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Janus Particles Applied in Environmental Detection

Danqing Zou , Cong Wang , Fei Xiao , Yuchen Wei , Lin Geng , Lei Wang

Progress in Chemistry ›› 2021, Vol. 33 ›› Issue (11) : 2056 -2068.

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Progress in Chemistry ›› 2021, Vol. 33 ›› Issue (11) : 2056-2068 DOI: 10.7536/PC200919
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Janus Particles Applied in Environmental Detection
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Abstract

Janus particles, also called Yin-Yang structured particles or bifacial asymmetric particles, refer to asymmetric particles with two or more different chemical compositions or properties. During the past decade, Janus particles have gradually become a new type of functional materials in the fields of biomedicine, catalysis, materials and anti-fouling, due to their unique structure and function. In the field of environmental detection, Janus materials also provide new research directions for improving detection sensitivity, selectivity and stability, on account of their special optical, magnetic and electrical properties. However, there is no updated review in environmental detection field yet. To summarize and provide the guidance for the future development, this article mainly discusses the properties, advantages and applications of Janus materials in the field of environmental detection. Finally, based on our group’s research experience and the problems in this field, this article puts forward an outlook on the development and future development direction of this field, in order to provide guidance for the future development of this field.

Contents

1 Introduction

2 Application of static Janus particles in the field of environmental detection

2.1 Detection based on optical properties of static Janus particles

2.2 Detection based on electrochemistry properties of static Janus particles

2.3 Detection based on other properties of static Janus particles

3 Application of Janus micro-nano motors in the field of environmental detection

3.1 Detection based on optical properties of Janus micro-nano motors

3.2 Detection based on electrochemistry properties of Janus micro-nano motors

3.3 Detection based on the motion performance of Janus micro-nano motors

4 Conclusions and outlook

Graphical abstract

Keywords

Janus particles / asymmetric particles / environmental protection / pollutants detection / micro/nanomotors

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Danqing Zou, Cong Wang, Fei Xiao, Yuchen Wei, Lin Geng, Lei Wang. Janus Particles Applied in Environmental Detection. Progress in Chemistry, 2021, 33(11): 2056-2068 DOI:10.7536/PC200919

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1 Introduction

In recent years, the rapid development of industrialization and the high concentration of urban population have led to the aggravation of various pollutant emissions, which has caused irreversible damage to the ecological environment. Environmental pollution problems involving the atmosphere, water, soil, food and other aspects of human life and health, production activities and social sustainable development posed a huge threat[1⇓~3]. Environmental monitoring, as the main way to assess and monitor environmental quality, is of great significance for preventing and controlling environmental pollution and maintaining the ecological environment system.
In the field of environmental monitoring, how to detect common pollutants such as chemical toxins, heavy metals and various organic and inorganic pollutants in ecosystems and food samples economically, rapidly, sensitively and selectively is a key concern in this field. At present, the conventional detection methods used in this field include spectroscopy, mass spectrometry, immunoassay, microbiological method, chromatography and capillary electrophoresis[4⇓~6][7,8][9][10][11,12][13]. Although the above methods have high detection sensitivity, selectivity and reliability, they require expensive equipment and professional technicians to operate, which can not meet the requirements of real-time and on-site detection, so they have great limitations in the field of environmental detection[14]. Nanoparticle-based detection methods have the potential of on-site real-time detection due to their convenient preparation and easy operation. Many reports have proved that nanoparticles with different structures, such as core-shell structure, crescent structure and spherical structure, can be used in the field of detection and sensing[14,15][16][17][15]. The nano material with the structure solves the problem that the traditional analysis method can not realize real-time and on-site detection to a certain extent,However, in the sensing process of nanoparticles with a single kind of material, there are some problems, such as mutual interference between the detection material and the sensing material, single sensing mechanism, single detection substance and inability to achieve multi-functional detection, which lead to small detection range, low reliability and poor particle stability[18].
Compared with single-component isotropic particles, Janus particles have the following unique advantages in the field of environmental detection due to their asymmetric structure and special properties: First, Janus particles have adjustable surface properties.Can be used as a carrier unit to be attached with a plurality of functional materials, and further can simultaneously realize the functions of targeted detection, sensing and subsequent degradation of pollutants on a single particle by selecting specific particle components or modifying materials; Secondly, in the process of detection and sensing, Janus particles can achieve multi-target pollutant detection, multi-mode sensing or pollutant synergistic degradation based on the synergistic effect of modified functional materials, and further improve the performance of particles. Thirdly, the asymmetric structure of the particles enables the components to achieve regional isolation, thus reducing the mutual interference between materials and ensuring the stability of the performance of each region of Janus particles to the greatest extent. At present, these particles have been widely used in many fields, such as biological imaging probes, biological detection sensors, catalysts and drug carriers[19,20][19,21][19][19,22,23]. In order to improve the structure and function of Janus particles, the preparation method of Janus particles has become a hot topic for scientists to explore and study[24,25]. At present, the mature preparation methods include self-assembly method, semi-shielded method, phase separation method, microfluidics method, Pickering emulsion method and seed polymerization method. There are many excellent reviews on the preparation methods of Janus particles.In this paper, we will not discuss the preparation methods, but mainly focus on the application of Janus particles in the field of environmental detection in the past decade, including the detection of optical and electrochemical properties based on static and dynamic Janus particles[26][27][19,20,28⇓⇓⇓⇓⇓ ~34]. Finally, based on the research experience of the research group in this field and the problems faced in the work, this paper summarizes the current progress in this field, and puts forward the prospect of future research directions, in order to provide help and guidance for the development of this field.

