Research progress in preparation of nanowires for selective removal of impurity anions in sewage

Guangfei Qu^a,b,Yuanchuan Ren^a,b,Ping Ning^a,b*,Junyan Li^a,b, Yan Hu^a,b,Fenghui Wu^a,b, Yuyi Yang^a,b, Can Yang^a,b, Liankai Sun^a,b, Ziying Li^a,b ,Chenpeng Wang^a,b

^a faculty of environmental science and engineering, Kunming University of Science and Technology, Kunming,Yunnan,650500, People’s Republic of China

^b National Regional Engineering Research Center-NCW, Kunming,Yunnan, 650500, People’s Republic of China

ABSTRACT

With the increasingly stringent requirements for sewage treatment in the construction of ecological civilization, the selective removal of anions in sewage has become a hot environmental issue that has received widespread attention in recent years. In view of the current deficiency of nanomaterials in removing anions, we have developed nanowires that can selectively remove impurity anions (F-, Cl-, etc.) in water. When using nanowires to treat sewage, they have found that they have excellent anion selective removal potential. In order to explain the mechanism of this process and provide a basis for the optimization of the process, this study intends to simulate the chemical treatment of sewage and strengthen the anion removal of materials and other control experiments to grasp the migration and transformation behavior of anions under the action of nanowires, and the key influencing factors; reveal nanowires The migration and transformation behavior of anions under the action, combined with quantum chemistry calculations, constructs a model of the migration and transformation behavior of anions under the action of nanowires; it provides a theoretical basis for the efficient use of materials in the process of anion removal from sewage and the development of new recycling technologies.

Keywords：Sewage; Anion; Selectivity; Removal; Nanowire; Preparation

Introduction

With the rapid development of China's industrialization, anionic pollution(Peng et al. 2021) in water bodies has become increasingly serious. According to data from China Report Network, my country's overall sewage discharge(Wei et al. 2021) in 2019 will be around 76 billion tons. Anions are generally considered to be the most dangerous water pollutants due to their high toxicity and carcinogenicity(Fumihiko et al. 2020). Arsenate ion is one of the typical representatives of anionic pollutants(Liu et al. 2021). It has always been considered a highly toxic substance because of its high lethality and side effects to organisms. The order of toxicity of arsenic substances is (AMA)>(MA)>(MMA) )>(DMA)(Vezza et al.). The anions in the water body, such as chloride ions(Oyekunle et al. 2021), are mainly desulfurization wastewater produced during wet flue gas desulfurization. These industrial waste waters(Liu et al. 2019) contain high levels of chloride. If they are discharged directly into the water body without treatment, they will seriously harm the water environment, disrupt the water balance(Goshime et al. 2021), and affect human health.

1.The bottleneck problem of traditional anion removal

The anion pollution in the water body is becoming more and more serious, which has caused a huge impact on the ecosystem and the survival of animals and plants(Wang et al. 2021). How to find a suitable adsorption degradation material that can remove anions simply and effectively is the main goal at present. As far as the removal of anions(Ji et al. 2021) is concerned, the conventional removal methods currently used mainly include physical and chemical methods(Vargas et al. 2020) and biological methods(Dwivedi and Dwivedi 2021). The physical and chemical methods are further divided into chemical precipitation methods, ion exchange methods, membrane separation methods, redox methods and adsorption methods.

Compared with emerging anion wastewater treatment methods such as ion exchange, adsorption, and biological adsorption, chemical precipitation(Chai et al. 2021) is still the most widely used anion treatment method due to its simplicity, ease of use, and economical advantages. However, this method also has its corresponding drawbacks: (1)Chemical precipitation method(Ati et al. 2021) is more suitable for treating wastewater with high anion concentration, and for low-concentration anion wastewater, its treatment effect is poor; (2)During the treatment process, a large amount of polymerization will be produced. Sludge is easy to block the reverse osmosis membrane; (3)The chemical precipitation method cannot selectively remove anions and does not have an advantage for its subsequent recycling.

As an important method for the treatment of anion wastewater, the ion exchange method(Zgür et al. 2021) has the advantages of low price, simple equipment, easy operation, no secondary pollution, high efficiency and energy saving, etc. It has been widely used, but it also has disadvantages, such as expensive ion exchange resins. Its treatment effect is easily affected by other factors such as wastewater quality (anion ion concentration, water temperature, pH) and contact time.

Compared with other anionic wastewater treatment technologies, membrane separation technology(Talebi et al. 2021) has a series of advantages such as high efficiency, simple process, low investment, compact membrane modules, simple operation, and convenient maintenance. Therefore, membrane separation technology has shown broad application prospects. At present, the following aspects are worth noting in the research of membrane materials: (1) The research of new membrane materials requires the development of polymer membrane materials(Chen et al. 2021a) with good performance. (2) Ionic liquid(Friess et al. 2021) is a new type of green solvent, and its biggest feature is designability. Although there have been some reports on ionic liquid-related membrane research, further in-depth research is needed. (3) There is an urgent need to study the relationship between microstructure and membrane separation performance, so as to achieve the design and development of membrane materials based on the molecular level(Li et al. 2021a).

