RELATED APPLICATIONS

[0001] This application claims the benefit of priority to co-pending United States Provisional Application Serial No. 63/380,142, filed October 19, 2022, the contents of which is incorporated by reference.

COPYRIGHT NOTICE

[0002] This patent disclosure may contain material that is subject to copyright protection. The copyright owner has no objection to the facsimile reproduction by anyone of the patent document or the patent disclosure as it appears in the U.S. Patent and Trademark Office patent file or records, but otherwise reserves any and all copyright rights.

STATEMENT REGARDING FEDERALLY SPONSORED RESEARCH OR DEVELOPMENT

[0003] This invention was made with government support under DE-SC0000989 awarded by U.S. Department of Energy (DOE). The government has certain rights in this invention.

BACKGROUND

[0004] Triboelectric effect involves a transfer of electrical charge between two bodies that contact each other (e.g., by rubbing or sliding). The triboelectric effect occurs in daily life, but it has not been utilized to store energy and supply ionic current. The challenge remains to connect the charging process to material science (to store the energy in chemical forms) and then release the energy at the point of use (via performing chemical reactions).

[0005] Electrostatics have been used to cyclically charge polymer substrates dating back to the Van de Graaff generator ¹ and Wimshurst/Bonetti machines. The design of these devices was described by the transport of electrostatic point charges without considering the details about which chemical species carry the charge.

[0006] There is a need for systems and methods that harvest electrostatic energy, produce chemical ions, and use those species to drive reactions on-demand. The exact mechanism by which charge is stored on polymer materials will inform the design of a new class of devices and chemical applications. Such devices can be optimized to maximize the energy and storage efficiency of charge transfer onto a substrate. Applications can also be designed to form desirable chemical intermediates (i.e., ions) directly on the material that carries the charge, a region that has largely been neglected in electrostatic devices to date.

[0007] There is a need for new distributed energy sources that can operate in environments that are devoid of resources. Applications include finding solutions to 1) the food crisis, 2) water contamination (e.g., by bacteria, viruses and parasites), 3) surface contamination (e.g., clinical tools) or fomite (surface) transmission, and 4) lack of point-of-care diagnostic tools. Harvesting electrostatics is one method to form chemical ions, which act as a localized energy source to facilitate these applications mentioned.

[0008] Where power sources are limited, there is a need for energy sources that can be passively generated while other activities are being performed (e.g., commuting, plowing fields, etc.). Furthermore, it would be desirable if this source of energy could be assembled from available materials virtually anywhere in the world without requiring access to the grid or any modern infrastructure.

SUMMARY

[0009] In accordance with an exemplary aspect, a system including an electrostatic energy generator, which generates an electrostatic charge, in one of an electrical form or a chemical form, a charge carrier converter, which is electrically connected to the electrostatic energy generator to convert the electrostatic charge from the electrostatic energy generator into an electric current or an ionic current, and a chemical reaction device, which is configured to receive the electric current or the ionic current from the charge carrier converter to drive a chemical reaction in the chemical reaction device is disclosed.

[0010] In some embodiments, the electrostatic energy generator includes a triboelectric generator or a piezoelectric generator.

[0011] In some embodiments, the electrostatic energy generator includes a triboelectric generator with a first contact charging layer including a first material and a second contact charging layer including a second material, wherein the first material has a more negative triboelectric series value than the second material.

[0012] In some embodiments, the chemical reaction device is electrically connected to the charge carrier converter to receive the electric current. [0013] In some embodiments, at least one of the first material and the second material is polytetrafluoroethylene (PTFE), polydimethylsiloxane (PDMS), polyethylene terephthalate (PET), poly(methyl methacrylate) (PMMA), metals, polyester, nylon, or combinations thereof.

[0014] In some embodiments, the triboelectric generator includes an endless belt contacting and moving relative to a first roller and a second roller, wherein the first contact charging layer is disposed on the endless belt and the second contact charging layer is disposed on at least one of the first and second rollers.

[0015] In some embodiments, the system further includes a capacitor electrically connected to the charge carrier converter and the chemical reaction device to store one or more of the electric current or the ionic current.

[0016] In some embodiments, the chemical reaction device includes a receptacle, wherein the receptacle contains a sample to be treated.

[0017] In some embodiments, the system also includes a discharge device including a negatively charged electrode and a positively charge electrode, wherein the discharge device is operable to generate an electrical discharge in the sample to be treated.

[0018] In some embodiments, the electrical discharge includes one or more of a plasma and a spark discharge.

[0019] In some embodiments, the electrical discharge is generated under ambient temperature and pressure conditions.

[0020] In some embodiments, the sample to be treated includes one or more of a contaminant.

[0021] In some embodiments, the sample to be treated includes at least one of water, an aqueous solution, and an agricultural material.

[0022] In some embodiments, the sample to be treated includes a chemical reactant or a chemical compound, wherein the chemical reactant or chemical compound undergoes one or more chemical reactions when subjected to an electrical discharge. [0023] In some embodiments, the chemical reaction device includes an analytical device to provide one or more of an electrochemical detection and an electrochemical production.

[0024] In some embodiments, the analytical device includes a first electrode, a second electrode and a microfluidic channel, wherein the microfluidic channel provides for fluid communication between the first electrode and the second electrode.

[0025] In some embodiments, the piezoelectric generator converts mechanical energy into chemical energy.

[0026] In accordance with some aspects, a method is described, wherein the method includes generating an electrostatic charge, converting the electrostatic charge into an electric current or an ionic current, and applying the electrical current or the ionic current to a chemical reaction device to drive a chemical reaction in the chemical reaction device.