2 Application of Static Janus Particles in Environmental Monitoring

At present, in the field of environmental detection, Janus particles can detect and sense various harmful pollutants (such as melamine, tetracycline, formaldehyde, etc.) in the environmental matrix, and the multifunctional characteristics of the particles enable them to combine the functions of pollutant degradation and wastewater recycling[35,36][37]. It is noteworthy that as a special type of Janus particles, Janus motor particles not only have the advantages of multi-functional sensing, but also can be combined with active motion function to facilitate the realization of rapid detection, mobile tracking, pick-up transmission and subsequent removal of target substances, which is conducive to improving the sensing performance of particles in this field. This section focuses on the application of static Janus particles in the field of environmental detection.

2.1 Detection of Optical Properties of Nanomaterials Based on Static Janus

Under the optical detection mechanism, the current research reports on static Janus particles are mainly based on the fluorescence properties, surface-enhanced Raman scattering (SERS) properties or colorimetric properties of the particles to achieve sensing functions. Among them, there are relatively many reports on the detection and sensing function based on the fluorescence properties of Janus particles. The particle mainly adopts a hemispherical structure, and ensures that the target detection material and the sensing material do not interfere with each other by distributing the target detection material and the sensing material in different areas, thereby realizing good detection and sensing functions. Current studies generally use fluorescent materials (such as polydiacetylene (PDA), fluorescein, etc.) To functionalize the particles, and use the fluorescence intensity as a signal to achieve the sensing function.
PDA has a wide range of applications in the sensing field due to its unique colorimetric fluorescence dual-detection capability and convenient molecular self-assembly preparation method[38⇓~40]. Although the PDA sensing system in the form of aqueous suspension has high practicability in aqueous solution environment, the aggregation characteristics of PDA lead to the low sensitivity of the sensing system, which limits its further development in the sensing field. In order to overcome the above problems, the researchers combined Janus particles, alginate particles with porous properties and PDA to improve the sensing performance. Kim et al. First introduced the concept of Janus particles into the field of environmental detection, and realized the function of detecting and sensing melamine[41]. They first demonstrated the detection and sensing function of alginate particle-coated PDA liposomes for melamine under the colorimetric detection mechanism, and then prepared Janus particles with two hemispherical compartments.Different PDA liposomes in the two compartments can selectively interact with avidin-fluorescein isothiocyanate and melamine respectively, thus realizing the sensing function under the fluorescence and colorimetric detection mechanism at the same time. The particle preparation process and sensing image are shown in Figure 1A. The interaction of Janus particles with melamine and avidin produced red and green fluorescence, which proved that the liposomes in the two hemispheres could achieve the targeted detection and sensing functions of the target substance respectively, and the two hemispheres would not interfere with each other. The particles can finally realize the function of detecting and sensing the melamine with the concentration of 50 ppb in the aqueous solution. Based on the same strategy, they prepared a three-compartment Janus structure alginate particle and verified its sensing performance. In this report, a Janus sensor particle model with alginate particles as the basic structure is constructed, which provides a design method of high-sensitivity sensor particles that can be applied to water environment substrates. Based on the same idea and in order to further realize the detection and removal of pollutants, Kim et al introduced magnetic nanoparticles into Janus alginate particles to realize the specific detection, sensing and removal of lead[42]. They are also based on two-compartment alginate particles, which are filled with sensing liposomes and magnetic nanoparticles respectively. The sensing liposomes are composed of PDA for generating sensing signals and liposomes for lead-specific detection. After the sensing substance interacts with lead, the color changes from blue to red, and the red fluorescence intensity increases with the increase of the concentration, so that the detection and sensing function of lead can be realized based on the change of the fluorescence intensity. The particle image and sensing result under an optical microscope are shown in fig. 1B. It can be seen from the figure that the addition of magnetic nanoparticles enables the particles to be controlled by the magnetic field, which is helpful for the particles to quickly detect a large number of target substances, thus achieving the purpose of improving the sensitivity and shortening the detection time, and also making the subsequent removal of particles more convenient. On the basis of realizing the specific recognition function of target substances, this report adds the subsequent removal function of particles, which provides the possibility for the development of multi-target and multi-functional sensing particles.
In the field of environmental detection, whether the enrichment of low-dose target substances and high capture efficiency can be achieved is an important indicator to evaluate the sensing performance of particle detection. Based on this, Chang et al. combined the excellent biocompatibility of magnetic nanoparticles and the optical properties of fluorescein dye, and successfully prepared fluorescent magnetic nanorod particles with Janus structure, which can enrich and detect food-borne bacteria in milk[43]. The particles are based on mesoporous silicon dioxide and magnetic ferroferric oxide particles, wherein the silicon dioxide particles are doped with a fluorescein dye modified by a bacterial antibody to realize a specific detection sensing function of a target substance, and the ferroferric oxide can realize bacterial enrichment and subsequent separation functions under the action of a magnetic field. In this report, in addition to the use of fluorescence detection method to achieve the specific capture and sensing function of bacteria, after the completion of the magnetic separation step, the complex of bacteria and Janus particles was detected by matrix-assisted laser desorption ionization time-of-flight mass spectrometry to achieve the function of bacterial identification. Taking E. coli and Staphylococcus aureus in milk as target pollutants, they verified the ability of particle detection and sensing bacteria, and further illustrated the advantages of Janus particles in the field of environmental detection. In order to construct a general model of Janus sensing particles under the fluorescence detection mechanism, Villalonga et al. Proposed a general paradigm for preparing optical detection probes