 120 rpm for 24 h.</li>
		<li>Collect a 5 mL sample in a plastic tube using a micropipette.</li>
		<li>Follow the step 2.8 to evaluate the equilibrium arsenic level in the solution using HPLC.</li>
	</ol>
	</li>
	<li>Repetition of the process
	<ol>
		<li>After collecting the gel from step 6.3, repeat the process in the following sequence for eight complete cycles: 6.2 &#62; 6.1 &#62; 6.2 &#62; 6.3 &#62; 6.2 &#62; 6.1 &#62; 6.2 &#62; 6.3.</li>
	</ol>
	</li>
</ol>

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The authors have nothing to disclose.

The main advancement of our developed method is the unique design strategy of the gel composite. The purpose of our gel preparation method was to maximize the amount of iron content in the gel. During the preparation, we added FeCl3 and NaOH to the &#8220;initiator solution&#8221; and the &#8220;monomer solution,&#8221; respectively. Once the monomer solution was mixed with the initiator solution, there was a reaction between FeCl3 and NaOH, producing FeOOH inside the gel. This phenomenon ensured maximum iron content in the gel composite. Despite the advantages of this method, the gel does not form under the following conditions: 1) When the solutions are not mixed thoroughly; 2) When the amount of FeCl3 exceeds 700 mol/m3 or the initiator, APS, and the accelerator, sodium sulfite, are lower.
If the gel does not form, add the initiator and accelerator gradually and mix the solution thoroughly. If the amount of initiator and accelerator are too high, the polymer structure of the gel differs, and the desired performance cannot be achieved. When the gel starts forming, stop mixing it to avoid distorting the gel.
Previous studies have reported ineffective adsorption of arsenic at neutral pH levels. Thus, the pH sensitivity experiment in the present work was important for indicating the practical applicability of the developed gel. Our studies demonstrate that the gel adsorbed arsenic effectively and was regenerated by NaCl at neutral pH levels. Although the adsorption amount of arsenic was high at acidic pH values and low at basic pH values, the adsorption was effective at neutral pH levels (Figure 4). To assess the adsorption behavior under real-life conditions, we conducted other experiments at neutral pH levels.
The relationship between the gel/arsenic solution contact times and arsenic adsorption amount was studied. The DMAPAAQ+FeOOH gel achieved adsorption equilibrium at 10 h (Figure 2). Additionally, we examined the rate of adsorption by the DMAPAAQ+FeOOH gel with the two kinetic models, pseudo first order and pseudo second order (Figure 3a,b). The correlation coefficients (R2) denoted the similarity between the experimental values and calculated values. We found that the R2 value was higher for the pseudo second order reaction kinetics. This finding suggests that the adsorption between the arsenic solution and DMAPAAQ+FeOOH gel is a chemisorption process19.
We performed the adsorption performance analyses at neutral pH levels. 20 mg of dry gel was immersed in the arsenic solution for 24 h at different concentrations of As(V). Figure 5 shows the amounts of arsenic adsorbed by the DMAPAAQ+FeOOH gel. These results were consistent with the Langmuir isotherm model of adsorption. The maximum adsorption amount by the gel reached 1.63 mM/g (Figure 5). Notably, the developed gel outperformed previously reported adsorbents studied at neutral pH levels. We rationalize this observation by the unique structure of the gel, which enables simultaneous arsenic adsorption by both the DMAPAAQ and FeOOH units. We found that 35.5% of arsenic was adsorbed by the amino group of the DMAPAAQ+FeOOH composite and 64.4% of arsenic was adsorbed by FeOOH particles15. During the adsorption process, make sure that the gel is immersed into the arsenic solution completely. The high levels of arsenic adsorption by the current gel over conventional and recently studied materials demonstrate its promising utility as a highly efficient adsorbent.
Selectivity is an important property of an adsorbent because there are many competing ions in water, including Cl&#8722;, HS&#8722;, SO32&#8722;, SO42&#8722;, H2CO3, HCO3&#8722;, and CO32&#8722; 20. The Hofmeister series suggests that the sulfate ion (SO42&#8722;) can disrupt hydrocarbon packing and penetrate the headgroup region of the monolayer of an adsorbent21. The concentration of sulfate in groundwater has been determined to be as high as 230 mg/L22. Therefore, if the developed gel can selectively adsorb arsenic with sulfate as a competing ion, it may be suitable for treating environmental groundwater. Thus, selectivity analyses with sulfate ions were performed and showed that the DMAPAAQ+FeOOH gel adsorbed arsenic effectively at high concentrations of sulfate (Figure 6). Since the adsorption amount of arsenic was similar in the absence or presence of sulfate ions, the gel may perform as effectively in groundwater as in the laboratory.
Regeneration is an important feature of any practical adsorbent because it ensures cost reductions, eco-friendliness, and usability23. The developed gel was regenerated successfully for eight consecutive days of experimentation (Figure 7). Additionally, 87.6% regeneration efficiency was achieved when the same gel was used for all eight adsorption-desorption cycles. One of the most important findings of our research was the use of NaCl in the desorption process. While NaOH is conventionally used for desorption, it can be harmful to human health. Therefore, we substituted NaOH for NaCl in our studies, which had not been reported previously.