BRIEF DESCRIPTION OF THE DRAWINGS

[0027] FIGS. 1A-E provide a conceptual overview illustrating examples of how electrostatics can be harvested to do chemistry by converting mechanical energy into chemical energy. FIG. 1A provides schematic illustrations showing inputs that are mechanical motions such as adhesion and stress. FIG. IB provides a schematic illustration showing examples of triboelectric and piezoelectric effects that can cause changes in chemical structures thereby inducing an electrical field. FIG. 1C provides a schematic illustration showing that high voltages can generate a plasma (i.e., ionized gas). FIG. ID provides a schematic illustration of examples of direct usage of the plasma to store and transport energy in the form of chemical ions, such as ionized polymers. FIG. IE provides an example in accordance with some embodiments showing that chemical ions can be further converted to an electrical current to do high-voltage and low-voltage chemistry.

[0028] FIG. 2 provides schematic illustrations showing one exemplary mechanism to use electrostatic energy to drive chemical reactions.

[0029] FIGS. 3A-D provide schematic illustrations showing one exemplary system wherein charge is accumulated and neutralized on a belt through two corona discharges. FIG. 3A is an illustration showing intensified CCD images of a PDMS belt wrapped around two spaced apart rollers. FIG. 3B is a graph of normalized intensity as a function of wavelength. The optical emission is predominantly from the excited nitrogen molecules in the discharge. FIG. 3C is a graph showing the ionization fraction expected for a corona discharge. FIG. 3D shows reaction schemes for materials that were exposed to a positive corona and materials that were exposed to a negative corona.

[0030] FIGS. 4A-D describe an exemplary system for harnessing electrostatic energy for chemistry. FIG. 4A illustrates an exemplary experimental setup used to measure the charging and discharging rates of the electrostatic harnessing apparatus. FIG. 4B is a graph of charging rate as a function of relative humidity. FIG. 4C is a graph of charging rate as a function of belt speed. FIG. 4D is a graph of rotational input power as a function of velocity. The exact value (e.g., charging efficiency) would depend on materials chosen and their geometries.

[0031] FIGS. 5A-C illustrate an exemplary system for harvesting electrostatics for water treatment (bacterial sanitization). FIG. 5A illustrates an experimental setup for treating water at high voltages, this voltage is not applied by any external power source, but rather being carried by the electrostatics harvested via a mechanical motion between two non-conductive or semi-conductive materials. FIG. 5B provides pictures of bacteria cultures via the viable count method, before and after the treatment by the harvested electrostatics. FIG. 5C is a graph of bacterial killing percentage as a function of electrostatic treatment time.

[0032] FIGS. 6A-E illustrate an exemplary system for harvesting electrostatics for agricultural chemistry. FIG. 6A provides an exemplary schematic of a system for treating seeds with ionic wind (also known as a corona discharge) by collecting electrostatic energy. FIG. 6B provides pictures of beans before and after treatment compared to control samples. FIG. 6C is a bar chart of sprouting length distribution for control and treated beans. FIG. 6D provides images of control and treated wheat seeds as well as graphs showing wettability, hydration and germination test results for treated seeds compared to control seeds. FIG. 6E provides graphs showing hydration and germination test results for treated lentil seeds compared to control seeds.

[0033] FIGS. 7A-D illustrate an exemplary system for harvesting electrostatics for point- of-use detection at low voltages. FIG. 7A provides an exemplary schematic of a system for electrostatic charging a capacitor of (0-5V) to perform electrochemical reactions on a paperbased device. FIG. 7B provides oxidation reactions for the oxidation of iodide and aminophenol and provides images showing that both oxidized products form colored products on the paper-based device. FIG. 7C is a graph of tunable voltage based on resistance. FIG. 7D is a graph of tunable voltage based on the separation distance between two electrodes, and the rotational speeds of the electrostatic harvester.

[0034] FIGS. 8A-D illustrate an exemplary system for harvesting electrostatics to drive electrochemical production. FIG. 8A provides an exemplary schematic of an experimental setup of producing Cl" containing cleaning agents from seawater. FIG. 8B provides a summary of the reaction mechanisms at the anode. FIG. 8C is an image showing the setup of the reaction vessel and that the resulting mixture appears yellowish green. FIG. 8D is a graph of currentvoltage electrochemical screening.

DETAILED DESCRIPTION

[0035] The present application discloses various methods and systems for using electrostatic harvesting to store energy, produce chemical intermediates, and drive useful chemical reactions. Some aspects of the present application include: 1) Harvesting electrostatics to form ionic species (i.e., store the energy in chemical bonds, wherein the formation of ionic species itself is a chemical process); (2) Using those ionic species to drive additional chemical reactions including some that are otherwise non-spontaneous at ambient conditions; and (3) Using material properties to create desired ionic species and consuming them on the material to form stable products. In other aspects, materials used for harvesting electrostatics (conventionally known as triboelectric materials) can act as non-conductive cathodes and anodes, which undergo (and/or induce) reduction and oxidation electrochemical reactions in between, with a mechanical input.

[0036] In accordance with one aspect, the present invention relates to a system including an electrostatic energy generator, a charge carrier converter, and a chemical reaction device. In some cases, the charge carrier converter itself can also act as the chemical reaction device. The electrostatic energy generator generates an electrostatic charge and the charge carrier converter converts the electrostatic charge from the electrostatic energy generator into an electric current or an ionic current. The charge carrier converter is electrically connected to the electrostatic energy generator and the chemical reaction device is configured to receive the electric current or ionic current from the charge carrier converter. The electric current or ionic current drives a chemical reaction in the chemical reaction device. There are various configurations through which the chemical reaction device can receive the electric current or ionic current from the charge carrier converter. For example, the charge carrier converter can be configured to receive the electric or ionic current via a conductive material, an electrical discharge, an ion beam, or through mechanical contact. In accordance with some aspects, chemical ions generated from the charge carrier converter can directly participate in further chemical reactions in the chemical reaction device.