based on enzyme reaction: an enzyme for realizing specific detection function and a fluorescent material for realizing sensing function are respectively connected to the surface of Janus particles.The reaction product of the enzyme and the substance to be detected is utilized to realize the shedding and release of the fluorescent material, thereby completing the information transmission function between the detection and sensing areas[44]. In order to prove the feasibility of the template, they designed a Janus particle based on gold and mesoporous silica materials, which can realize the function of urea detection (Fig. 1C). In the design of Janus particles, the surface of silica is functionalized by amino groups, and oligonucleotides end-labeled with fluorescent dyes are connected to it through electrostatic interaction to achieve sensing function. The functional urease for urea detection can be realized by the surface modification of gold particles, and the urea is converted into ammonia and carbon dioxide after being recognized by the urease, so that the amino groups on the surface of silicon dioxide fall off and fluorescent materials are released, and then the sensing function is realized. The particle was applied to the detection of milk and human plasma, and the results proved that the particle has the potential to be applied to the field of food detection and clinical medical detection. In this report, a general design process of Janus sensing particles is proposed by combining the concepts of fluorescence detection and enzyme reaction sensing. In the study of pollutant removal and degradation, Jia et al. proposed a new visible-light-driven photocatalytic degradation method in addition to the introduction of external magnetic field, which can realize the degradation of tetracycline (TCs), a common pollutant in wastewater and ecosystem, and the degradation efficiency of TCs can reach 93.33% within 40 min[42][45]. Citrate (Cit) and Eu were used as functional materials to modify the amino clay (AC) -gold Janus structure composite. Wherein the Eu3+ has a specific detection function for the tetracycline, and the beta-diketone functional group contained in the tetracycline enables energy to be transferred to the Eu3+ so as to realize the fluorescence detection function. Cit replaces the water molecule to coordinate with the Eu3+ to avoid the fluorescence quenching phenomenon. The as-prepared AC-Au nanomaterials were used as visible-light-driven photocatalysts and showed good TCs degradation efficiency. It is noteworthy that, as shown in Figure 1D, in order to simplify the sensing process, they developed a paper-based detection probe that uses the program to digitize the color, which can quickly detect the concentration of tetracycline. Furthermore, Chen et al. also applied TiO2-SiO2Janus particles to the degradation of methyl blue in water environment based on photocatalytic degradation reaction, which verified the ability of photocatalytic materials to degrade pollutants in water environment and had great application prospects in the field of decontamination[36].
In the field of environmental detection, compared with the research based on fluorescence detection mechanism, there are relatively few reports on SERS and colorimetric detection mechanism based on optical detection mechanism. At present, only Liu et al. And Zhao et al. Have applied Janus materials in this field based on these two mechanisms respectively, and have studied the detection of complex samples and the improvement of the accuracy of sensing results under a single detection mechanism respectively[46,47][48].
In the research of this field, the environmental matrix to be detected is generally complex, so how to achieve fast, sensitive, highly reliable and accurate sensing in complex samples is one of the concerns in this field. Based on this, Liu et al. Developed a Janus gold nanoparticle that can detect contaminants in complex samples based on the colorimetric detection mechanism[46]. Under the mechanism of colorimetric detection, the use of gold nanoparticles as sensing particles has attracted much attention in the sensing field, but the non-specific aggregation of gold nanoparticles and their high sensitivity to the environment (salt concentration, pH and temperature) limit their further application in the sensing field[47]. Polyethylene glycol (PEG) and 4-aminobenzenethiol (4-ABTs) were modified on the surface of gold nanoparticles respectively. PEG probes with good water solubility and biocompatibility were used to maintain the stability of particles in the detection environment and restrict the aggregation characteristics of gold nanoparticles. The existence of 4-ABTs realized the specific detection function of nitrite ions. In the sensing process, nitrite ion reacts with 4-ABTs to form diazonium salt, and then reacts with other 4-ABTs to form dimercaptoazobenzene, which changes the color of the solution from red to purple, and the spectrum in the visible region changes accordingly. With the dissolved sausage as the sensing environment, the particle successfully realized the detection of nitrite ions, proving its ability to achieve sensing function in complex samples. The color change of the purple solution after detection is almost negligible in a few days, indicating that the sensing particles have the potential to be applied in remote areas. When the environmental matrix is complex and the detection mechanism is single, how to evaluate the reliability and accuracy of the detection results is also a key concern in the field of environmental testing. In the field of SERS sensing, the problem of weak Raman signal generated by a single nanoparticle is also one of the urgent problems to be solved in this field. In order to solve the above problems, Zhao et al. developed a bimetallic Janus structure Ag-Au nanoparticle, which uses MXenes nanosheets that can generate stable Raman signals as an internal calibration material to enhance the sensing signal and improve the reliability of the detection results[48]. They used gold and silver as the basic components of the particles to synthesize Janus particles with fixed Raman signals under the guidance of 2-mercaptobenzimidazole-5-carboxylic acid (MBIA), which can be used to detect the mycotoxin ochratoxin A (OTA). The detection mechanism of the OTA sensor is as follows: the Ag-Au nanoparticles and MBIA jointly realize the function of amplifying the SERS signal, and the OTA aptamer modified on the surface of the Au particles realizes the targeting function of the OTA. The products formed after the OTA and the Janus particles are compounded are separated from the MXenes nanosheets, so that the Raman signals corresponding to the nanoparticles are attenuated, and then the detection and sensing functions are realized. The schematic diagram of the particle preparation process and the sensing result are shown in Figure 2. During the sensing process, the signal corresponding to the MXenes nanosheet remains constant, so this signal can be used as an internal standard to calibrate the detection result and realize the signal correction function. The internal calibration signal improves the linearity of the test results, which proves that the method has the ability to improve the accuracy and reliability of the test results.