Water pollution is a great environmental concern, motivating researchers to develop methods for removing contaminants such as arsenic from wastewaster1. Among all the reported methods, adsorption processes are a relatively low cost approach for heavy metal removal2,3,4,5,6,7. Iron oxyhydroxide powders are considered to be one of the most efficient adsorbents for extracting arsenic from aqueous solutions8,9. Still, these materials suffer from a number of drawbacks, including early saturation times and toxic synthetic precursors. Additionally, there is a severe adverse effect in the water quality when these adsorbents are used for a long period of time10. An additional separation process, such as sedimentation or filtration, is then needed to purify the contaminated water, which increases the cost of the production further8,11.
Recently, researchers have developed polymer gels such as cationic hydrogels, microgels, and cryogels that have demonstrated efficient adsorption properties. For example, an arsenic removal rate of 96% was achieved by the cationic cryogel, poly(3-acrylamidopropyl) trimethyl ammonium chloride [p(APTMACl)]12. Additionally, at pH 9, approximately 99.7% removal efficiency was achieved by this cationic hydrogel13. At pH 4, 98.72 mg/g of maximum arsenic adsorption capacity was achieved by the microgel, based on tris(2-aminoethyl) amine (TAEA) and glyceroldiglycidyl ether (GDE), p(TAEA-co-GDE)14. Although these gels demonstrated good adsorption performances, they failed to effectively remove arsenic from water at neutral pH levels, and their selectivities in all studied environments were not reported15. A maximum adsorption capacity of 227 &#956;g/g of was measured when Fe(III)-Sn(IV) mixed binary oxide-coated sand was used at a temperature of 313 K and a pH of 716. Alternatively, Fe-Zr binary oxide-coated sand (IZBOCS) has also been used to remove arsenic and achieved a maximum adsorption capacity of 84.75 mg/g at 318 K and a pH of 717. Other reported adsorbents suffer from low adsorption performances, lack of recyclability, low stability, high operational and maintenance costs, and the use of hazardous chemicals in the synthesis process4.
We sought to address the above limitations by developing a material with improved arsenic adsorption performance, high selectivity in complex environments, recycling capability, and efficient activity at neutral pH levels. Therefore, we developed a cationic gel composite of N,N-dimethylamino propylacrylamide methyl chloride quaternary (DMAPAAQ) gel and iron(III) hydroxide (FeOOH) particles as an adsorbent for arsenic removal. We chose to combine FeOOH with our gel because FeOOH increases the adsorption of both forms of arsenic18. In this study, our gel composite was designed to be non-porous and was impregnated with FeOOH during preparation. In the next section, the details of the gel preparation method, including our strategy for maximizing the content of FeOOH is discussed further.

<table>
	<tbody>
		<tr>
			<td>N,N&#8217;-dimethylamino propylacrylamide, methyl chloride quaternary (DMAPAAQ) (75% in H2O)</td>
			<td>KJ Chemicals Corporation, Japan</td>
			<td>150707</td>
			<td></td>
		</tr>
		<tr>
			<td>N,N&#8217;-Methylene bisacrylamide (MBAA)</td>
			<td>Sigma-Aldrich, USA</td>
			<td>1002040622</td>
			<td></td>
		</tr>
		<tr>
			<td>Sodium sulfite (Na2SO3)</td>
			<td>Nacalai Tesque, Inc., Japan</td>
			<td>31922-25</td>
			<td></td>
		</tr>
		<tr>
			<td>Sodium sulfate (Na2SO4)</td>
			<td>Nacalai Tesque, Inc., Japan</td>
			<td>31916-15</td>
			<td></td>
		</tr>
		<tr>
			<td>Di-sodium hydrogenarsenate heptahydrate(Na2HAsO4.7H20)</td>
			<td>Nacalai Tesque, Inc., Japan</td>
			<td>10048-95-0</td>
			<td></td>
		</tr>
		<tr>
			<td>Ferric chloride(FeCl3)</td>
			<td>Nacalai Tesque, Inc., Japan</td>
			<td>19432-25</td>
			<td></td>
		</tr>
		<tr>
			<td>Sodium hydroxide(NaOH)</td>
			<td>Kishida Chemicals Corporation, Japan</td>
			<td>000-75165</td>
			<td></td>
		</tr>
		<tr>
			<td>Ammonium peroxodisulfate (APS)</td>
			<td>Kanto Chemical Co. Inc., Japan</td>
			<td>907W2052</td>
			<td></td>
		</tr>
		<tr>
			<td>Hydrochloric acid (HCl)</td>
			<td>Kanto Chemical Co. Inc., Japan</td>
			<td>18078-01</td>
			<td></td>
		</tr>
		<tr>
			<td>Sodium Chloride (NaCl)</td>
			<td>Nacalai Tesque, Inc., Japan</td>
			<td>31320-05</td>
			<td></td>
		</tr>
	</tbody>
</table>