[0037] In accordance with one aspect, the present invention provides methods for conducting one-pot chemical reactions with no additional reactants needed besides the sample to treat (e.g., wastewater, medical equipment) and air. Samples suitable for treating include gas, liquid and/or solid samples. In accordance with certain embodiments, the effective chemical ingredients are generated via electrostatics in air for immediate usage onsite, without the need for storage and transfer.

[0038] Adhesion between materials from daily activities generates electrostatic charge. In accordance with one aspect, the disclosed method can be used to store such energy in chemical forms (e.g., ionization of polymeric materials) and transport it to the point of use. This energy can either be released at high voltage by building up excess charge in a capacitor (to do plasma chemistry or chemical biology) or low voltage by processing the charge directly (to do electrochemistry or form useful products). The systems and methods disclosed herein can be used for various interdisciplinary applications across multiple industries, including agriculture (seed germination), water supply and consumption (bacterial treatment and point-of-use detection), and global health (food sterilization and point-of-care diagnostics). In accordance with some aspects, the technology disclosed herein can be off-the-grid with an energy supply based on human capital, such that it is particularly suitable for developing economies. The disclosed technology offers a simple platform to perform chemical reactions that does not depend on expensive materials or modem infrastructures.

[0039] Materials that can be used in accordance with the present invention are not particularly limited. The materials can be natural, synthetic, inorganic, organic, metallic, polymeric, composite materials or combinations thereof. The materials can be charge-neutral, positively charged, or negatively charged. Some examples of inorganic non-metallic materials that may be used are disclosed in Zou et al., “Quantifying the triboelectric series,” Nat. Commun. 2019, 10 (1), 1427 (see, e.g., Fig. 3), the contents of which are hereby incorporated by reference. Examples of useful materials include, but are not limited to, those materials listed below in Table 1. Table 1. Examples of useful materials.

[0040] A conceptual overview of how electrostatics can be harvested to do chemistry is shown in FIG. 1. Mechanical motions (e.g., rotatory, oscillatory, or linear) can cause a structural change of chemical species and induce a potential difference in electrical fields, carried by static charges in chemical forms. In accordance with certain embodiments, the built- up voltage is high enough to ionize gas molecules and generate a plasma to do further chemistry. The plasma can be used for energy storage and transport via ionization. The present examples were studied in air, but other gas compositions (e.g., pure CO2, N2/CO2, Ar, etc.) could also be used. In some cases, the gas composition can be selected to induce different or/and selective reaction pathways for different applications (e.g., nitrogen fixation and CO2 reduction).

[0041] As shown in FIG. 1A, various types of mechanical motion inputs, such as adhesion and stress, can be used to initiate the process of converting mechanical energy into chemical energy. In accordance with one aspect, two sheets of polymers, typically with different triboelectric characteristics, can be used to induce an electrical field. One polymer may be an electron accepting insulator and the other polymer may be an electron donating insulator. Movement of one polymer surface relative to the other polymer surface results in the induction of an electrical field due to the triboelectric effect as shown in FIG. IB. Polymer ionization occurs at the inner surface of contact between the two polymer sheets. In addition to polymers, other materials such as an insulating or semi-conductive material, could be used. In accordance with another aspect, a piezoelectric material sandwiched between two conductors can be used to generate an electrical field due to the piezoelectric effect as shown in FIGS. 1A-B. Piezoelectric effect is the ability of a material to generate electrical voltage when subject to a mechanical stress. There are several classes of materials that could lead to piezoelectric effect. These materials include, but are not limited to, crystalline materials, ceramics, semiconductors, and polymers. Subjecting the piezoelectric material to stress and releasing the stress can cause changes in chemical structures, such as in the ZnO crystals, to induce an electrical field. As shown in FIG. 1C, static charges in chemical forms can build up in potential to a point where the built-up voltages can ionize air and generate a plasma. FIG. ID provides an example showing that the air plasma can be directly used to store and transport energy in the form of chemical ions, such as ionized polymers. In accordance with the embodiment shown in FIG. ID, the plasma can be directly used for energy storage and transport via the ionization of an insulating polymer, such as PDMS. Using rotational motions (e.g., as part of daily activities, such as cycling), the electrical energy of the ionized polymer can be harnessed, thereby generating an electrical current that can be released at either low or high voltages, depending on the capacitance.

[0042] The systems and methods disclosed herein provide a simple and low-cost platform to perform chemical reactions. Specific examples for using energy that is generated through electrostatics is exemplified in eight applications, shown in FIG. IE. For example, at high voltages, an electrical discharge can be used to 1) generate fertilizers (i.e., nitrogen fixation) 2) reduce carbon dioxide, 3) produce hydrogen gas, 4) produce chlorine gas, 5) purify water by killing pathogenic bacteria, 6) sanitize surfaces, and 7) improve seed properties for faster growth. The controlled release of energy at low voltages can 8) perform electrochemical reactions for production and detection purposes. In accordance with certain aspects, these and other applications are possible without the need for a power cord or a battery. These applications are representative of the potential uses for the disclosed systems and methods; many other applications would benefit from the disclosed systems and methods.