2.2 Detection of Electrochemical Properties Based on Static Janus Nanomaterial

Under the electrochemical detection mechanism, Janus nanoparticles need to achieve energy conversion and specific detection functions respectively. As a transducing element, the particles are mainly used to enhance the conductivity and catalytic performance of the electrode surface, accelerate the transfer of electrons on the sensing interface and the conversion of target substances, and then realize the sensing function. As a detection element, the particle is mainly modified by a ligand material (avidin, aptamer, enzyme, etc.) To realize a specific detection function of a target substance.
In the research reports in this field, S Sánchez et al. First realized the sensing function by using the electrochemical properties of Janus materials, and achieved rich research results[49]. They first designed a complete electrochemical biological reaction signal system with gold-mesoporous silica Janus particles as the carrier, and successfully realized the recognition of biotin on gold surface. In the preparation process of the nanoparticles, horseradish peroxidase as an enzyme-catalyzed signal transduction element was modified on the surface of mesoporous silica, streptavidin as a target substance recognition agent, and methoxy polyethylene glycol thiol (PEG-SH) as a nanoparticle solubilizer were modified on the surface of gold, and the sensing performance was improved by the combined action of the three. During the sensing experiment, they first coated the gold electrode surface with target biotin, and exposed Janus particles to the electrode surface. The effect of biotin and nanoparticles on the gold surface was evaluated by surface plasmon resonance signal, which proved that biotin adsorbed well on the gold electrode surface. After biotin and nanoparticles were sequentially modified on the electrode surface, they were analyzed by electrochemical impedance spectroscopy and cyclic voltammetry to prove the recognition function of the particles to biotin on the gold surface. Based on this report, they also prepared a dual-enzyme biosensor based on gold-mesoporous silica Janus particles, and successfully determined the glucose content in market drinks. The sensing process and results are shown in Figure 3A[50]. They first deposited single-walled carbon nanotube (CNT) materials that can increase the surface area of the electrode on the glassy carbon electrode to achieve the purpose of improving the electrocatalytic performance, and then modified glucose oxidase and horseradish peroxidase on the surface of mesoporous silica particles and gold particles respectively to achieve glucose detection and catalytic functions. During the sensing process, the cathodic current on the electrode functionalized by CNT and Janus particles increased significantly, indicating that the composite material of CNT and Janus particles had strong electrocatalytic conversion with hydrogen peroxide and glucose, forming a stable electrocatalytic sensing interface. The system was then applied to the glucose detection of commercial beverages, and the sensing results proved its ability to detect glucose in food samples.Subsequently, different target substances can be detected and sensed by changing the way of modifying enzymes, which provides a general way for the development of multi-functional Janus sensing particles under the mechanism of enzymatic reaction.
In terms of realizing the specific recognition of the target substance, in addition to the use of enzymes, He et al. developed an OTA sensor under the electrochemical detection mechanism based on the aptamer modification method. The particle preparation process and sensing results are shown in Fig. 3B[51]. They used polystyrene particles as the basic structure, one side was coated with gold thin layer by vacuum evaporation, and then OTA aptamer was used to modify the gold coating to achieve specific detection function. The other hemisphere is modified by amino and combined on the surface of the glassy carbon electrode modified by carboxylation, and the amino and the carboxyl can form an amide bond after dehydration and condensation to ensure that the nanoparticles are fixed on the surface of the electrode. They detected OTA concentration by differential pulse voltammetry, and the results showed that the system could achieve linear detection of OTA concentration in the 1×10-14~1×10-8mol·L-1 range with a correlation coefficient of 0.9931. They tested the selectivity, stability and reproducibility of the sensor and finally detected OTA in red wine samples. The experimental results showed that the sensor particles had good selectivity, stability and reproducibility, and could accurately determine the OTA concentration in red wine samples. It is expected to achieve OTA detection function in other foods.