removal of arsenic using a cationic polymer gel impregnated with iron hydroxide

In this work, we prepared an adsorbent composed of a cationic polymer gel containing iron hydroxide in its structure designed to adsorb arsenic from groundwater. The gel we selected was the N,N-dimethylamino propylacrylamide methyl chloride quaternary (DMAPAAQ) gel. The objective of our preparation method was to ensure the maximum content of iron hydroxide in the structure of the gel. This design approach enabled simultaneous adsorption by both the polymer structure of the gel and the iron hydroxide component, thus, enhancing the adsorption capacity of the material. To examine the performance of the gel, we measured reaction kinetics, carried out pH sensitivity and selectivity analyses, monitored arsenic adsorption performance, and conducted regeneration experiments. We determined that the gel undergoes a chemisorption process and reaches equilibrium at 10 h. Moreover, the gel adsorbed arsenic effectively at neutral pH levels and selectively in complex ion environments, achieving a maximum adsorption volume of 1.63 mM/g. The gel could be regenerated with 87.6% efficiency and NaCl could be used for desorption instead of harmful NaOH. Taken together, the presented gel-based design method is an effective approach for constructing high-performance arsenic adsorbents.

Figure 1 describes the experimental setup for the preparation of the DMAPAAQ+FeOOH gel. Table 1 illustrates the compositions of the materials involved in the preparation of the gel.
Figure 2 shows the relation of contact time with the adsorption of arsenic by the DMAPAAQ+FeOOH gel. In the figure, the amount of adsorption of arsenic was examined at 0.5, 1, 3, 7, 11, 24, and 48 h. The results show that the adsorption of arsenic reaches its equilibrium after 10 h, and after 24 h of adsorption, minimal increase in the amount of adsorption of arsenic was detected.
Figure 3a,b shows the pseudo first order and pseudo second order reaction kinetics for arsenic adsorption by the DMAPAAQ+FeOOH gel. The results suggest that the correlation coefficients (R2) for pseudo first order and pseudo second order were 0.866 and 0.999, respectively.
Figure 4 shows the pH sensitivity of the DMAPAAQ+FeOOH gel. The same amount of dry DMAPAAQ+FeOOH gel (20 mg) was immersed in arsenic solutions (0.2 mM) at different pH levels for 24 h at 20 &#176;C and 120 rpm. The results suggest that the adsorption of arsenic was high at low and neutral pH levels and low at high pH levels.
Figure 5 shows the adsorption performance of DMAPAAQ+FeOOH. The same amount of dry DMAPAAQ+FeOOH gel (20 mg) was immersed in different arsenic solution concentrations (0.1, 0.2, 0.5. 1, 2 mM) at 20 &#176;C and 120 rpm for 24 h. The results show that the maximum arsenic adsorption capacity of the DMAPAAQ+FeOOH gel was 1.63 mM/g. The data were also consistent with the Langmuir isotherm.
Figure 6 shows the selectivity analysis of the DMAPAAQ+FeOOH gel. The same amount of dry DMAPAAQ+FeOOH gel (20 mg) was immersed in the arsenic solution (0.2 mM) with different SO42&#8722; concentrations (1, 2, 5, 10, 20 mM) at 20 &#176;C and 120 rpm for 24 h. The analysis shows that the adsorption amount of arsenic decreased slightly with an increase in SO42&#8722; concentration; however, the change was small, and at high concentrations of SO42&#8722;, the gel still adsorbed arsenic effectively.
Figure 7 shows the regeneration experiment of the DMAPAAQ+FeOOH gel. The same amount of dry gel (20 mg) was used for eight consecutive days of experimentation. The experiment was conducted using a 0.2 mM arsenic solution at 20 &#176;C and 120 rpm for 24 h. To perform the desorption process, the gel was then washed and immersed into a 0.5 M NaCl solution at 20 &#176;C and 120 rpm for 24 h. The gel was regenerated successfully after eight days of continuous adsorption-desorption cycles. We calculated the regeneration efficiency from the adsorption data on day 1 and day 7; a regeneration efficiency of 87.6% was achieved.