[0043] FIG. 2 provides schematic illustrations showing one exemplary mechanism to use electrostatics for chemistry, which involves generating charge (in chemical forms), converting charge to current, and using that current to do chemistry. In some aspects, current is produced in multiple steps. First, the triboelectric effect is used to build up enough charge to break down air. Subsequently, ionic gas molecules react with the surface of the belt due to the imposed direction of the electric field. This process is inverted to complete a cycle and harness electrostatic charging. The produced current can be used to drive chemical reactions at both high and low voltages. In accordance with some aspects, the generated charge in chemical forms can be involved in reactions directly. [0044] In more detail, FIG. 2 illustrates the use of a commercial benchtop Van de Graaff to efficiently store and transport electrostatic energy in chemical forms and use these chemical ions and the built-up potential to do useful chemistry. As shown in Step 1, charged species are initially generated from the triboelectric effect during contact between a belt (e.g., PDMS) and a roller (e.g., PTFE). In accordance with certain aspects, these materials are selected such that the roller is more negative in the triboelectric series and remains negatively charged after interaction.

[0045] As shown in Step 2, the amount of charged species is built up on the polymer belt between the roller and a finely tipped grounded electrode until the imposed electric field is sufficient to break down the surrounding air. This process results in a positive corona discharge where cation species generated from air (such as N2 ⁺ , N ⁺ , etc.) are forced to collide (and possibly react) with a rotating belt, which has net positive charges as a result. ⁶

[0046] Evidence of the cyclical belt charging process is illustrated in FIG. 3. Although FIG. 3 illustrates this process using a belt, the process is not limited to using a belt. In accordance with some embodiments, the described charging process can be used with other materials, such as i) a piece of non-conductive or semi-conductive material or ii) a carrier material coated with a non-conductive or semi-conductive material that act as the reactant. If the shape is different from a “belt” format, the geometry and the configuration of the device can be slightly different to accommodate the different configuration, but the underlying concept (of utilizing a mechanical input to build up chemical ions) stays the same.

[0047] An intensified CCD camera was used to detect any optical emission during the revolution of the belt. Near both the top and bottom combs, a glow was observed that stretched to the surface of the belt. The principal component of this emission was found to originate from the N2 rovibrational C ³ n _u ->B ³ n _g band. This lends evidence to the existence of excited state neutral species which are characteristic of any partially ionized gas. Thermodynamics calculations of a simplified two-component system are shown in FIG. 3C. Using the law of mass action and Saha equilibrium, ionization mole fractions of ~10 ^-8 to 10 ^-5 are expected for N2 ⁺ , the principal ionic species.

[0048] As shown in Step 3 of FIG. 2, the charging process is then reversed to extract charge from the belt and form a complete cycle for harnessing electrostatic interactions. During the extraction process, a negative-corona discharge forces ions generated in air to impact a cathode and generate secondary electrons. ⁷ Both anions and electrons are attracted towards the belt, neutralizing the positively charged species on the belt as it continues to rotate. This process converts electrostatic charge (carried by the belt, likely in chemical forms) into a DC current (carried by a conductive metal) during each rotation.

[0049] Charge-bearing species on the polydimethylsiloxane (PDMS) belt material appear to be ionic polymer fragments formed through mechanical action. ² PDMS undergoes a crosslinking process and becomes positively ionized upon electrospray ionization, characterized using mass spectroscopy. ³ FIG. 3D shows the proposed electrochemical reactions of materials interacting with positive and negative corona.

[0050] Although not wishing to be bound by theory, it is hypothesized that polymers undergo an electrochemical process (via either oxidation or reduction) to become charged, either positively or negatively, depending on its position in tribo-electric series (e.g., if the monomer unit contains an electron-donating functional group or electron-withdrawing functional group). Such electrochemical process may involve structural crosslinking or scission. For example, in the case of Nylon (polyamide, PA), the amide group becomes positively charged by forming a cyclic structure. ⁴ In the case of Teflon (PTFE) on the other hand, the carbon-carbon bonds break, forming fluorocarboanions. ⁵ Such a mechanism is expected to hold true for other halogen-containing polymers that can be negatively charged, such as Poly(vinylchloride) (PVC).

[0051] The triboelectric series and charge densities on polymeric materials ⁶ can be measured using a non-contact voltmeter to measure the amount and lifetime of the surface charge on different polymers.

[0052] Furthermore, bond enthalpies can be used to estimate the theoretical energy storage densities achievable on various polymer substrates. A preliminary example of this is shown in Table 2. The quoted surface charge density was obtained from probe measurements on polymer substrates. The peak charge density is observed to saturate as the induced electric field on the surface exceeds the available kinetic energy of the ionic species. Using the bond enthalpy of Si-O, this corresponds to a surface energy density of -3.8 mJ/m ² . The energy efficiency of this process depends on the charging mechanism and its inherent losses. For corona discharges, the principal energy loss is gaseous heating (-95%). The ability to store accumulated electrostatic charge in the form of longer living stable bonds as a form of chemistry will be investigated. These desirable products can then be used on-demand when they are needed.

[0053] Table 2 presents a preliminary estimate of the storage density of charged ionic polymer fragments on PDMS belts. The surface charge density is derived from surface probe measurements in the literature. ⁷ These values suggest an upper limit on the storage density based on the electrostatic repulsion caused by the surface charge. The storage of uncharged products on the belt will be investigated to improve the storage density.

Table 2. A preliminary estimate of the storage density of charged ionic polymer fragments on PDMS belts.