2.3 Detection of Other Properties Based on Static Janus Nanomaterial

In the field of environmental detection, it is also a problem for researchers to develop new signal conversion mechanisms or propose new sensing signal concepts to achieve high-performance sensing. At present, only Zeng et al. Have reported the research on the detection of volatile organic compounds formaldehyde by using nanoparticle resistance as a sensing signal[52]. In the process of particle preparation, they first coated gold nanorods with zinc oxide, then partially modified zeolite imidazolate framework (ZIF-8) on their surface, and finally prepared Au @ ZnO @ ZIF-8 Janus particles with the characteristics of metal oxide and metal-organic framework (MOF). The particle combines the advantages of high conductivity of zinc oxide, superior gas adsorption ability of ZIF-8 and plasmon resonance effect of gold nanorods, and successfully detects formaldehyde in the concentration range of 0. 25 ~ 100 ppm. They believe that the sensing principle is that the plasmon resonance effect of gold nanorods under visible light irradiation leads to the release of electrons in the formaldehyde reaction process, which reduces the particle resistance. During the detection process, formaldehyde was partially oxidized to formic acid, which proved that the particles also had the potential to degrade volatile organic compounds. In this report, a new sensing method using particle resistance as sensing signal is developed, which provides an idea for the proposal of other sensing signals.
At present, in the field of environmental detection, the research on static Janus particles is mainly based on optical and electrochemical sensing mechanisms. Because the modifiable area of the particles is larger and the preparation method is more mature, various material modifications can be realized on the surface of the particles, thereby realizing multifunctional, multi-target substance and multi-mode sensing, and having higher sensing result accuracy and more stable particle performance. However, due to the static characteristics of particles, the detection and sensing under the two mechanisms are mainly based on static diffusion transport, and the detection time is relatively long, which limits its application in the field of environmental detection.

3 Application of Janus Micro/Nano Motor in Environmental Monitoring

In the research reports in the field of environmental detection, besides the static Janus particles, Janus motor particles, as a special kind of dynamic Janus particles, also have great application potential in this field because they can quickly detect and pick up and track the transfer of target substances. Motor particles can be powered by a variety of mechanisms, such as gas or concentration gradient produced by the catalysis of metal platinum, lipase and other materials.Magnesium, aluminum and other metals are used as fuels to participate in the oxidation-reduction reaction to produce gas to promote the movement of particles, in addition, the magnetic field or the inherent substances of the environmental matrix itself are used as natural fuels to achieve the movement of particles[53⇓~55][56⇓~58][59][60,61]. In addition to a single motion mechanism, motor particles can also achieve motion function by mixing multiple motion mechanisms[62,63]. Similar to the static Janus particles, the research of motor particles in this field is still mainly based on the optical or electrochemical properties of the particles. In addition, the unique motion characteristics of motor particles make it possible to propose new sensing concepts (such as speed, distance, etc.).

3.1 Detection of Optical Properties Based on Janus Micro-nano Motor

At present, under the optical detection mechanism, the research reports in the field are all based on the fluorescence quenching phenomenon of Janus motor particles to realize the sensing function, and the power source of the motor particles is bubbles generated by redox reaction or an external magnetic field.
Because the target substances studied in this field are harmful to the environment and human body, whether rapid detection can be achieved is one of the important indicators to evaluate the sensing performance of particles. In order to shorten the sensing time, Wang et al. combined the concept of motor particles with environmental detection, and prepared a Janus motor particle capable of detecting the organophosphorus nerve agent sarin and the soman analogue, diethyl chlorophosphate (DCP). The particle preparation process and energy dispersive X-ray spectroscopy image are shown in Fig. 4A[64]. Silica particles were used as the basic structure, coated with fluorophore fluorescamine (FLA) on the surface, and then platinum was asymmetrically deposited on the surface of the particles, and finally a platinum-fluorescamine hemispherical coated silica Janus motor particle was prepared. The sensing experiments were carried out in aqueous solution simulating natural environment, and the results showed that the motor particles could achieve instantaneous fluorescence quenching and the reaction rate was much faster than that of static particles, which was attributed to the interaction between phosphate and fluorescamine. In order to prove the practical application value of the particle, they also carried out sensing experiments in seawater, pond water and lake water, and obtained the same fluorescence intensity curve as the initial experimental results, proving that the particle is suitable for a variety of natural environments. As shown in Fig. 4A, the experimental results show that the particle can complete the detection of DCP in the concentration range of 10-6~10-1mol·L-1 within 3 min. In this report, the realization of sensing function based on fluorescence quenching phenomenon is proposed.
The basic model of Janus motor particles can further increase the function of particles by modifying materials. Jurado-S Sánchez et al. Modified Janus motor particles with specific recognition receptors to improve the specific recognition performance of sensor particles for target substances[65]. They developed a dual-powered hybrid mechanism Janus motor microparticle based on graphene quantum dots (GQD), which can be used for the detection and sensing of endotoxin lipopolysaccharide (LPS). The particle takes GQD as the basic structure. After the surface is coated with highly fluorescent phenylboronic acid (PABA), a large number of magnetic ferroferric oxide particles and platinum particles with catalytic effect are introduced on one side, which are used to realize magnetic field pushing and bubble pushing respectively. The motor particle is shown in Figure 4B under the optical microscope. In the process of detection and sensing, the specific recognition receptor PABA of LPS realizes the detection function, and the fluorescence quenching phenomenon occurs after the interaction between GQD and LPS, thereby realizing the sensing function. Fig. 4B illustrates the effect of the motion mechanism on the sensing performance. The sensing results show that the minimum detectable amount of LPS in Janus motor particles with dual power sources is lower than that in motor particles with single power source driven by magnetic field or bubble, which proves that Janus motor particles have the potential application value of reducing the detection limit. Then they reported the relationship between the fluorescence intensity of particles and the concentration of LPS, which made the quantitative detection of LPS possible. The sensing results and the fluorescence decay under various movement mechanisms are shown in Figure 4C[66]. In order to verify the ability of particles to detect LPS in food, the report uses milk, mayonnaise, egg yolk and egg white samples with a toxin concentration of 1 ng/mL as the matrix for experiments. After a period of time, obvious fluorescence quenching occurred in the four samples, and the minimum detection concentration of the particles was 0. 07 ng/mL, which was far below the level of 275 μg/mL that LPS was harmful to human body, indicating that the motor particles had great application potential in the field of food detection with complex viscosity. Also based on the fluorescence quenching phenomenon, Gao et al. successfully detected the water pollutant 2,4,6-trinitrotoluene (TNT) by using a catalytic Janus micromotor particle with capsule structure. The particle preparation process and sensing results are shown in Fig. 4D[67]. In the detection process, the presence of TNT leads to the luminescence quenching of the transformed nanoparticles, thereby realizing the detection and sensing function, and the lowest detection concentration is calculated to be 2.4 ng/mL. The motor particles based on the optical detection mechanism realize the environmental detection function through the fluorescence quenching phenomenon. On the basis of using fluorescence switch to detect the existence of target substances, the researchers established the relationship between fluorescence intensity and fluorescence quenching time and the concentration of target substances, and successfully realized the quantitative detection of target substance concentration.