<table border="1" fo:keep-together.within-page="1" fo:keep-with-next.within-page="always">
	<tbody>
		<tr>
			<td></td>
			<td>Chemical</td>
			<td>Quantity (mol/m3)</td>
		</tr>
		<tr>
			<td>Monomer</td>
			<td>DMAPAAQ</td>
			<td>500</td>
		</tr>
		<tr>
			<td>Crosslinker</td>
			<td>MBAA</td>
			<td>50</td>
		</tr>
		<tr>
			<td>Accelerator</td>
			<td>Sodium Sulfite</td>
			<td>80</td>
		</tr>
		<tr>
			<td></td>
			<td>Sodium Hydroxide (NaOH)</td>
			<td>2100</td>
		</tr>
		<tr>
			<td>Initiator</td>
			<td>Ammonium peroxodisulfate (APS)</td>
			<td>30</td>
		</tr>
		<tr>
			<td></td>
			<td>Ferric Chloride (FeCl3)</td>
			<td>700</td>
		</tr>
	</tbody>
</table>
Table 1: Composition of the DMAPAAQ+FeOOH gel. This table has been adopted from Chemosphere [217, 808-815, doi: 10.1016/j.chemosphere.2018.11.050 (2019)]15 and details the materials used in preparing the DMAPAAQ+FeOOH gel.
<img alt="Figure 1" class="xfigimg" src="/files/ftp_upload/59728/59728fig1.jpg" /> 
Figure 1: Experimental setup for preparing the DMAPAAQ+FeOOH gel. This figure shows the arrangement of equipment for preparing the DMAPAAQ+FeOOH gel. Since our preparation method is unique, this figure will help researchers replicate our setup. <a href="https://www-jove-com.remotexs.ntu.edu.sg/files/ftp_upload/59728/59728fig1large.jpg" target="_blank">Please click here to view a larger version of this figure.</a>
<img alt="Figure 2" class="xfigimg" src="/files/ftp_upload/59728/59728fig2.jpg" /> 
Figure 2: Relating the contact time with the adsorption amount between the DMAPAAQ+FeOOH gel and arsenic solution. This figure has been modified from Chemosphere [217, 808-815, doi: 10.1016/j.chemosphere.2018.11.050 (2019)]15 and shows the relationship between the adsorption amount of arsenic by the DMAPAAQ+FeOOH gel and the contact time. Additionally, it illustrates the time required for the gel to reach its adsorption equilibrium. <a href="https://www-jove-com.remotexs.ntu.edu.sg/files/ftp_upload/59728/59728fig2large.jpg" target="_blank">Please click here to view a larger version of this figure.</a>
<img alt="Figure 3" class="xfigimg" src="/files/ftp_upload/59728/59728fig3.jpg" /> 
Figure 3: Arsenic adsorption reaction kinetics of the DMAPAAQ+FeOOH gel. (a) Pseudo first order. (b) Pseudo second order. This figure has been modified from Chemosphere [217, 808-815, doi: 10.1016/j.chemosphere.2018.11.050 (2019)]15 and shows the suitability of the kinetic model to the DMAPAAQ+FeOOH gel. <a href="https://www-jove-com.remotexs.ntu.edu.sg/files/ftp_upload/59728/59728fig3large.jpg" target="_blank">Please click here to view a larger version of this figure.</a>
<img alt="Figure 4" class="xfigimg" src="/files/ftp_upload/59728/59728fig4.jpg" /> 
Figure 4: pH sensitivity analysis of the DMAPAAQ+FeOOH gel. This figure has been adopted from Chemosphere [217, 808-815, doi: 10.1016/j.chemosphere.2018.11.050 (2019)]15 and shows the results of the pH sensitivity analysis of the DMAPAAQ+FeOOH gel in arsenic solutions. <a href="https://www-jove-com.remotexs.ntu.edu.sg/files/ftp_upload/59728/59728fig4large.jpg" target="_blank">Please click here to view a larger version of this figure.</a>
<img alt="Figure 5" class="xfigimg" src="/files/ftp_upload/59728/59728fig5.jpg" /> 
Figure 5: Adsorption performance of the DMAPAAQ+FeOOH gel. This figure has been modified from Chemosphere [217, 808-815, doi: 10.1016/j.chemosphere.2018.11.050 (2019)]15 and shows the arsenic adsorption amount by the DMAPAAQ+FeOOH gel at different concentrations of arsenic and the fitting of these data with the Langmuir isotherm model. <a href="https://www-jove-com.remotexs.ntu.edu.sg/files/ftp_upload/59728/59728fig5large.jpg" target="_blank">Please click here to view a larger version of this figure.</a>
<img alt="Figure 6" class="xfigimg" src="/files/ftp_upload/59728/59728fig6.jpg" /> 
Figure 6: Selectivity analysis of the DMAPAAQ+FeOOH gel. This figure has been modified from Chemosphere [217, 808-815, doi: 10.1016/j.chemosphere.2018.11.050 (2019)]15 and shows the arsenic adsorption selectivity of the DMAPAAQ+FeOOH gel in the presence of different concentrations of sulfate ions. <a href="https://www-jove-com.remotexs.ntu.edu.sg/files/ftp_upload/59728/59728fig6large.jpg" target="_blank">Please click here to view a larger version of this figure.</a>
<img alt="Figure 7" class="xfigimg" src="/files/ftp_upload/59728/59728fig7.jpg" /> 
Figure 7: Regeneration analysis of the DMAPAAQ+FeOOH gel. This figure has been adopted from Chemosphere [217, 808-815, doi: 10.1016/j.chemosphere.2018.11.050 (2019)]15. The reusability of the DMAPAAQ+FeOOH gel was examined for eight continuous days using arsenic solutions for adsorption and NaCl for desorption processes. <a href="https://www-jove-com.remotexs.ntu.edu.sg/files/ftp_upload/59728/59728fig7large.jpg" target="_blank">Please click here to view a larger version of this figure.</a>