Surface Charge Number Charge Surface Density Ionization Bond Surface Energy

Density [#/m ² ] [mC/m ² ] Enthalpy (Si-O) Density [mJ/m ² ]

[eV]

[0054] Electron-beam irradiation is an analogous process that uses high-energy electrons to treat an object. Major industrial applications include, for example, 1) crosslinking of polymer-based products to improve mechanical, thermal, chemical and other properties, ⁸ ' ⁹ 2) material degradation for recycling purposes, ¹⁰ and 3) sterilization of water and medical goods. ¹¹ ' ¹²

[0055] One exemplary method for utilizing the DC current produced from the triboelectric effect is provided in FIG. 2. In the first, highlighted in step 4(i) in FIG. 2, the current can be used to charge up a capacitor. If the capacitor has low capacitance (e.g., ~ 10 pF), typical of a metal dome, then a rapid increase in voltage will occur,

[0056] For instance, with C ~10 pF, I ~ 10 //A, then dV /dt ~ 10 ⁶ V/s. This increase will continue until the air surrounding the capacitor is broken down (until about 3 kV/mm is achieved). In accordance with some aspects, a capacitor is not necessarily required. More generally, the process could include electrostatic harvesting a source of constant current (I) in ionic form. [0057] If a breakdown pathway to ground is presented, a rapid spark discharge will occur. This filamentary discharge is similar to lightning and highly efficient at producing reactive radicals and UV that are useful for a variety of applications. ^3,8

[0058] The current can also be used as a source for low voltage chemistry without the need for an external power supply or battery. For such applications, the current could be transferred directly to the load as it is produced, as shown in FIG. 2. Loads in excess of 100 k/2 allow constant voltages to be produced to drive various electrochemical redox reactions.

[0059] As shown in FIGS. 3A-D, charge is accumulated and neutralized on the belt using two corona discharges. FIG. 3A shows intensified CCD images of a PDMS belt. The optical emission is predominantly from the excited nitrogen molecules in the discharge. FIG. 3B provides an optical spectroscopy plot showing the dominant spectral components of the emission including the N2 rovibrational C ³ n _u ->B ³ Ilg band. FIG. 3C provides a graph of mole fraction as a function of electron temperature based on thermodynamic calculations showing the ionization fraction expected for a corona discharge. FIG. 3D provides hypothesized ionization mechanisms of tribo-positive materials (which become positively charged) and tribo-negative materials (which become negatively charged) through a corona discharge in air generated via contact electrification.

[0060] FIGS. 4A-D show one exemplary scheme for harnessing electrostatic energy for performing chemical reactions and shows impact of variables on the charging rate achievable by harnessing electrostatics. At increasing levels of humidity, the measured charging rate was observed to decrease. When a ground electrode was added to the discharge, the frequency of high voltage spark discharges was also observed to decrease in frequency. This can be attributed to the lower dV/dt and thus longer time it takes to reach the critical breakdown threshold voltage for air.

[0061] The charging rate was also measured as a function of the belt rotation speed using a DC motor as shown in FIG. 4B. The charging rate was found to be linearly proportional to the belt speed. Achievable rotation speeds for various applications such as bikes and hand cranks are included for comparison.

[0062] A model was developed to quantify the input power requirements to achieve particular rotation speeds. It was found that all of the highlighted rotation speeds in FIG. 4D are well below the threshold power output of a human. The efficiency of the process is limited by the frictional losses encountered by the belt during rotation and gas phase recombination within the corona discharge. These macroscopic losses can be reduced or eliminated by quantifying the energy storage and process efficiency using the belt ionization mechanism disclosed herein. This will only include bond enthalpies and the kinetic energies of ionic species. This formulation can then be extended to include forming intermediate products that scavenge the surface charge away on the polymer substrate.

[0063] The proposed design is unique because it can be passively grounded during everyday activities. In particular, it can be combined with any rotary motion. For example, it can be combined with rotary motions associated with daily life, such as a bicycle, fan, windmill, or a hand crank.

EXAMPLES

[0064] Examples are provided below to facilitate a more complete understanding of the invention. The following examples illustrate the exemplary modes of making and practicing the invention. However, the scope of the invention is not limited to specific embodiments disclosed in these Examples, which are illustrative only, since alternative methods can be utilized to obtain similar results.

[0065] Various demonstrations are presented below to illustrate the versatility of the methods disclosed herein. When the harvested electrostatic energy is released at high voltages, plasma occurs in the form of either a spark or corona discharge. ¹³ ' ¹⁵ The transition between these two regimes is determined by how uniform the electric field is across the gap between the electrodes. Any strong non-uniformities, such as using a pointed electrode, can cause a transition to a corona type discharge.

1. High Voltage for Bacterial decontamination

[0066] FIGS. 5A-C provide one example of harvesting electrostatics for water treatment (bacterial sanitization) at high voltages. FIG. 5A shows an experimental setup for using such a method for water sanitization, specifically in killing Escherichia coli (E. coli), that is a major contaminant in water and on foods. The E. coli often originates from soil or irrigation water contaminated by animal or human feces. ¹⁶ [0067] FIGS. 5B-C show that the disclosed method is highly efficient (>99%) at eliminating of the E. coli. One minute of plasma treatment was enough to reduce population of bacteria in tap water (-1000 E. coli /sample before treatment) and 10 minutes for bottled mineral water, below the detection limit. The difference observed appears to be due to the residual chlorine in tap water (which is typically used by urban water purification facilities), which may have killed some of the added E. coli.

