Use of nanosealant in geopolymer systems

Abstract

Sealants are deployed to a set geopolymer material and are reacted to seal defects. The sealant is brought into contact with the set geopolymer and allowed or caused to react to seal defects of the set geopolymer. Such methods can be used to repair defects of set geopolymers deployed in subterranean wells.

Description

USE OF NANOSEALANT IN GEOPOLYMER SYSTEMSCROSS-REFERENCE TO RELATED APPLICATIONS

[0001] This application for patent claims priority benefit of United States Provisional Patent Application Serial No. 63 / 666,455 filed July 1 , 2024, which is entirely incorporated herein by reference.FIELD

[0002] This application for patent relates to geopolymer compositions. More particularly the invention relates to the use of repair sealants with geopolymers.BACKGROUND

[0003] Geopolymers are a class of materials that are formed by chemical reaction of various aluminosilicates, oxides, and silicates to form an amorphous three- dimensional framework cement-like structure. The term “geopolymer” was proposed and first used by J. Davidovits. His work is described in Davidovits, J: “Synthesis of New High-Temperature GeoPolymers for Reinforced Plastics / Composites.' Society of Plastics Engineers, IUPAC International Symposium on Macromolecules, Stockholm (1976). Other terms have been used to describe materials synthesized utilizing a similar chemistry, such as alkali-activated cement, geocement, alkali- bonded ceramic, inorganic polymer, and hydroceramic. In the following description, the term “geopolymer” will be used.

[0004] Geopolymers have been investigated for use in several applications, including as concrete systems within the construction industry, as refractory materials and as encapsulants for hazardous and radioactive waste streams. Geopolymers are also recognized as being rapid setting and hardening materials. They exhibit superior hardness and chemical stability. The preparation of geopolymers generally involves mixing a blend of reactive solid materials and activating the polymerization reaction by adding an alkaline solution. Typically, the slurry mixture is then applied and allowed to harden in place. In construction, faster hardening is usually valued.

[0005] In the hydrocarbon industry, cement-like materials are used to line wells to provide isolation and structural support within the well. Use of cement-like materials in hydrocarbon wells presents unique challenges. The slurry mixture precursor is typically pumped over long distances to the location where the mixture is to set, so the mixture must be pumpable without undue burden on equipment. Additionally, ambient conditions encountered in a typical hydrocarbon well are much more extreme than those encountered in a typical construction application. Further, the large vertical extent of hydrocarbon well applications presents challenges of density, temperature, and pressure not faced in the construction industry. Other applications, like plugs, squeeze, and injector wells for water or carbon dioxide, also require a cementitious precursor to be pumped to an application site, so geopolymer compositions find broad use where pumping is required.

[0006] Upon setting, geopolymers can be subjected to stresses, such as thermal and mechanical stresses from fluid flows and earth movements. These stresses can result in formation of cracks in the geopolymer, which in turn can lead to loss of isolation with a well. Methods are needed to manage stresses and repair cracks in geopolymer structures.SUMMARY

[0007] Embodiments described herein provide a method of treating a subterranean well, the method comprising obtaining a sealant that reacts when brought into contact with a sealant setting component of a set cementitious material; pumping the sealant into a subterranean well containing a set geopolymer material that has a sealant setting additive; and reacting the sealant to seal defects of the set geopolymer material.

[0008] Other embodiments described herein provide a method, comprising obtaining a sealant that reacts when brought into contact with a sealant setting component of a set cementitious material; disposing the sealant in contact with a set geopolymer material that has a sealant setting additive; and reacting the sealant to seal defects of the set geopolymer material.

[0009] Other embodiments described herein provide a method, comprising forming a geopolymer that contains a sealant setting additive; obtaining a sealant that reacts when brought into contact with a set cementitious material containing a sealant setting component; disposing the sealant in contact with the geopolymer; and reacting the sealant to seal defects of the geopolymer.DETAILED DESCRIPTION

[0010] In the following description, numerous details are set forth to provide an understanding of the present disclosure. However, it may be understood by those skilled in the art that the methods of the present disclosure may be practiced without these details and that numerous variations or modifications from the described embodiments may be possible.