3.2 Detection of Electrochemical Properties Based on Janus Micro-nano Motor

Under the electrochemical detection mechanism, the motion performance of Janus motor particles makes it have the function of "autonomous stirring", which can be used to improve the problem that the sensing effect of static solution is limited by diffusion transport reaction. At present, under this mechanism, motor particles mainly use the gas produced by metal catalytic reaction as the power source to achieve self-propulsion function.
In the field of environmental detection, Jurado-S Sánchez et al. Have done a lot of research on pollutant detection and degradation based on the electrochemical performance of Janus micro-nano motor particles. They first combined the motion characteristics of motor particles with the adsorption capacity of activated carbon particles, and proposed a Janus motor particle that can remove various pollutants in the water environment matrix (Fig. 5A)[68]. The particles take platinum as a catalytic metal, the platinum is asymmetrically deposited on the surface of activated carbon particles, and bubbles are generated under the action of hydrogen peroxide fuel, so that the self-propulsion function is realized. In addition, the rough platinum layer area significantly increases the surface area of the particles and further improves the catalytic performance. In order to investigate the actual decontamination ability of the particle, the ability to remove various organic (nerve agents, explosives, fuels) and inorganic (heavy metals) pollutants was verified by experiments. The experimental results show that the electrochemical response of pollutants in the matrix is significantly reduced after the treatment of the particles, which verifies the excellent water purification effect of the particles. Then they successfully detected the persistent pollutant diphenyl phthalate (DPP) in food and biological samples based on magnesium-gold Janus motor particles[69]. The particles are based on magnesium spheres and are coated with a thin layer of gold over a wide range of asymmetry on their surface. NaCl is used as the fuel and electrolyte in the detection process, and the surface of magnesium is easily oxidized after reacting with it, which leads to the generation of bubbles and hydroxyl products. The schematic diagram of the prepared particle image and sensing process is shown in Figure 5B. Hydroxyl ions increase the pH value of the solution, which leads to the degradation of the non-electroactive DPP to be detected into electroactive phenol, thus realizing the function of pollutant degradation. They combined motor particles with screen-printed electrodes and applied them to DPP detection and sensing experiments in water, milk and whiskey. The experimental results show that the DPP concentration in water and milk is in the range of 0.12~1 mmol·L-1, and that in whisky is in the range of 0.5~2 mmol·L-1, and the correlation coefficients are all higher than 0. 990, so the sensing effect is good. However, the particle has the disadvantage of short lifetime, and it will be dissolved after 5 min of movement in the sample, which limits the possibility of further improving its sensing sensitivity and degradation efficiency. In the field of environmental detection, how to prolong the life of Janus motor particles and ensure the long-term stability of particle performance is also one of the urgent problems to be solved by researchers.
In order to improve the problems of the traditional electrochemical detection mechanism (beaker-type) electrochemical cell, such as large equipment and difficult to use, the researchers developed a strip cell based on screen printing technology. Based on this idea, Palleschi et al. Combined Janus motor particles with strip batteries, and proposed an electrochemical sensing system of strip batteries assisted by motor particles[70]. The strip-shaped battery is divided into two main areas, one side is provided with motor particles, and the other side is provided with a working electrode. The motor particles are driven by the hydrogen produced by the reaction of magnesium and water, and the action of the external magnetic field prevents the motor particles from entering the working electrode area due to movement. The reaction generated in the sensing process significantly increases the pH value of the solution, thereby leading to the rapid degradation of the organophosphorus nerve agent, and the non-toxic degradation product nitrophenol can be used for electrochemical detection to realize the sensing function in the electrode area. The results show that the current response intensity has a good linear correlation with the concentration of organophosphorus nerve agent in the range of 0~20 mmol·L-1, and the correlation coefficient can reach 0.995. The sensing platform has the advantages of simple design and convenient operation, can detect and sense various target substances by selecting different motor particles or electrode materials, and is expected to be applied to the actual sensing environment.
Under the electrochemical detection mechanism, the researchers also studied a special kind of Janus motor particles based on the electroluminescence (ECL) phenomenon to realize the sensing function. The design of this type of motor particle is mainly based on the concept of bipolar electrochemistry. Compared with conventional electrochemical reactions, bipolar electrochemistry combines the anode and cathode, that is, two redox reactions are combined on the same particle. This kind of particle is mainly driven by the gas produced by the redox reaction of one pole or the different amount of gas produced by the redox reaction of two poles, and can play a role in the sensing field after adding the electroluminescence function. Compared with Janus particles based on fluorescence detection mechanism, this type of motor particles has the advantages of good signal-to-noise ratio performance and no need for additional modification of fluorescein in the field of sensing, which is convenient for tracking moving objects[71]. Bouffier et al. Successfully prepared Janus motor particles with blue light emission performance based on graphite beads, which can play a role in the field of sensing by modifying functional materials on the surface of particles[72]. Based on this report, Bouffier et al. Successfully applied electroluminescent motor particles to the field of glucose detection and sensing[73]. As shown in fig. 6, the particle is based on a glassy carbon bead located between two electrodes, and the motion of the particle is propelled by hydrogen gas generated at the cathode end of the particle. Glucose is oxidized by glucose dehydrogenase under the condition that NAD+ is used as an auxiliary oxidation factor, NADH generated by the enzymatic reaction leads to the emission of ECL, and the emission intensity can be related to the concentration of glucose, thereby realizing the sensing function. In addition, this method can also detect the spatial distribution of glucose concentration changes, such as motor particles moving in a medium with non-uniform concentration, so ECL is only activated in the region where the substance to be detected exists. This study shows the possibility of the application of motor particles combined with ECL and bipolar electrochemistry in the field of sensing and detection, but there are still relatively few studies on the application of such particles in the field of sensing.

