Printable Composition for an Ionic Gel Separation Layer for Energy Storage Devices

Abstract

Representative embodiments provide a composition for printing a liquid or gel separator utilized to separate and space apart first and second conductors or electrodes of an energy storage device, such as a battery or a supercapacitor. A representative composition comprises a plurality of particles, typically having a size (in any dimension) between about 0.5 to about 50 microns; a first, ionic liquid electrolyte; and a polymer or polymeric precursor. In another representative embodiment, the plurality of particles comprise diatoms, diatomaceous frustules, and/or diatomaceous fragments or remains. Another representative embodiment further comprises a second electrolyte different from the first electrolyte; the plurality of particles are comprised of silicate glass; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid; and the polymer comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”). Additional components, such as additional electrolytes and solvents, may also be included.

It is claimed: 
     
         1 . A composition comprising:
 a plurality of particles;   a first, ionic liquid electrolyte; and   a polymer or polymeric precursor.   
     
     
         2 . The composition of  claim 1 , wherein the plurality of particles have a size (in any dimension) between about 0.5 to about 30 microns. 
     
     
         3 . The composition of  claim 1 , wherein the plurality of particles have a size (in any dimension) between about 0.5 to about 50 microns. 
     
     
         4 . The composition of  claim 1 , wherein the plurality of particles have a size (in any dimension) between about 5.0 to about 15 microns. 
     
     
         5 . The composition of  claim 1 , wherein the ionic liquid electrolyte comprises one or more ionic liquid cations selected from the group consisting of: ammonium-based, imidazolium-based, piperidinium-based, pyridinium-based, pyrrolidinium-based, phosphonium-based, sulphonium-based, and mixtures thereof. 
     
     
         6 . The composition of  claim 1 , wherein the ionic liquid electrolyte comprises one or more ionic liquid anions selected from the group consisting of: tetrafluoroborate-based, hexafluorophosphate-based, chloride-based, nitrate-based, sulphate-based, acetate-based, (trifluoromethylsulfonyl)imide-based, and mixtures thereof. 
     
     
         7 . The composition of  claim 1 , wherein the ionic liquid electrolyte comprises one or more ionic liquid cations selected from the group consisting of: butyltrimethylammonium, 1-ethyl-3-methylimidazolium, 1-butyl-3-methylimidazolium, 1-methyl-3-propylimidazolium, 1-hexyl-3-methylimidazolium, choline, ethylammonium, tributylmethylphosphonium, tributyl(tetradecyl)phosphonium, trihexyl(tetradecyl)phosphonium, 1-ethyl-2,3-methylimidazolium, 1-butyl-1-methylpiperidinium, diethylmethylsulfonium, 1-methyl-3-propylimidazolium, 1-methyl-1-propylpiperidinium, 1-butyl-2-methylpyridinium, 1-butyl-4-methylpyridinium, 1-butyl-1-methylpyrrolidinium, and mixtures thereof. 
     
     
         8 . The composition of  claim 1 , wherein the ionic liquid electrolyte comprises one or more ionic liquid anions selected from the group consisting of: tris(pentafluoroethyl)trifluorophosphate, trifluoromethanesulfonate, hexafluorophosphate, tetrafluoroborate, ethyl sulfate, methyl sulfate, dimethyl phosphate, trifluoromethanesulfonate, methanesulfonate, triflate, tricyanomethanide, dibutylphosphate, bis(trifluoromethylsulfonyl)imide, bis-2,4,4-(trimethylpentyl)phosphinate, iodide, chloride, bromide, nitrate, thiocyanate, and mixtures thereof. 
     