[0068] Air plasmas are sources of reactive oxygen and nitrogen species, such as O, Ch, OH, NO and NO2. Non-equilibrium electrons within the plasma drive the gas kinetics responsible for the production of these reactive molecules. The oxidizing molecules and radicals have direct impact on the membrane lipids and protein molecules of cells and microorganisms. ¹⁸

[0069] A study by Dobrynin et al. using DC corona discharge shows no inactivation of bacteria in pure N2, pure O2 nor an N2-H2O mixture. ¹⁹ Their results show that neither UV, ozone, nor other neutral active species alone produced by corona affects bacteria viability. The best sterilization was achieved in the case of direct treatment, when discharge was ignited through an O2-H2O mixture.

2. High Voltage for Improvement of Seed Properties

[0070] FIGS. 6A-E illustrate one example of harvesting electrostatics for agricultural chemistry. FIG. 6a show a schematic of the setup used to treat the seeds with ionic wind by collecting electrostatic energy. Seeds exposed to the ionic wind resulted in an increase in the rate of hydration and ultimately germination. Three types of seeds were treated: beans, wheat and lentil seeds. These crops are of major importance in agriculture and to feed the population of the world.

[0071] FIG. 6B shows that this treatment was observed to reduce microbial growth on beans in a flooding scenario (beans were fully immersed in MilliQ water for 10 days). There is a significant difference in microbial activity for the two treatments — the 10 min plasma treatment shows significantly less growth of mold. Growth of white mold on beans was only found for the No treatment seeds (the inset shows a close-up image of the mold). Growth of grey mold on beans was observed in both plasma-treated set and the control set (the inset shows a close-up image of the mold). There was approximately twice as many grey mold colonies for the beans without plasma treatment. The grey mold appeared mostly in the area of the hilum on the beans. It is hypothesized that the fungi are Rhizopus, Penicillium, and possibly Fusarium Spp.

[0072] Cold plasma treatment inactivates bacteria and fungi present on the seeds, which means that plasma-treated seeds would be less likely to pose health risks related to microbial contamination and cause economic losses. ²⁰ ' ²¹

[0073] FIG. 6C shows the radical length of beans four days after sprouting, measured among a set of 50 seeds. The control set shows a normal distribution with an average radical length of 37.9 mm. The plasma-treated set has a skewed distribution with 36% more population in the upper range (>50mm), though the average radical length is only slightly higher at 38.0 mm.

[0074] FIGS. 6D-E show improvements in surface wettability, hydration, and seed germination speed of wheat and lentil seeds with 10-minute treatment through ionic wind. 200 seeds were studied in each set of experiment, which includes control (dashed lines), 10-minute treatment (solid lines), low supply of water (grey lines, 5g water/lg cotton), and high supply of water (black lines, 10g water/lg cotton). The error bars depict the standard deviations. There is a significant decrease (up to 40° for wheat) in contact angle between the seed, water and air. The treatment disclosed herein increases wetting properties (i.e., the hydrophilicity) of the surface of seeds, improving the water absorbance (up to 4% increase for wheat and 12% increase for lentil seeds) before the germination starts. ²² At a given time during the germination process, the ionic wind treated sample has a higher germination yield of up to 15% for wheat and 30% for lentil seeds.

[0075] The seed coat is a semi-permeable membrane that allows passage of small molecules or ions. The oxidizing agents and radicals generated from the ionic wind likely influenced the early growth of seeds. ²³ Plasma treatment has been reported to cause erosion of the seed coat erosion. Some seeds require scratching or nicking of the hard seed coat to allow moisture to enter the seed to begin the germination process - it was observed that as a result of plasma treatment seeds often have a slightly damaged surface. ^{20, 24}

[0076] The accelerated germination process means that sprouts will emerge out of the soil earlier. Such improvement helps farmers to reduce the risk of over hydration or dehydration of seeds due to prolonged time exposure in extreme climates (e.g., during a storm season or a dry season).

[0077] Improvement of germination, longer shoots and roots of the seedlings, and higher yields of plasma-treated seeds have been reported by several authors using various seeds, including wheat ²⁵ ' ²⁷ , maize ²⁸ , and soybeans ²⁹ .

[0078] Plasma-activated water, which contains nitrates and hydrogen peroxide, has a fertilizing effect on the growth of the plants. ³⁰ These reactive nitrogen and oxygen species stimulate a chemical and hormonal response in the seed that breaks its dormancy by weakening the endosperm (i.e., the coat of the seed) and moving the stocked-up resources of the seed to a ready-to-use location. This allows the seedling to erupt easily from the seed and to grow faster and healthier. ³¹

3. Electrochemical Detection and Production

[0079] Different from the first two demonstrations, which utilize the special characteristics of plasma at high voltages, the third demonstration releases a controlled voltage at lower ranges (e.g., 0-5V) to do electrochemistry. FIGS. 7A-D provide an example of harvesting electrostatics for point-of-use detection at tunable voltages. This setup is an example in which harvesting of electrostatics gives a relatively constant current source. This setup acts as passive amperometry, during which the current (and therefore the resulting rate of chemical reactions) is tunable via the amount of the mechanical input (e.g., rpm in the case of using a rotary setup). FIG. 7A shows the experimental setup of electrostatic charging a capacitor of (0-5V) to perform electrochemical reactions on a paper-based device. As shown, the electrostatic harvester connects directly to a paper-based analytical device with wax-printed channels for aqueous-based reactions.

[0080] FIG. 7B provides reaction mechanisms for exemplary redox-active analytes. For this example, the reactions include the oxidation of iodide and aminophenol, both forming colored products. This application is particularly useful for low-cost monitoring and detection of environmental contaminants, such as heavy metals and aromatic toxicants.