3.3 Detection of self-motion performance of Janus micro-nano motor

Due to the motion property of the motor particle itself, the sensing function can also be realized by establishing the relationship between the substance to be detected and the characteristic parameters of the motor particle, such as speed, distance or degradation time.
Wang et al. Are the pioneers of applying Janus nanomotor to this detection field. Based on gold-platinum Janus nanomotor particles, they established the relationship between the concentration of the substance to be detected and the speed of the motor particles, and realized the detection and sensing function of silver ions[74]. They found that in the case of hydrogen peroxide as fuel, silver ions had a significant selective acceleration effect on the motor particles compared with other metal ions (platinum ions, copper ions, etc.), and the particle velocity could be related to the concentration of silver ions. Based on the particularity of silver ions, this study can realize the sensing function of silver ions in a certain range, which lays a foundation for the research of sensing function based on the motion properties of motor particles. Similarly, Dong et al. Prepared a light-driven Janus motor particle which can realize the detection and degradation of 2,6-dichloroindole sodium (DCIP) by using the speed of the motor particle as the sensing signal[75]. As shown in fig. 7A, a Au-WO3@C Janus motor particle with good photocatalytic performance was finally prepared by coating a hemispherical gold layer after modifying tungsten trioxide on the surface of the colloidal carbon sphere as the basic structure. The hydrophilic surface, high specific surface area and nano-porous structure of WO3@C particles promote the absorption and subsequent degradation of organic pollutants, and the WO3 ensures the good photocatalytic performance of the particles. The results of sensing experiments show that the particle can be used as a sensing signal to detect and sense low concentration dyes such as DCIP. In addition, the movement of the motor particles can be controlled by the magnetic field by covering a Ni layer between the WO3 layer and the Au layer, and the dual power sources of ultraviolet light and a magnetic field provide more possibilities for the practical application of the motor particles. Similar to the idea that dual power sources can improve the motion performance of motor particles, dual degradation mechanisms can also improve the decontamination ability of particles. Based on this idea, Zhang et al. prepared a Janus motor particle with bottom modified Fe3O4@Ag nanoparticles and surface modified ZIF-8 @ ZnONPs nanoparticles based on MOF materials, which has the function of synergistic degradation of pollutants by photocatalytic mechanism and oxidation mechanism[35]. Rhodamine B was used as the target pollutant in the experiment, and the results showed that compared with the control group with single degradation mechanism and the control group with double degradation mechanisms but without particle self-propulsion, Janus micromotor particles showed good degradation performance and had great application potential in the field of decontamination. Also based on the problem of pollutant removal and degradation, Li et al. Realized the removal and recovery of precious metal ions by using the replacement reaction of magnesium in hydrogen peroxide solution[76]. The Janus particle is composed of polycaprolactone (PCL) and magnesium particles, and has three functions of sensing, removal and recovery of noble metal ions (gold, silver, platinum, etc.). The particle image and movement mechanism are shown in Figure 7B. In the sensing process, the displacement reaction of magnesium and noble metal ions can simultaneously realize two functions of motor particle propulsion and noble metal ion removal. Because that velocity of the motor particle is highly dependent on the type and concentration of the noble metal ions, the velocity of the motor particle can be used to realize the sensing function. In addition, the characteristic that PCL polymer is easy to be dissolved can be used to realize the recovery function of precious metals, and gold is taken as an example to verify the ability of particles to recover precious metals. The method for removing and recycling the target pollutants based on the displacement reaction provides a new idea for solving the problem of removing the pollutants in the field of environmental detection, and has great application potential in the field of noble metal ion sensing and recycling.
In addition to using the movement speed or movement distance of the motor particles as the sensing signal, Chattopadhyay et al. prepared a motor particle by randomly distributing palladium particles on polymer microspheres, which can show different movement patterns (random walk, translation, vertical movement, jump, etc.) at different pH values. The pH detection process is shown in Figure 7C[77]. This signal transmission mechanism, which judges the concentration of the substance to be detected by the motion pattern, is relatively novel in the field of sensing. In addition, some motor particles may use the substance to be detected as a chemical fuel, such as motor particles using hydrazine as a chemical fuel, or use the substance to be detected as a reactant to participate in a chemical reaction, such as motor particles that achieve a self-propulsion function based on various enzymatic reactions[55,78][79⇓⇓~82]. This type of particle can cause the change of particle motion property through the change of fuel concentration in the reaction process, and then establish the relationship between the particle motion property and the concentration of the substance to be detected. However, the fuel used by motor particles is relatively limited, which limits the application of such particles in the field of sensing.
In order to improve the environmental friendliness of decontamination particles, Pumera et al innovatively used pollen particles as the basic structure of motor particles, and prepared a Janus motor particle with the gas generated by platinum catalytic reaction as the power source, which showed good adsorption effect on Hg2+ in aqueous solution[83]. Compared with carbon and polymer motor particles, the outer wall of pollen particles has good mechanical stability, and the hollow inner shell structure also makes the particles have the potential to be used in the field of drug delivery. Nine kinds of motor particles were prepared based on different kinds of pollen particles, and their abilities of adsorbing Hg2+ and loading drug doxorubicin were verified, which indicated that the particles had potential applications in the fields of environmental remediation and biomedicine. Also based on the development of decontamination particles with good environmental friendliness, Makarov et al. Prepared a Janus motor particle by coating functional nanoparticles on the surface of hydrogel microspheres[84]. The particles can degrade methylene blue in aqueous solution and have good water purification ability. It is noteworthy that the preparation method used in this report has strong versatility, and multi-functional motor particles can be prepared by attaching different functional nanoparticles on the surface of microspheres. The particle has the potential of degrading various pollutants at the same time and has great application value in the field of environmental remediation.
Similar to static Janus particles, Janus motor particles are also currently used for environmental detection based on their optical and electrochemical properties. Under the optical detection mechanism, the motion performance of particles can greatly accelerate the detection time, but the current research under this mechanism is based on the phenomenon of fluorescence quenching, and the sensing mode is relatively single. Under the electrochemical detection mechanism, the "autonomous stirring" function of motor particles improves the problem that the sensing results under static particle conditions are limited by diffusion and transport reactions.At the same time, the movement characteristics of Janus particles enable it to be used in complex environmental matrices (such as viscous food samples) to achieve sensing function, but the relatively short service life of Janus particles limits its development in the field of environmental detection.