[0011] At the outset, it should be noted that in the development of any such actual embodiment, numerous implementation — specific decisions are made to achieve the developer's specific goals, such as compliance with system related and business related constraints, which will vary from one implementation to another. Moreover, it will be appreciated that such a development effort might be complex and time consuming but would nevertheless be a routine undertaking for those of ordinary skill in the art having the benefit of this disclosure. In addition, the composition used / disclosed herein can also comprise some components other than those cited. In the summary of the disclosure and this detailed description, each numerical value should be read once as modified by the term "about" (unless already expressly so modified), and then read again as not so modified unless otherwise indicated in context. The term “about” should be understood as any amount or range within 10% of the recited amount or range (for example, a range from about 1 to about 10 encompasses a range from 0.9 to 11 ). Also, in the summary and this detailed description, it should be understood that a concentration range listed or described as being useful, suitable, or the like, is intended that any concentration within the range, including the end points, is to be considered as having been stated. For example, “a range of from 1 to 10” is to be read as indicating each possible number along the continuum between about 1 and about 10. Furthermore, one or more of the data points in the present examples may be combined together, or may be combined withone of the data points in the specification to create a range, and thus include each possible value or number within this range. Thus, even if specific data points within the range, or even no data points within the range, are explicitly identified or refer to a few specific data points, it is to be understood that inventors appreciate and understand that any data points within the range are to be considered to have been specified, and that inventors possessed knowledge of the entire range and the points within the range.

[0012] Regarding chemical formulas, it should be noted that measurements may not conform precisely to the chemical formulas described herein due to various sources of error that can affect real-world testing. The chemical formulas described herein should therefore be understood as expressing the nominal chemical makeup of compounds, where real-world testing may show close, but not exact, conformity to the formulas.

[0013] As used herein, “embodiments” refers to non-limiting examples disclosed herein, whether claimed or not, which may be employed or present alone or in any combination or permutation with one or more other embodiments. Each embodiment disclosed herein should be regarded both as an added feature to be used with one or more other embodiments, as well as an alternative to be used separately or in lieu of one or more other embodiments. It should be understood that no limitation of the scope of the claimed subject matter is thereby intended, any alterations and further modifications in the illustrated embodiments, and any further applications of the principles of the application as illustrated therein as would normally occur to one skilled in the art to which the disclosure relates are contemplated herein.

[0014] Sealant materials that can react, or be caused to react, when in contact with set cementitious materials or species within a set cementitious material, can be used to repair defects in hardened geopolymers. Geopolymer materials, and other alkali activated materials, are formed by disposing an aluminosilicate source and an alkali activator in a water mixture having high pH. Geopolymers are cementitious materials made from sources of oxidized aluminum and silicon. Currently, geopolymers are mostly made from aluminosilicate byproducts, but geopolymers can be made from a properly prepared mixture of alumina and silica as well. Examples ofalum inosilicate sources that can be used include (but are not limited to) ash materials such as fly ash and volcanic ash, slag materials such as blast furnace and mining slags, calcined or partially calcined clays, biomass ashes, and the like. Common ingredients are metakaolin and blast furnace slag.

[0015] Alkali activators can be solid materials or liquid materials. Aqueous solutions of metal hydroxides, such as sodium or potassium hydroxide, can be used as alkali activators. Solid activators, such as alkali metal salts, for example silicates, orthosilicates, metasilicates, pyrosilicates, hexafluoridosilicates, carbonates, sulfates, sulfites, phosphates, oxalates, fluorides, iodates, and molybdates can be used along with alkaline earth metal hydroxides, oxides, and / or peroxides as coagents to form a high pH aqueous medium for reacting the aluminum, silicon, and oxygen in the geopolymerization reactants. Where the reactant materials have metal oxides such as calcium oxide in significant quantities, the alkali metal salts can be used without additional alkaline earth metal co-agents can be omitted. The oxidized aluminum and silicon materials are dispersed into an aqueous medium, along with the alkali activators, to form a geopolymer precursor that is then deployed to a target location and hardened into a geopolymer.