[0081] FIG. 7C shows a linear relationship between the voltage released and the resistance of the device, which is tunable by the concentration of electrolytes and separation distances between electrodes. The voltage can be further tuned by the rotational speed of the polymer belt around rollers, as shown in FIG. 7D. [0082] Table 3 lists a variety of potential analytes whose oxidation can be monitored visually (forming colored products) and whose redox potentials are fully accessible to the disclosed device.

Table 3. A selection of analytes that undergo redox reactions with a colored product or intermediate. Redox voltages were measured against standard Ag/AgCl electrodes.

[0083] In addition to detection, the electrostatic harnesser can also be used for chemical production, such as producing chlorine-related oxidizing agents. FIGS. 8A-D provide an example relating to harnessing electrostatics to drive electrochemical production. FIG. 8A illustrates one example of an experimental setup of producing Cl-containing cleaning agents from seawater. FIG. 8B provides the reaction mechanisms at the anode; chloride anions are oxidized into Ch, CIO", CICh' and CIOs'. FIG. 8C shows that electrical discharge through air onto a concentrated NaCl aqueous solution turns the mixture into a light-green color after approximately 2 minutes, likely due to the production and dissolution of Cb. Preliminary electrochemical current-voltage screening shows multiple peaks, likely due to chlorine- containing products at different oxidation states, such as CI2, CIO", CIO2, and CIO2' (FIGS. 8B and 8D).

[0084] The experimental results were obtained using the high-voltage setup of the lightning experiment. The lightning setup features similar discharge characteristics but amplifies the current to more quickly produce desired products.

[0085] Previous research has shown the mechanism and kinetics of ozone reacting with chloride anions to form chlorine and related products. ³² ' ³³ Therefore, the production of ozone driven by electrical discharge is crucial to for further oxidizing chloride anions in the aqueous phase.

EXPERIMENTAL METHODS

A. Device setup and characterization

[0086] Electrostatic charge was harvested by rotating a 1 mm thick rubber belt around 1 diameter silicon and nylon rollers. The rollers were placed 30 cm apart. Rotation was driven using a DC motor with three separate rotation speeds, 60 rpm, 90 rpm, and 120 rpm. The charging rate from the device was measured by connecting it to a 10 F electrolytic capacitor. The voltage across the capacitor was measured over time using a 350 MHz bandwidth Rohde & Schwarz RTM 2034 oscilloscope and voltage probe. Humidity was controlled by placing the apparatus in a Coy glovebox with a model 5100 microcontroller to maintain specified levels of relative humidity. High voltage discharge characteristics were measured using a Model 6595 Pearson current probe.

[0087] A dynamics model was used to quantify the amount of input power required to rotate the apparatus. The coefficients of static and kinetic friction required for the model were measured using a pull test with a Instron Universal Test System. Separate weights of 140 g, 340 g, and 1140 g were used. The tensile load was measured using an elongation test on the rubber belt.

B. Bacterial decontamination studies

[0088] E. coli cells were grown overnight in Luria Bertani (LB) medium at 37°C, diluted 1 : 100, and re-grown in LB medium. For colony-forming unit (CFU) counts and viability tests, cells were diluted serially in LB medium and 50pL of solution was spread on LB agar plates, which were incubated for 24 h at 37°C. Aqueous samples of E. coll were prepared in three types of water: double distilled, tap, and bottled water (purchased from Evian), with standard concentration of 1.0* 10 ³ cells/mL.

[0089] A metallic dome (r = 11cm) was used as a high-voltage capacitor to collect the electrostatics harvested from material adhesion. A plastic cylindrical container (r = 1.5 cm, I = 1.5 cm) was in direct contact with the dome surface, which acts as the positive electrode. A metal rod with a spherical end (r = 0.5 cm) was placed right above the container, acting as the negative electrode. Aqueous solutions of E. coll (3mL) were added into the container, between the two electrodes (d = 1.2 cm) with an air gap (d = 0.6 cm). For consistency across measurements, discharges were maintained with a periodicity of ~ 50ms and amplitude of ~400mA, measured by a Rohde & Schwarz RTM 2034 oscilloscope and a Pearson 6595 current monitor.

[0090] Viability tests using plate count method were performed on a set of controls (both positive and negative) and samples treated with plasma at various exposure durations.

C. Seed germination studies

[0091] The following seeds were purchased from Johnny’s Selected Seeds, Winslow, ME: Spring wheat (Triticum aestivum L. variety ‘Glenn’), beans (Phaseolus vulgaris variety ‘Bush Beans’) and lentils (Lens culinaris variety ‘xxx’). Similarly, to the setup discussed in Section B, five seeds at the time were treated at the same time inside of the container. The ionic wind (instead of spark discharge) was generated using a metal wire with a sharp end as the negative electrode. The sharp end of the wire was placed on top of the seeds with an air gap (d = 0.5 cm). The ionic wind provides a DC compared to the AC spark discharge that lasts for ~ ns.

[0092] The wetting properties of wheat and soybeans were established using a goniometer (model 500-F1, Rame-Hart) and analyzed using the ImageJ contact-angle plugins.