Watch this Scientific Journal Video about Removal of Arsenic Using a Cationic Polymer Gel Impregnated with Iron Hydroxide at JoVE.com

Removal of Arsenic Using a Cationic Polymer Gel Impregnated with Iron Hydroxide

In this work, we prepared an adsorbent composed of the cationic N,N-dimethylamino propylacrylamide methyl chloride quaternary (DMAPAAQ) polymer gel and iron hydroxide for adsorbing arsenic from groundwater. The gel was prepared via a novel method designed to ensure the maximum content of iron particles in its structure.

In this work, we prepared an adsorbent composed of a cationic polymer gel containing iron hydroxide in its structure designed to adsorb arsenic from ...

removal-arsenic-using-cationic-polymer-gel-impregnated-with-iron

Nanyang Technological University

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7.4K Views.  Hiroshima University. In this work, we prepared an adsorbent composed of the cationic N,N-dimethylamino propylacrylamide methyl chloride quaternary (DMAPAAQ) polymer gel and iron hydroxide for adsorbing arsenic from groundwater. The gel was prepared via a novel method designed to ensure the maximum content of iron particles in its structure.

Video: Removal of Arsenic Using a Cationic Polymer Gel Impregnated with Iron Hydroxide

Automated Gel Size Selection to Improve the Quality of Next-generation Sequencing Libraries Prepared from Environmental Water Samples

Next-generation sequencing of environmental samples can be challenging because of the variable DNA quantity and quality in these samples. High quality DNA libraries are needed for optimal results from next-generation sequencing. Environmental samples such as water may have low quality and quantities of DNA as well as contaminants that co-precipitate with DNA. The mechanical and enzymatic processes involved in extraction and library preparation may further damage the DNA. Gel size selection enables purification and recovery of DNA fragments of a defined size for sequencing applications. Nevertheless, this task is one of the most time-consuming steps in the DNA library preparation workflow. The protocol described here enables complete automation of agarose gel loading, electrophoretic analysis, and recovery of targeted DNA fragments. 
In this study, we describe a high-throughput approach to prepare high quality DNA libraries from freshwater samples that can be applied also to other environmental samples. We used an indirect approach to concentrate bacterial cells from environmental freshwater samples; DNA was extracted using a commercially available DNA extraction kit, and DNA libraries were prepared using a commercial transposon-based protocol. DNA fragments of 500 to 800 bp were gel size selected using Ranger Technology, an automated electrophoresis workstation. Sequencing of the size-selected DNA libraries demonstrated significant improvements to read length and quality of the sequencing reads.

This manuscript describes an automated gel size selection approach for purifying DNA fragments for next-generation sequencing. The Ranger Technology provides complete automation of the entire process of agarose gel loading, electrophoretic analysis, and recovery of targeted DNA fragments allowing for high-throughput and high quality next-generation sequencing libraries.

Next-generation sequencing of environmental samples can be challenging because of the variable DNA quantity and quality in these samples. High quality DNA ...