[0016] After the geopolymer has set and hardened, where defects exist or develop in or around the geopolymer, a sealant material can be applied in contact with the geopolymer and reacted to seal and close the defects. Such defects include defects within the geopolymer itself, such as cracks, holes, fissures, and excessive porosity, and also defects at interfaces between the geopolymer and other materials, such as debonding or detachment defects. All these defects of the geopolymer that give rise to enlarged openings can allow unwanted fluid flow in, around, and through the geopolymer. Sealants for closing or reducing such defects are typically dispersions of silica, metal silicates, or both that, when placed in contact with a set cementitious material react and harden. An example is the D264 Nanosealant material available from SLB of Houston, Texas. Such solutions are typically low-viscosity solutions that allow pumping of the sealant material to the geopolymer. For example, where a geopolymer is deployed in a subterranean location, like a well, the low viscosity sealant solution can be pumped into the well to a location in contact with thegeopolymer. Commonly a geopolymer material is placed and hardened in the annular space between a well casing and the well wall. The solution flows through the annulus and around the geopolymer, penetrating the geopolymer and filling small defects. In some cases, upon contact with the set geopolymer, the sealant begins reacting and hardening to restore the geopolymer to a relatively impermeable state. In other cases, the sealant can be deployed to the set geopolymer, to a location containing defects, and caused to react and harden to restore the geopolymer.

[0017] The sealant materials used herein can be colloidal silica materials, alkali metal silicates (metasilicate, orthosilicate, pyrosilicate, or combination thereof), for example potassium silicates, sodium silicates, or a combination thereof. Some such solutions or dispersions are sometimes called “water glass.” These materials are typically stable in neutral and alkaline solutions, but will react with substances found in hardened geopolymers to polymerize into a hard, or substantially hard, material. In some cases, silica gels are formed. In some cases, the sealants are deployed in a microcrystalline or nanocrystalline form, for example as nanocrystalline silica. The silica can also be amorphous or partially crystalline. Mixtures of silica particles having different morphologies can also be used. Where carbon dioxide is present, carbonates can also be formed in addition to silicas. These materials can form solid seals within defect areas of a geopolymer to seal the defects and restore impermeability. Thus, in some cases, the sealant material can be, or can comprise, carbon dioxide. For example, carbon dioxide gas can be placed into contact with a set geopolymer in some cases to precipitate carbonate solids in defects to slow or stop flow through defects of the geopolymer. In some cases, the carbon dioxide gas can be provided with, or combined with, carbon dioxide solution, also referred to as carbonic acid.

[0018] The presence of metal ions such as calcium and aluminum in the geopolymer may facilitate reaction of the sealant materials in some cases. When using geopolymer reactants that contain no metal ions that are at least divalent, adding calcium oxide, calcium hydroxide, calcium chloride, or any combination thereof to the geopolymer precursor, such that calcium ions are present in the geopolymer that results from the precursor, may facilitate using sealants such asthose described herein after the geopolymer has set and hardened. Sealants using alkali metal silicates will generally react with calcium ions (and other divalent ions such as magnesium and beryllium) to precipitate solids, which may be or include calcium silicate in a gel form. Likewise, adding an aluminum material such as aluminum chloride to the geopolymer precursor, such that aluminum ions are present in the resulting geopolymer, can also facilitate using such sealants. Other multivalent (at least divalent) metal ions, such as magnesium and gallium, will also facilitate reaction of the sealants herein. Such metal ions can be used in any combination. Thus, a geopolymer precursor can be made that includes calcium oxide and aluminum chloride, and other combinations can be used.

[0019] Generally, sealant setting additives are materials that trigger chemical reactions to set, solidify, or gel a sealant material. The additives can be materials that precipitate solids from a sealant material, or from the set geopolymer itself. The sealant setting additives herein are materials that are added to an alkaline-reactive precursor blend or to a set cementitious material. In one aspect, the sealant setting additive is a salt that can form a gel when in contact with a water dispersion of silica. In another aspect, the sealant setting additive is an alkaline material that can precipitate solids when an acidic sealant material is contacted with the alkaline material. Forming a gel having good shear stability, and / or precipitating solids, in defects of a geopolymer material can seal the defects and generally reduces porosity of the geopolymer material. In some cases, the reaction can form a hydrogel that, over time and with exposure to elevated temperature, for example in a subterranean environment, will eliminate water and may form solids.

[0020] Such sealants will react with set geopolymers that have common additives, such as accelerators, retarders, density modifiers, viscosity modifiers, anti-foam agents, defoamers, silica, fluid-loss control additives, dispersants, expanding agents, and anti-settling additives. The sealants can work with geopolymers made from precursors having wide range of slurry densities from about 11 pounds per gallon up to about 25 pounds per gallon. Such sealants can also be used in geopolymer applications that are not associated with subterranean wells, for example in industries such as construction and mining.