In general, the oxidation-reduction method(2021a) for sewage treatment does not need to add a lot of chemicals, the removal efficiency is high, and the post-treatment is simple, the management is convenient, the area is small, and the amount of sludge is small, so it is called the clean treatment method(Yu et al. 2021). In addition, the oxidation-reduction method(Shiga et al. 2021) can directly recover pure metals from anion sewage. Including anions and precious metals in industrial wastewater, about 30 kinds of metal ions(Kostelnik et al. 2021) can also be electrodeposited. The redox method(Zhang et al. 2019) has broad application prospects and has the potential to become an anion treatment method in the new energy era.

Efficient treatment of anion pollution in water bodies is a hot and urgent task of environmental protection(Claudia 2021) today. Chemical precipitation method(Sun et al. 2021), electrochemical method(Petersen et al. 2021), ion exchange method(Jankowska et al. 2021) and adsorption method(Rashid et al. 2021) have their own advantages and disadvantages. The adsorption method has attracted wide attention due to its advantages(Katou et al. 2001) such as simple operation, high processing efficiency, and wide application range. Adsorption material is an important factor that affects the treatment of anion wastewater by adsorption method(Chettri et al. 2021). Currently, the adsorption materials actually used generally have the problems of high cost(Liu et al. 2018), secondary pollution(Zhang et al. 2021b) or poor selectivity(Qian et al. 2014). Therefore, the development of new selective adsorption materials(Naim et al. 2021) that are inexpensive, efficient and environmentally friendly is an important direction for future adsorption research.

The removal of anions by microorganisms(Cai et al. 2022) has broad application prospects, and it has opened up a new way for us to solve the pollution of anions to the environment(Markus et al. 2021). However, it is worth noting that the current research in this area is mainly limited to laboratories and has not been widely used in industrial production and environmental protection(Zhang et al. 2021a). The main reason is that the ability of microorganisms(Cruz et al. 2021) to remove anions is not large enough. In addition, in the removal process of the time to reach equilibrium is still relatively long(Li et al. 2021b).

At present, the methods used at home and abroad to remove chloride ions(Oyekunle et al. 2021) in industrial wastewater mainly include precipitation, ion exchange, membrane separation technology, electrosorption, electrolysis, electrodialysis and reverse osmosis, but these methods are suitable for high-concentration chlorinated wastewater(Ranjan and Policy 2021). There are common disadvantages such as low removal efficiency, high cost, high energy consumption, complicated operation methods, and difficulty in meeting environmental protection requirements for the effluent. The chemical precipitation method has high industrial cost due to the addition of precipitation reagents(Nowicki et al. 2021) and is not widely used. The membrane separation method(Yang et al. 2021b) is currently used in many industrial applications for the treatment of salty wastewater, but it is prone to membrane clogging and pollution and high operating costs(Weng 2021); electrochemical technologies(Thangamani et al. 2021) such as electricity Dialysis, electrodeposition, etc., with high processing efficiency, not easy to bring in new impurities, but high energy consumption; adsorption and removal of chlorine requires a long reaction time, susceptible to temperature, competing ions, chloride ion concentration, etc., and the choice of adsorbent Sex and recycling are more difficult. Therefore, it is of great significance to find a method that is inexpensive, has no secondary pollution, and efficiently removes Cl- in acidic smelting wastewater(Guo et al. 2021).

2.Traditional nanowires have defects in removing anion selectivity

Research on the removal of anions by nanowires(Zeng et al. 2021) has been seen in major journals, among which the use of nanowires as adsorbents for the removal of anions (As) has been reported(Bui et al. 2021). For example, magnetic graphene oxide(Rebekah et al. 2021), zero-valent iron(Gong et al. 2021), magnetic nano-iron oxide(Mirzaei et al. 2021), nano-hydroxyapatite(Karimipour-Fard et al. 2021), nano-titanium oxide(Bai et al. 2021), Nano-cerium oxide(Goujon et al. 2021), nano-spherical zirconia(Yang et al. 2020), nano-copper oxide(Qian et al. 2021), nano-manganese compounds(Zhu et al. 2021) studied the removal of As in water by Fe3O4 nanoflake and confirmed that it has a good removal effect on As (Ⅴ) in aqueous solution, and the removal rate can reach 90%.Hott et al.(Hott et al. 2016)studied the adsorption of δ-FeOOH on As(Ⅲ) in water and found that the adsorption capacity was 40.0mg·g-1. Wu Shaolin et al. (2013)have shown that the adsorption capacity of magnetic nano Fe3O4·ZrO(OH)₂ to the total As in the solution can reach 133mg·g-1. Wang Can et al. (Can et al. 2014)found that the maximum adsorption of As(Ⅲ) on graphene-loaded zero-valent nano-iron was 35.8 mg·g-1. Zhou Shuang et al. (Onnby et al. 2014)found that nano-scale manganese dioxide materials can reduce the accumulation of As in rice, but cannot affect the spatial distribution of As in various organs of rice at various stages, that is, the content of As in rice is root>stem>leaf. . Cantu et al. (Cantu et al. 2016)studied the adsorption effect of nano-Fe7S8 on As(Ⅲ) under different pH conditions. The adsorption effect was the best at pH=4, and the adsorption amount could reach 14.3 mg·g-1. Liu Chuang et al. (Liu et al. 2015)found that graphene oxide has good adsorption performance, and as the pH increases, its adsorption performance for As(Ⅴ) decreases. Lin Lina et al. (2017)found that the removal rate of As (Ⅲ) by biochar-iron and manganese oxide at a concentration of 0.0160 g·mL-1 can reach 82.6%. The hydroxyl functional group will undergo ligand exchange and complexation reaction with As(Ⅲ), so as to achieve a better adsorption effect.