     
         9 . The composition of  claim 1 , wherein the ionic liquid electrolyte comprises one or more ionic liquid electrolytes or salts selected from the group consisting of: butyltrimethylammonium bis(trifluoromethylsulfonyl)imide; 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide; 1-methyl-3-propylimidazolium bis(trifluoromethylsulfonyl)imide; 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide; choline bis(trifluoromethylsulfonyl)imide; ethylammonium nitrate; tributylmethylphosphonium methylsulfate; 1-ethyl-2,3-methylimidazolium tetrafluoroborate; 1-butyl-1-methylpiperidinium iodide; diethylmethylsulfonium bis(trifluoromethylsulfonyl)imide; 1-methyl-3-propylimidazolium iodide; 1-ethyl-3-methylimidazolium thiocyanate; 1-methyl-1-propylpiperidinium bis(trifluoromethylsulfonyl)imide; 1-butyl-2-methylpyridinium bis(trifluoromethylsulfonyl)imide; 1-butyl-4-methylpyridinium bis(trifluoromethylsulfonyl)imide; 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide; diethylmethylsulfonium bis(trifluoromethylsulfonyl)imide; including salts, such as metallic salts such as lithium, zinc, silver, cadmium and nickel of bis(trifluoromethylsulfonyl)imide, tris(pentafluoroethyl)trifluorophosphate, trifluoromethanesulfonate, hexafluorophosphate, tetrafluoroborate, ethyl sulfate, dimethyl phosphate, trifluoromethanesulfonate, triflate, tricyanomethanide, dibutylphosphate; and mixtures thereof. 
     
     
         10 . The composition of  claim 1 , wherein the polymer or polymeric precursor comprises one or more polymers selected from the group consisting of: polymers (or equivalently, polymeric precursors or polymerizable precurors) such as polyvinyl pyrrolidone (“PVP”, also referred to or known as polyvinyl pyrrolidinone), polyvinyl alcohol (“PVA”), polyvinylidene fluoride (“PVFD”), polyvinylidene fluoride-trifluoroethylene, polytetrafluoroethylene (“PTFE”), polydimethylsiloxane, polyethelene, polypropylene, polyethylene oxide, polypropylene oxide, polyethylene glycolhexafluoropropylene, polyethylene terefphtalatpolyacrylonitryle, polyvinylalcogel, polyvinylpyrrolidone, polyvynilchloride, polyvinyl butyral; polyimide polymers and copolymers (including aliphatic, aromatic and semi-aromatic polyimides) such as polyamide, polyaramides, polyacrylamide; acrylate and (meth)acrylate polymers and copolymers such as polymethylmethacrylate, polyacrylonitrile, acrylonitrile butadiene styrene, allylmethacrylate, polyvinylcaprolactam, polystyrene, polybutadiene, polybutylene terephthalate, polycarbonate, polychloroprene, polyethersulfone, nylon, styrene-acrylonitrile resin; clays such as hectorite clays, garamite clays, organo-modified clays; saccharides and polysaccharides such as guar gum, xanthan gum, starch, butyl rubber, agarose, pectin; celluloses and modified celluloses such as hydroxy methylcellulose, methylcellulose, ethyl cellulose, propyl methylcellulose, methoxy cellulose, methoxy methylcellulose, methoxy propyl methylcellulose, hydroxy propyl methylcellulose, carboxy methylcellulose, hydroxy ethylcellulose, ethyl hydroxylethylcellulose, cellulose ether, cellulose ethyl ether, chitosan; fumed silica (such as Cabosil), silica powders and modified ureas such as BYK® 420 (available from BYK Chemie GmbH); and mixtures thereof. 
     
     
         11 . The composition of  claim 1 , further comprising a second electrolyte different from the first electrolyte. 
     
     
         12 . The composition of  claim 11 , wherein the second electrolyte comprises one or more electrolytes selected from the group consisting of: potassium hydroxide, sodium hydroxide, ammonium hydroxide, lithium hydroxide, nickel hydroxide, cadmium hydroxide, magnesium hydroxide, sulfuric acid, hydrochloric acid, fluoroboric acid, ammonium chloride, zinc chloride, zinc bis(trifluoromethanesulfonyl)imide, aluminium chloride, chromium chloride, magnesium perchloride, barium chromate, lithium chromate, lithium-thyonyl chloride, lithium perchlorate, lithium bromide, lithium triflate, lithium hexafluorophosphate, lithium tetrafluoroborate, lithium bis-oxalato borate, lithium bis(trifluoromethanesulfonyl)imide, lithium bisoxalatoborate, lithium iodide, lithium tetrachloroaluminate, potassium carbonate, potassium fluoride, potassium borate, silver nitride, silver tetrafluoroborate; and mixtures thereof. 
     