[0021] Acidic materials can be used as sealants for geopolymers. Acidic solutions can be deployed into contact with the geopolymer to react with alkaline materials in the geopolymer to precipitate solids, for example by reaction of silicate ions with hydrogen ions. Thus, an alkaline material can be used as a sealant setting additive, and the acidic solution can act as a sealant, reacting with the alkaline material to form a gel and / or precipitate solids. Carbon dioxide can also precipitate silica gel and carbonates from an alkali metal silicate material. In other cases, organic molecules containing hydroxyl (-OH) groups, such as ethanol and phenolphthalein, can be used as a sealant setting additive in a geopolymer such that an acidic sealant, when brought into contact with the geopolymer containing the organic hydroxyl sealant setting additive, forms a polymeric substance to close defects of the geopolymer.

[0022] These sealants can also be used to improve the mechanical properties of a newly deployed geopolymer material. The material that develops from the reaction of the sealant materials with the sealant setting additives can penetrate the geopolymer material and add toughness to the material to absorb stresses that might otherwise produce cracks. In such cases, a sealant material can be deployed (form example pumped) to a location in contact with a newly set geopolymer containing a sealant setting additive and allowed to react to form a strength component for the geopolymer.

[0023] In general, the sealants herein can be used to repair defects in and around geopolymer installations in a well. In one case, the sealant can be pumped into the well inside a casing of the well and then pressured through openings in the casing to contact a geopolymer disposed between the casing and the wall of the well. The sealant reacts with sealant setting additives in the geopolymer upon contact, and precipitated solids or gel or polymer resulting from the reaction can fill the openings in the casing to repair casing leaks. In another case, the sealant can be pumped into the annular space between the casing and the well wall to repair defects of a geopolymer installation within the annular space, which may be defects in the geopolymer matrix itself or debonding between the geopolymer and the casing.

[0024] A sealant setting additive can be added to a geopolymer before or after the geopolymer is hardened. In one aspect, a sealant setting additive can be added to ageopolymer precursor so that, after the geopolymer precursor is set, the sealant setting additive is disposed within the geopolymer for future use with a sealant material to seal future defects. In another aspect, the sealant setting additive can be added to the set geopolymer before subsequently adding a sealant material selected to react with the sealant setting additive. Thus, in such cases, to seal defects of a geopolymer material, a fluid that is, or comprises, a sealant setting additive is placed into contact with the geopolymer material, and then the sealant material is placed into contact with the sealant setting additive to form sealing materials within the defects of the geopolymer.

[0025] The sealant setting additive may be a salt having solubility in water of at least about 0.15 g / mL, such as at least about 0.20 g / mL, for example at least about 0.30 g / mL or 0.40 g / mL. Examples of sealant setting additives are alkali metal salts, alkaline earth metal salts, ammonium salts, and boron group metal salts. The salts may have inorganic or organic anions. Thus, for example, moderately soluble to highly soluble chloride, iodide, bromide, sulfate, persulfate, nitrate, phosphate, chromate, dichromate, silicate, carbonate, bicarbonate, manganate, permanganate, iodate, borate, borohydride, bromate, perchlorate, thiosulfate, chlorite, hypochlorite, and hypobromite salts, and mixtures thereof can be used as sealant setting additives in geopolymers. Salts with organic anions can also be used. Moderately soluble to highly soluble formate, acetate, citrate, oxalate, propionate, benzoate, sulfonate, alkylsulfonate, maleate, malonate, butyrate, gluconate, mellitate, amino acid, and tartrate salts, and mixtures thereof can also be used. Mixtures of organic and inorganic metal and / or ammonium salts can also be used.

[0026] The sealant setting additive can be a material that participates in the geopolymerization reaction in some way, but in general where such materials are used, an excess of the material, above what is typically used to drive a geopolymerization reaction, is used as a sealant setting additive. Thus, for example, where a metal silicate is used to promote a geopolymerization reaction, an excess of the metal silicate may be added to provide setting activity for a sealant material. In another example, a metal chloride may have accelerating or retarding effect on a geopolymerization reaction. In such cases, it may be advantageous to introduce thesealant setting additive after the geopolymer hardens so that the additive has no effect on the geopolymerization reaction. In other cases, the sealant setting additive has no effect on the geopolymerization reaction and has activity only when a sealant material is introduced.