There are few reports on the research of nanowires in the removal of anions. Gilanizadeh et al. (Gilanizadeh and Zeynizadeh 2019)studied the structural characterization of nanohydrotalcite and its ability to remove chloride ions. The study showed that the nanometerization of hydrotalcite increased the specific surface area and pore volume of the material. Shows strong removal performance. Benali et al. (Benali et al. 2021)studied the preparation of CeO2@SiO2 microsphere adsorbent and the efficient adsorption of fluoride ions, which showed a good removal effect.

In the above research on the removal of anions and anions by nanowires, the removal effects of materials on pollutants are varied, and the effects are uneven(Dwivedi et al. 2021). Although they have adsorption effects, they do not show good selectivity.

3.Nanowires are an effective way to selectively remove anions

Nanostructures are an important means to improve the properties of materials(Kotha et al. 2021). Among them, nanowires have many advantages: easy to single-crystallize(Chen et al. 2021b), which can reduce the hole-electron recombination rate; large specific surface area, increase the boundary effect, and reduce the conductivity(Wu et al. 2021); it is conducive to the miniaturization and integration of the device(Kang et al. 2021). The preparation of nanowires(Yang et al. 2021a) can be generally divided into physical methods, chemical methods and comprehensive methods, among which chemical methods are divided into chemical vapor deposition (CVD)(Martella et al. 2021) and hydrothermal methods(Haq et al. 2021), Template method(Chauhan 2021) and so on. The hydrothermal method has the advantages of simple preparation conditions, wide range of applications, controllability and modulability, and is very popular. Hydrothermal method(Tan et al. 2021) (also known as high temperature hydrolysis method) refers to the preparation of nanowires and nanometers by placing a certain form of precursor in an aqueous autoclave solution, reacting under high temperature and high pressure conditions, and then after separation, washing, drying and other post-treatments. Powder method(Arkhangel'Skii et al. 2021, Simonenko et al. 2021, Wiranata et al. 2021). Its biggest advantage is that nanowires can be directly obtained without high-temperature sintering, and materials with low melting point, high vapor pressure and high temperature decomposition that are difficult to prepare by solid-phase reaction can be prepared. Compared with the gas phase method and the solid phase method, the powder obtained by the hydrothermal method has high purity, good dispersibility, uniformity, controllable shape, and is conducive to environmental purification(Cheng et al. 2021, Mamonov et al. 2021, Silva et al. 2021). However, the process conditions in the hydrothermal method will significantly affect the structure and properties of the nanowires(2021b, Min et al. 2021, Oleg et al. 2021, Serikov et al. 2021, Stopikowska et al. 2021).

4.Conclusions and prospects

The hydrothermal method has shown good diversity in the synthesis of nanowires that selectively remove impurity anions in sewage, and has been increasingly used. However, the current hydrothermal method is not suitable for preparing some compounds that react with water and are prone to hydrolysis and decomposition. Solvothermal method is a preparation method of materials developed on the basis of hydrothermal method. Solvothermal method is to replace the water in the hydrothermal method with an organic solvent, using a principle similar to the hydrothermal method to prepare new materials. There are many kinds of organic solvents with different properties, which can provide more space for the synthesis of materials. At the same time, by crossing and combining the hydrothermal method with other technologies, the hydrothermal technology has been further improved and improved, and the effect of the hydrothermal method has been expanded. The integration of synthesis technology will also be a major development trend of hydrothermal preparation of nanowires that select and remove impurity anions in sewage.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

Financial support for this project was provided by The National Key Research and Development Plan-Ecological Link Technology for Clean processing of Typical by-products of Unconventional Wet/thermal Production (2018YFC1900203) and The National Key Research and Development Plan- The environmental functional materials of long-acting solidification/stabilizer for heavy metal tailings pollution, technologies and equipment etc (2018YFC1801702), which is greatly acknowledged.

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