4 Conclusion and prospect

In this paper, the unique properties of Janus (yin-yang structure) micro-nano particles and their advantages and related representative applications in the field of environmental detection are discussed in detail.This paper focuses on how to use the optical and electrochemical performance advantages of static Janus particles and Janus micro-nano motor particles for detection, in order to provide guidance for the future design of Janus sensor particles with high selectivity, high sensitivity, high reliability and high stability. At present, the reports in this field have not fully developed the application potential of Janus materials. In the future, Janus sensing particle systems that can achieve multi-function (targeted positioning, detection and sensing, removal and degradation), multi-target substances (various organic and inorganic pollutants) and multi-mode (optical and electrochemical) sensing can be developed based on the mature preparation methods of static Janus particles.It can also be combined with the superior motion performance of Janus micro-nano motor particles to further develop the advantages of the particles in complex sample detection (such as sticky food samples) and pollutant degradation. However, the research and development of Janus nanomaterials for environmental detection is still in the exploratory stage, and there are still many problems to be solved. In the synthesis of Janus particles, how to precisely control the structure and properties of Janus nanoparticles in the preparation process, and then efficiently and massively prepare Janus materials with stable structure and properties is one of the urgent problems to be solved. In addition, it is necessary to focus on the development of green and environment-friendly Janus particles to avoid secondary pollution in the process of detection and sensing, and to design new particle recovery methods to solve the problem that magnetic field recovery methods are difficult to apply to the actual sensing environment. In the application of Janus particles, motor particles, as a new material, can improve the sensing performance because of their good motion properties, but they still have some shortcomings, such as complex preparation process, short service life, single sensing mode and poor specific recognition function.In the future, its application value in the field of environmental detection can be further improved by developing new preparation methods, proposing new power sources or modifying various types of materials.

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Funding

National Natural Science Foundation of China(52073071)

National Natural Science Foundation of China(51703043)

China Postdoctoral Science Foundation(2017M611367)

China Postdoctoral Science Foundation(2016M600247)

China Postdoctoral Science Foundation(2020T130144)

Natural Science Foundation of Heilongjiang(F2018014)

Postdoctoral Science Foundation of Heilongjiang(LBH-Z17056)

Postdoctoral Science Foundation of Heilongjiang(LBH-Z16066)

Laboratory of Zhejiang(2019MC0AB03)

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