[0027] As noted above, the sealant setting additive can be added before or after setting the geopolymer. Such additives are generally solid materials when not dissolved in water. The additives may be added as solids to a blend of dry geopolymer precursor materials include, for example, aluminosilicates and solid activators. Alternately, the additives may be added as liquid materials to a dry or slurry geopolymer precursor. In such cases, the additives may be dissolved and / or dispersed in water or an aqueous medium containing water and optionally other liquids miscible with water.

[0028] A sealant setting additive may be added in any suitable amount to a geopolymer precursor blend. Where the sealant setting additive is added to a dry geopolymer precursor blend, the sealant additive, in solid form, is added in a quantity of 5-30% by weight of the dry precursor blend. Adding more sealant setting additive to the geopolymer precursor blend provides a quicker reaction when a sealant material is introduced to a set geopolymer. Further increasing the amount of sealant setting additive in the dry geopolymer precursor blend risks reducing the general polymerization reactivity of the blend by diluting the reactants. Where the sealant setting additive is added to a slurry geopolymer precursor, the sealant setting additive may be present in the geopolymer precursor at a concentration of 1-5% by weight of the slurry geopolymer precursor.

[0029] The sealant reaction with sealant setting additive may proceed by creating a gel from the sealant material or by precipitating solids. For example, where a silica dispersion in water is used as the sealant, the sealant setting additive may react with the silica of the dispersion to produce a gel, such as a hydrogel, or the sealant setting additive may react with the silica to precipitate solids. It should be noted that in some cases, a silica gel, when exposed to high temperatures in a subterranean formation, may dehydrate to form solids. Any of a suitably shear-stable gel and precipitated solids, or any mixture thereof, can seal flow channels in a set cementitious material.

[0030] In some cases, the sealant setting additive can be added to the hardened geopolymer before adding the sealant material. Thus, for example, a solution or dispersion of a sealant setting salt can be pumped into a hardened geopolymer in a subterranean location to deploy the sealant setting salt before adding a sealant. After adding the sealant setting salt, an aqueous dispersion of sealant material can then be pumped into the hardened geopolymer to react with the previously deployed sealant setting salt to seal flow channels in the geopolymer.

[0031] In some cases, the sealant setting additive can be added to the geopolymer precursor after the precursor is placed at a target location for setting but before the geopolymer precursor has hardened. Thus, a geopolymer precursor can be deployed to a target location, for example by pumping into a subterranean well, and after the geopolymer precursor has arrived at the target location, but before the geopolymer precursor has substantially set, a fluid containing a sealant setting additive is pumped to the target location to contact the geopolymer precursor. When the geopolymer precursor hardens, the resulting geopolymer will contain a sealant setting additive.

[0032] It should be noted that sealant setting additives can be deployed in a set geopolymer in multiple ways. For example, a first sealant setting additive can be blended with the geopolymer precursor before the precursor is deployed to a target location, and a second sealant setting additive can be deployed to the target location after the geopolymer precursor containing the first sealant setting additive is deployed to the target location. In this way, if an amount of sealant setting additive is desired that is more than can be blended into the precursor, the second sealant setting additive can provide additional sealant setting capacity without further burdening the geopolymer precursor composition. The first and second sealant setting additives can be the same compound or different compounds. The first and second sealant setting additives can be deployed to the target location using the same fluid or different fluids.

[0033] In still other cases, a sealant setting additive that is reactive with carbon dioxide can be disposed within a geopolymer by mixing the additive with the geopolymer precursor or by pumping the additive into the hardened geopolymer. Thereafter, carbon dioxide can be introduced into the geopolymer to react with the sealant setting additive to precipitate carbonate solids. The carbon dioxide can beintroduced as gaseous carbon dioxide, or optionally with a small amount of water. Typically, in these cases, most or all of the carbon dioxide, for example at least about 80% of the carbon dioxide, is introduced as gas to avoid substantial pre-dissociation of carbon dioxide as carbonic acid.