Laboratory Simulation of an Iron(II)-rich Precambrian Marine Upwelling System to Explore the Growth of Photosynthetic Bacteria

A conventional concept for the deposition of some Precambrian Banded Iron Formations (BIF) proceeds on the assumption that ferrous iron [Fe(II)] upwelling from hydrothermal sources in the Precambrian ocean was oxidized by molecular oxygen [O2] produced by cyanobacteria. The oldest BIFs, deposited prior to the Great Oxidation Event (GOE) at about 2.4 billion years (Gy) ago, could have formed by direct oxidation of Fe(II) by anoxygenic photoferrotrophs under anoxic conditions. As a method for testing the geochemical and mineralogical patterns that develop under different biological scenarios, we designed a 40 cm long vertical flow-through column to simulate an anoxic Fe(II)-rich marine upwelling system representative of an ancient ocean on a lab scale. The cylinder was packed with a porous glass bead matrix to stabilize the geochemical gradients, and liquid samples for iron quantification could be taken throughout the water column. Dissolved oxygen was detected non-invasively via optodes from the outside. Results from biotic experiments that involved upwelling fluxes of Fe(II) from the bottom, a distinct light gradient from top, and cyanobacteria present in the water column, show clear evidence for the formation of Fe(III) mineral precipitates and development of a chemocline between Fe(II) and O2. This column allows us to test hypotheses for the formation of the BIFs by culturing cyanobacteria (and in the future photoferrotrophs) under simulated marine Precambrian conditions. Furthermore we hypothesize that our column concept allows for the simulation of various chemical and physical environments &#8212; including shallow marine or lacustrine sediments.

Laboratory Simulation of an IronII-rich Precambrian Marine Upwelling System to Explore the Growth of Photosynthetic Bacteria

We simulated a Precambrian ferruginous marine upwelling system in a lab-scale vertical flow-through column. The goal was to understand how geochemical profiles of O2 and Fe(II) evolve as cyanobacteria produce O2. The results show the establishment of a chemocline due to Fe(II) oxidation by photosynthetically produced O2.

A conventional concept for the deposition of some Precambrian Banded Iron Formations (BIF) proceeds on the assumption that ferrous iron [Fe(II)] upwelling ...

Biofilm Removal Using Carbon Dioxide Aerosols without Nitrogen Purge

Biofilms can cause serious concerns in many applications. Not only can they cause economic losses, but they can also present a public health hazard. Therefore, it is highly desirable to remove biofilms from surfaces. Many studies on CO2 aerosol cleaning have employed nitrogen purges to increase biofilm removal efficiency by reducing the moisture condensation generated during the cleaning. However, in this study, periodic jets of CO2 aerosols without nitrogen purges were used to remove Pseudomonas putida biofilms from polished stainless steel surfaces. CO2 aerosols are mixtures of solid and gaseous CO2 and are generated when high-pressure CO2 gas is adiabatically expanded through a nozzle. These high-speed aerosols were applied to a biofilm that had been grown for 24 hr. The removal efficiency ranged from 90.36% to 98.29% and was evaluated by measuring the fluorescence intensity of the biofilm as the treatment time was varied from 16 sec to 88 sec. We also performed experiments to compare the removal efficiencies with and without nitrogen purges; the measured biofilm removal efficiencies were not significantly different from each other (t-test, p &gt; 0.55). Therefore, this technique can be used to clean various bio-contaminated surfaces within one minute.

Biofilms on surfaces can be effectively and rapidly removed by using a periodic jet of carbon dioxide aerosols without a nitrogen purge.

Biofilms can cause serious concerns in many applications. Not only can they cause economic losses, but they can also present a public health hazard. ...

Protocol for Microplastics Sampling on the Sea Surface and Sample Analysis

Microplastic pollution in the marine environment is a scientific topic that has received increasing attention over the last decade. The majority of scientific publications address microplastic pollution of the sea surface. The protocol below describes the methodology for sampling, sample preparation, separation and chemical identification of microplastic particles. A manta net fixed on an &#187;A frame&#171; attached to the side of the vessel was used for sampling. Microplastic particles caught in the cod end of the net were separated from samples by visual identification and use of stereomicroscopes. Particles were analyzed for their size using an image analysis program and for their chemical structure using ATR-FTIR and micro FTIR spectroscopy. The described protocol is in line with recommendations for microplastics monitoring published by the Marine Strategy Framework Directive (MSFD) Technical Subgroup on Marine Litter. This written protocol with video guide will support the work of researchers that deal with microplastics monitoring all over the world.

The protocol below describes the methodology for: microplastics sampling on the sea surface, separation of microplastic and chemical identification of particles. This protocol is in line with the recommendations for microplastics monitoring published by the MSFD Technical Subgroup on Marine Litter.

Microplastic pollution in the marine environment is a scientific topic that has received increasing attention over the last decade. The majority of ...

Determination of Inorganic Arsenic in a Wide Range of Food Matrices using Hydride Generation - Atomic Absorption Spectrometry.