[0093] The effect of ionic wind exposure on kinetics of water hydration (imbibition) and germination for seeds of wheat, beans, and lentils was investigated. The seeds (50 seeds for each treatment) were germinated on wet cotton (1 g) at room temperature in round Petri dishes. The cotton was hydrated with 5g or 10g of water per 1g of cotton. The emergence of the radicle through the endosperm (observed by eye) was defined as successful germination. The relative proportion of seeds that successfully germinated was plotted for each point of time. The hydration of the seeds was followed by draining the seeds from water, removing any excess water by gently rolling them on paper tissues, and by weighing the seeds every 2-4 hours using a microbalance. The degree of water imbibition was calculated using the following equation: (AW(/)/W 0) ^x 100% =[(W(Z)-W0]/W 0 ^x 100%, where WO is total weight of the seeds before the addition of water, and W(/) is the total weight of seeds at each point of time (t) after water was added.

D. Electrochemical detection studies

[0094] Microfluidic zones were patterned onto chromatography papers using a wax printer. The patterned paper was placed in an oven (T = 145 °C) for 60 s to allow the wax to penetrate the paper fully. Graphite electrodes were prepared by painting chromatography paper with carbon graphite paste and left overnight to dry. Once dry, electrodes were cut and taped to the device taped to the device from behind, in contact with the hydrophilic channels (FIG. 7A). One alligator clip joins the electrostatic harvester with the positive electrode of the device. The other alligator clip joins the negative electrode of the device to the ground.

[0095] Aqueous solutions containing 100 mM of either Nal or 4-aminophenol were used as example analytes due to the generation of colored products upon oxidization (FIG. 7B). All solutions contained 100 mM KC1 as supporting electrolyte. A small volume (~40pL) of the sample is added to the center of the device and allowed to wick towards the electrodes through the hydrophilic channel.

[0096] A Fluke 77IV multimeter was used to measure the resistance of the device (before and after the experiment) and the voltage generated during the experiment (FIG. 7C).

[0097] Electrostatics could also be used to sterilize sprouts at the point-of-use. The world’ s food supply consists of up to 70% of seeds, mostly in the form of grains or beans. Grains are also an important food source for farm animals. One of the most sensitive phases in the life of a crop is germination. The sprouting seed are in this phase sensitive to drought, flooding, or soil- or water-borne pathogens, such as molds and fungi. Sprouts is a food source of significant economic and nutritional value. ³⁴

[0098] Sprouts are a nutrients source of food with a high economic value per unit weight. Sprouts are produced by placing seeds in trays, bins, or rotating drums, watering regularly for four to seven days. Common sprouts used for food include, alfalfa, broccoli, clover, mung bean, wheat, sunflower, radish, sunflower, and soybean. ³⁵

[0099] Sprouts are a source of a reoccurring food-borne illness that affect large groups of people, commonly resulting in fatalities. The outbreaks can take long time to trace, increasing the number of people affected. In the US alone there were 56 foodborne outbreaks between 1998 to 2016, 29 were multi-state outbreaks. These outbreaks resulted in a total of 1,878 cases of illnesses. ³⁶ The most common pathogens in these outbreaks are -Salmonella spp. (39 outbreaks) and E. coli (10 outbreaks).

[0100] Contaminated sprouts cause severe damage to the economy and the public trust of the farmers that produces the sprouts, and the stores and restaurants that sell them. There is hence a strong incentive to use new cost-effective innovations that could reduce or removes the problem of bacterial contamination on sprouts. ^35,37

[0101] Seeds that are used for germination are currently sterilized just before starting the germination using solutions of calcium hypochlorite. ³⁸ Sterilization using plasma enables sterilization of the seeds in a dry state, before they are shipped in closed bags to the farmers. Common methods of dry sterilization include gamma irradiation or heat treatment, both methods are detrimental to the essential biological processes needed for the germination of quality sprouts for human consumption.

[0102] In accordance with one aspect, the system disclosed herein allows one to perform sterilization, gemination enhancement and fertilizer enrichment in one pot in a farm or remote setting. The chemical reactor component of the disclosed device first treats seed surfaces through air, during which nitrogen is fixed into fertilizers and captured in the reservoir for either immediate or future usage. The seeds can then be exposed to plasma under ambient (temperature and pressure) conditions, which allows the technology to require very little capital to fabricate and operate. This provides an advantage of other systems which require a vacuum system and precisely controlled capacitive-inductive plasma source. Furthermore, in accordance with some aspects, the present application describes a system that utilizes mechanical energy as an input to drive chemical reactions. An energy storage component (e.g., a battery) or a power amplifier (e.g., transformer) is not required. This allows this technology to be uniquely suited for on-site applications where energy-harvesting is possible. [0103] The methods and systems disclosed herein may be used to address issues associated with high salinity. Plasma treatment changes in seed surface wettability resulting in increases in water absorption. ^{22, 39} Less irrigation water would be needed for plant growth, which would be particularly important in countries in which water resources are limited. Germination is especially problematic in soils that have high levels of soluble salts. The salts can be toxic or cause osmotic stress in the seeds. Seeds that imbibe water have difficulty absorbing water in saline soils because these soils have a low water potential. There are more than 400 million hectare (23% of the arable land) of farmlands that are high in salinity, and over 1500 million ha of dryland agriculture. Most of these poor-quality lands are in developing economies, [ref: FAO/UNESCO],

[0104] Although the invention has been described and illustrated in the foregoing illustrative embodiments, it is understood that the present disclosure has been made only by way of example, and that numerous changes in the details of implementation of the invention can be made without departing from the spirit and scope of the invention, which is limited only by the claims that follow. Features of the disclosed embodiments can be combined and/or rearranged in various ways within the scope and spirit of the invention to produce further embodiments that are also within the scope of the invention. Those skilled in the art will recognize, or be able to ascertain, using no more than routine experimentation, numerous equivalents to the specific embodiments described specifically in this disclosure. Such equivalents are intended to be encompassed in the scope of the following claims.

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