     
         13 . The composition of  claim 1 , further comprising a solvent. 
     
     
         14 . The composition of  claim 13 , wherein the solvent comprises one or more solvents selected from the group consisting of: solvents selected from the group consisting of: water; alcohols such as methanol, ethanol, N-propanol (including 1-propanol, 2-propanol (isopropanol or IPA), 1-methoxy-2-propanol), butanol (including 1-butanol, 2-butanol (isobutanol)), pentanol (including 1-pentanol, 2-pentanol, 3-pentanol), hexanol (including 1-hexanol, 2-hexanol, 3-hexanol), octanol, N-octanol (including 1-octanol, 2-octanol, 3-octanol), tetrahydrofurfuryl alcohol (THFA), cyclohexanol, cyclopentanol, terpineol; lactones such as butyl lactone; ethers such as methyl ethyl ether, diethyl ether, ethyl propyl ether, and polyethers; ketones, including diketones and cyclic ketones, such as cyclohexanone, cyclopentanone, cycloheptanone, cyclooctanone, acetone, benzophenone, acetylacetone, acetophenone, cyclopropanone, isophorone, methyl ethyl ketone; esters such ethyl acetate, dimethyl adipate, propylene glycol monomethyl ether acetate, dimethyl glutarate, dimethyl succinate, glycerin acetate, carboxylates; glycols such as ethylene glycols, diethylene glycols, polyethylene glycols, propylene glycols, dipropylene glycols, glycol ethers, glycol ether acetates; carbonates such as propylene carbonate; glycerols and other polyols and polymeric polyols or glycols such as glycerin, diol, triol, tetraol, pentaol, ethylene glycol, 1,4-butanediol, 1,2-butanediol, 2,3-butanediol, 1,3-propanediol, 1,4-butanediol, 1,5-pentanediol, 1,8-octanediol, 1,2-propanediol, 1,3-butanediol, 1,2-pentanediol, etohexadiol, p-menthane-3,8-diol, 2-methyl-2,4-pentanediol; tetramethyl urea, n-methylpyrrolidone, acetonitrile, tetrahydrofuran (THF), dimethyl formamide (DMF), N-methyl formamide (NMF), dimethyl sulfoxide (DMSO), thionyl chloride; sulfuryl chloride; and mixtures thereof. 
     
     
         15 . The composition of  claim 1 , wherein the plurality of particles comprise one or more particles selected from the group consisting of: silicate glass, silicon dioxide, alumina, polystyrene, melamine, and mixtures thereof. 
     
     
         16 . The composition of  claim 1 , wherein the plurality of particles comprise diatoms, diatomaceous frustules, diatomaceous fragments, diatomaceous remains, and mixtures thereof. 
     
     
         17 . A method of using the composition of  claim 1 , the method comprising:
 printing the composition to form a liquid or gel separator.   
     