The European Food Safety Authority (EFSA) underlined in its Scientific Opinion on Arsenic in Food that in order to support a sound exposure assessment to inorganic arsenic through diet, information about distribution of arsenic species in various food types must be generated. A method, previously validated in a collaborative trial, has been applied to determine inorganic arsenic in a wide variety of food matrices, covering grains, mushrooms and food of marine origin (31 samples in total). The method is based on detection by flow injection-hydride generation-atomic absorption spectrometry of the iAs selectively extracted into chloroform after digestion of the proteins with concentrated HCl. The method is characterized by a limit of quantification of 10 &#181;g/kg dry weight, which allowed quantification of inorganic arsenic in a large amount of food matrices. Information is provided about performance scores given to results obtained with this method and which were reported by different laboratories in several proficiency tests. The percentage of satisfactory results obtained with the discussed method is higher than that of the results obtained with other analytical approaches.

The usefulness of an analytical method to determine inorganic arsenic in a wide range of food matrices is demonstrated. The method consists of selective extraction of inorganic arsenic into chloroform with a final determination by hydride generation-atomic absorption spectrometry.

The European Food Safety Authority (EFSA) underlined in its Scientific Opinion on Arsenic in Food that in order to support a sound exposure assessment to ...

On-Site Molecular Detection of Soil-Borne Phytopathogens Using a Portable Real-Time PCR System

On-site diagnosis of plant diseases can be a useful tool for growers for timely decisions enabling the earlier implementation of disease management strategies that reduce the impact of the disease. Presently in many diagnostic laboratories, the polymerase chain reaction (PCR), particularly real-time PCR, is considered the most sensitive and accurate method for plant pathogen detection. However, laboratory-based PCRs typically require expensive laboratory equipment and skilled personnel. In this study, soil-borne pathogens of potato are used to demonstrate the potential for on-site molecular detection. This was achieved using a rapid and simple protocol comprising of magnetic bead-based nucleic acid extraction, portable real-time PCR (fluorogenic probe-based assay). The portable real-time PCR approach compared favorably with a laboratory-based system, detecting as few as 100 copies of DNA from Spongospora subterranea. The portable real-time PCR method developed here can serve as an alternative to laboratory-based approaches and a useful on-site tool for pathogen diagnosis.

Rapid and accurate detection of plant pathogens on-site, especially soil-borne pathogens, is crucial to prevent further inoculum production and proliferation of plant diseases in the field. The method developed here using a portable real-time PCR detection system enables on-site diagnosis under field conditions.

On-site diagnosis of plant diseases can be a useful tool for growers for timely decisions enabling the earlier implementation of disease management ...

Optimized Procedure for Determining the Adsorption of Phosphonates onto Granular Ferric Hydroxide using a Miniaturized Phosphorus Determination Method

This paper introduces a procedure to investigate the adsorption of phosphonates onto iron-containing filter materials, particularly granular ferric hydroxide (GFH), with little effort and high reliability. The phosphonate, e.g., nitrilotrimethylphosphonic acid (NTMP), is brought into contact with the GFH in a rotator in a solution buffered by an organic acid (e.g., acetic acid) or Good buffer (e.g., 2-(N-morpholino)ethanesulfonic acid) [MES] and N-cyclohexyl-2-hydroxyl-3-aminopropanesulfonic acid [CAPSO]) in a concentration of 10 mM for a specific time in 50 mL centrifuge tubes. Subsequently, after membrane filtration (0.45 &#181;m pore size), the total phosphorus (total P) concentration is measured using a specifically developed determination method (ISOmini). This method is a modification and simplification of the ISO 6878 method: a 4 mL sample is mixed with H2SO4 and K2S2O8 in a screw cap vial, heated to 148-150 &#176;C for 1 h and then mixed with NaOH, ascorbic acid and acidified molybdate with antimony(III) (final volume of 10 mL) to produce a blue complex. The color intensity, which is linearly proportional to the phosphorus concentration, is measured spectrophotometrically (880 nm). It is demonstrated that the buffer concentration used has no significant effect on the adsorption of phosphonate between pH 4 and 12. The buffers, therefore, do not compete with the phosphonate for adsorption sites. Furthermore, the relatively high concentration of the buffer requires a higher dosage concentration of oxidizing agent (K2S2O8) for digestion than that specified in ISO 6878, which, together with the NaOH dosage, is matched to each buffer. Despite the simplification, the ISOmini method does not lose any of its accuracy compared to the standardized method.

This paper introduces a procedure to investigate the adsorption of phosphonates onto iron-containing filter materials, particularly granular ferric hydroxide, with little effort and high reliability. In a buffered solution, the phosphonate is brought into contact with the adsorbent using a rotator and then analyzed via a miniaturized phosphorus determination method.

This paper introduces a procedure to investigate the adsorption of phosphonates onto iron-containing filter materials, particularly granular ferric ...