[0034] The wells described herein can be wells for hydrocarbon production or for other uses. In some embodiments, the wellbore may be used for carbon capture, utilization, and storage (CCUS) and / or for recovery and use of geothermal energy. Geothermal energy is a promising source of renewable energy that captures energy from heat generated or stored within the earth. For example, geothermal energy may be used to perform climate control (e.g., heating, cooling) for structures (e.g., buildings) using heat pumps and / or to generate electricity (e.g., by heating water to generate steam and drive a turbine with the steam). The wellbores described herein may be used to circulate a working fluid that exchanges heat within the earth formation through which the wellbore extends. The working fluid may be circulated to the surface where a surface heat exchanger is used to transfer thermal energy to another fluid used to generate electricity and / or for climate control. After the thermal energy is transferred from the working fluid in the surface heat exchanger, the working fluid is circulated back to the earth formation to continue the cycle.

[0035] CCUS facilitates the capture, use, and / or storage of carbon (e.g., carbon dioxide), which has a goal of achieving carbon neutrality and / or net zero carbon emissions (NZE). Carbon capture may include the capture of carbon dioxide from large point sources, such as power plants, refineries, cement plants, other industrial processing plants, or other industrial facilities that use fossil fuels, biomass fuels, or other fuels that generate carbon dioxide. The captured carbon dioxide may be converted into valuable products such as, for example, ethanol, sustainable aviation fuel, chemicals, mineral aggregates, and / or other products. Alternatively, the carbon dioxide may be stored in geologic formations, such as in depleted hydrocarbon reservoirs. The carbon dioxide may be introduced into the earth formation through a wellbore, such as the wellbores described herein. In the earth formation, the carbon in the carbon dioxide may be dispersed in an aqueous phase and stored as carbondioxide, may be stored in mineral form (e.g., as a carbonate, such as calcium carbonate, magnesium carbonate, iron(ll) carbonate), or as another form of carbon.

Claims

CLAIMSWe claim:1 . A method of treating a subterranean well, the method comprising: obtaining a sealant that reacts when brought into contact with a sealant setting component of a set cementitious material; pumping the sealant into a subterranean well containing a set geopolymer material that has a sealant setting additive; and reacting the sealant to seal defects of the set geopolymer material.

2. A method, comprising: obtaining a sealant that reacts when brought into contact with a sealant setting component of a set cementitious material; disposing the sealant in contact with a set geopolymer material that has a sealant setting additive; and reacting the sealant to seal defects of the set geopolymer material.

3. A method, comprising: forming a geopolymer that contains a sealant setting additive; obtaining a sealant that reacts when brought into contact with a set cementitious material containing a sealant setting component; disposing the sealant in contact with the geopolymer; and reacting the sealant to seal defects of the geopolymer.

4. The method of any of claims 1 -3, wherein the sealant comprises a nanocrystalline silica.

5. The method of any of claims 1-4, wherein the sealant is brought into contact with the set geopolymer by disposing the sealant inside a casing of the well and pressurizing the sealant through openings in the casing or by disposing the sealant into an annular space between a casing of the well and a wall of the well.

6. The method of any of claims 1 -5, wherein the sealant setting additive is a salt having solubility in water of at least about 0.15 g / mL.

7. The method of any of claims 1 -5, wherein the sealant setting additive is a metal salt having solubility in water of at least about 0.20 g / mL.

8. The method of any of claims 1 -5, wherein the sealant setting additive is a salt of an alkali metal, an alkaline earth metal, or a boron group metal.

9. The method of any of claims 1 -3, further comprising disposing the sealant setting additive in the geopolymer by pumping a fluid containing the sealant setting additive into the geopolymer after the geopolymer is set.

10. The method of claim 9, wherein the sealant setting additive is a metal salt.

11. The method of any of claims 1 -3, wherein the sealant comprises carbon dioxide.

12. The method of any of claims 1 -10, wherein the sealant setting additive is a material that does not participate in a geopolymerization reaction.

13. The method of any of claims 1 to 10, wherein the sealant setting additive comprises aluminum chloride and the sealant comprises silica.

14. The method of any of claims 1 -3, wherein the sealant setting additive is an organic chemical having hydroxyl groups.

15. The method of claim 12, further comprising disposing the sealant setting additive in the geopolymer by adding a fluid containing the sealant setting additive to a geopolymer precursor before the geopolymer is set.

16. The method of any of claims 1-15, wherein the defects of the geopolymer include defects within the geopolymer and defects at the interface of the geopolymer with another material.