Assessing the Particulate Matter Removal Abilities of Tree Leaves

Based on the conventional cleaning methods (water cleaning (WC) + brush cleaning (BC)), this study evaluated the influence of ultrasonic cleaning (UC) on collecting various sized particulate matter (PM) retained on leaf surfaces. We further characterized the retention efficiency of leaves to various sized PM, which will help to assess the abilities of urban trees to remove PM from ambient air quantitatively. 
Taking three broadleaf tree species (Ginkgo biloba, Sophora japonica, and Salix babylonica) and two needleleaf tree species (Pinus tabuliformis and Sabina chinensis) as the research objects, leaf samples were collected 4 days (short PM retention period) and 14 days (long PM retention period) after the latest rainfall. PM retained on the leaf surfaces was collected by means of WC, BC, and UC in sequence. Then, retention efficiencies of leaves (AEleaf) to three types of the various sized PM, including easily removable PM (ERP), difficult-to-remove PM (DRP), and totally removable PM (TRP), were calculated. Only around 23%-45% of the total PM retained on leaves could be cleaned off and collected by WC. When the leaves were cleaned through WC+BC, the underestimation of the PM retention capacity of different tree species was in the range of 29%-46% for various sized PM. Almost all PM retained on leaves could be removed if UC was supplemented to WC+BC. 
In conclusion, if the UC was complemented after the conventional cleaning methods, more PM on leaf surfaces could be eluted and collected. The procedure developed in this study can be used for assessing the PM removal abilities of different tree species.

The ultrasonic cleaning method was applied to elute the particulate matter (PM) retained on leaf surfaces after PM was eluted by the conventional cleaning methods (water cleaning only or water cleaning plus brush cleaning). The methodology can help to improve the estimation accuracy for PM retention capacity of leaves.

Based on the conventional cleaning methods (water cleaning (WC) + brush cleaning (BC)), this study evaluated the influence of ultrasonic cleaning (UC) on ...

Quantifying Plant Soluble Protein and Digestible Carbohydrate Content, Using Corn (Zea mays) As an Exemplar

Elemental data are commonly used to infer plant quality as a resource to herbivores. However, the ubiquity of carbon in biomolecules, the presence of nitrogen-containing plant defensive compounds, and variation in species-specific correlations between nitrogen and plant protein content all limit the accuracy of these inferences. Additionally, research focused on plant and/or herbivore physiology require a level of accuracy that is not achieved using generalized correlations. The methods presented here offer researchers a clear and rapid protocol for directly measuring plant soluble proteins and digestible carbohydrates, the two plant macronutrients most closely tied to animal physiological performance. The protocols combine well characterized colorimetric assays with optimized plant-specific digestion steps to provide precise and reproducible results. Our analyses of different sweet corn tissues show that these assays have the sensitivity to detect variation in plant soluble protein and digestible carbohydrate content across multiple spatial scales. These include between-plant differences across growing regions and plant species or varieties, as well as within-plant differences in tissue type and even positional differences within the same tissue. Combining soluble protein and digestible carbohydrate content with elemental data also has the potential to provide new opportunities in plant biology to connect plant mineral nutrition with plant physiological processes. These analyses also help generate the soluble protein and digestible carbohydrate data needed to study nutritional ecology, plant-herbivore interactions and food-web dynamics, which will in turn enhance physiology and ecological research.

Quantifying Plant Soluble Protein and Digestible Carbohydrate Content, Using Corn Zea mays As an Exemplar

The protocols described herein provide a clear and approachable methodology for measuring soluble protein and digestible (non-structural) carbohydrate content in plant tissues. The ability to quantify these two plant macronutrients has significant implications for advancing the fields of plant physiology, nutritional ecology, plant-herbivore interactions and food-web ecology.

Elemental data are commonly used to infer plant quality as a resource to herbivores. However, the ubiquity of carbon in biomolecules, the presence of ...

Separation of Spinach Thylakoid Protein Complexes by Native Green Gel Electrophoresis and Band Characterization using Time-Correlated Single Photon Counting

The light reactions of photosynthesis are carried out by a series of pigmented protein complexes in the thylakoid membranes. The stoichiometry and organization of these complexes is highly dynamic on both long and short time scales due to processes that adapt photosynthesis to changing environmental conditions (i.e., non-photochemical quenching, state transitions, and the long-term response). Historically, these processes have been described spectroscopically in terms of changes in chlorophyll fluorescence, and spectroscopy remains a vital method for monitoring photosynthetic parameters. There are a limited number of ways in which the underlying protein complex dynamics can be visualized. Here we describe a fast and simple method for the high-resolution separation and visualization of thylakoid complexes, native green gel electrophoresis. This method is coupled with time-correlated single photon counting for detailed characterization of the chlorophyll fluorescence properties of bands separated on the green gel.

Here we present a protocol to separate solubilized thylakoid complexes by Native Green Gel electrophoresis. Green gel bands are subsequently characterized by Time Correlated Single Photon Counting (TCSPC) and basic steps for data analysis are provided.