     
         18 . The composition of  claim 1 , wherein the plurality of particles comprise one or more particles selected from the group consisting of: polymers (or equivalently, polymeric precursors or polymerizable precurors) such as polyvinyl pyrrolidone (“PVP”, also referred to or known as polyvinyl pyrrolidinone), polyvinyl alcohol (“PVA”), polyvinylidene fluoride (“PVFD”), polyvinylidene fluoride-trifluoroethylene, polytetrafluoroethylene (“PTFE”), polydimethylsiloxane, polyethelene, polypropylene, polyethylene oxide, polypropylene oxide, polyethylene glycolhexafluoropropylene, polyethylene terefphtalatpolyacrylonitryle, polyvinylalcogel, polyvinylpyrrolidone, polyvynilchloride, polyvinyl butyral; polyimide polymers and copolymers (including aliphatic, aromatic and semi-aromatic polyimides) such as polyamide, polyaramides, polyacrylamide; acrylate and (meth)acrylate polymers and copolymers such as polymethylmethacrylate, polyacrylonitrile, acrylonitrile butadiene styrene, allylmethacrylate, polyvinylcaprolactam, polystyrene, polybutadiene, polybutylene terephthalate, polycarbonate, polychloroprene, polyethersulfone, nylon, styrene-acrylonitrile resin; clays such as hectorite clays, garamite clays, organo-modified clays; saccharides and polysaccharides such as guar gum, xanthan gum, starch, butyl rubber, agarose, pectin; celluloses and modified celluloses such as hydroxy methylcellulose, methylcellulose, ethyl cellulose, propyl methylcellulose, methoxy cellulose, methoxy methylcellulose, methoxy propyl methylcellulose, hydroxy propyl methylcellulose, carboxy methylcellulose, hydroxy ethylcellulose, ethyl hydroxylethylcellulose, cellulose ether, cellulose ethyl ether, chitosan; fumed silica, silica powders, modified ureas; and mixtures thereof. 
     
     
         19 . The composition of  claim 1 , wherein the plurality of particles have a size (in any dimension) between about 0.5 to about 30 microns and are present in an amount between about 10%-90% by weight; the ionic liquid electrolyte is present in an amount between about 10%-90% by weight; and the polymer or polymeric precursor is present in an amount between about 0.5%-90% by weight. 
     
     
         20 . The composition of  claim 1 , wherein the plurality of particles have a size (in any dimension) between about 0.5 to about 30 microns and are present in an amount between about 30%-80% by weight; the ionic liquid electrolyte is present in an amount between about 5%-50% by weight; and the polymer or polymeric precursor is present in an amount between about 1.0%-20% by weight. 
     
     
         21 . The composition of  claim 1 , wherein the plurality of particles have a size (in any dimension) between about 0.5 to about 30 microns and are present in an amount between about 40%-60% by weight; the ionic liquid electrolyte is present in an amount between about 15%-30% by weight; and the polymer or polymeric precursor is present in an amount between about 1.0%-10% by weight. 
     
     
         22 . The composition of  claim 1 , further comprising a second electrolyte different from the first electrolyte; and wherein the plurality of particles have a size (in any dimension) between about 5.0 to about 15 microns and are comprised of silicate glass; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid; and the polymer or polymeric precursor comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof. 
     
     
         23 . The composition of  claim 1 , further comprising a second electrolyte different from the first electrolyte; and wherein the plurality of particles have a size (in any dimension) between about 5.0 to about 15 microns, are comprised of silicate glass, and are present in an amount between about 40%-75% by weight; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid and are present in an amount between about 15%-45% by weight; and the polymer or polymeric precursor comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof and present in an amount between about 0.5%-15% by weight. 
     
     
         24 . The composition of  claim 1 , further comprising a second electrolyte different from the first electrolyte and further comprising a solvent comprising N-methyl-2-pyrrolidinone; and wherein the plurality of particles have a size (in any dimension) between about 5.0 to about 15 microns and are comprised of silicate glass; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid; and the polymer or polymeric precursor comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof. 
     
     
         25 . The composition of  claim 1 , further comprising a second electrolyte different from the first electrolyte and further comprising a solvent comprising N-methyl-2-pyrrolidinone present in an amount between about 15%-25% by weight; and wherein the plurality of particles have a size (in any dimension) between about 5.0 to about 15 microns, are comprised of silicate glass, and are present in an amount between about 40%-75% by weight; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid and are present in an amount between about 15%-45% by weight; and the polymer or polymeric precursor comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof and present in an amount between about 0.5%-15% by weight. 
     
     
         26 . A composition comprising:
 a plurality of particles having a size (in any dimension) between about 0.5 to about 30 microns, wherein the plurality of particles comprise one or more particles selected from the group consisting of: silicate glass, silicon dioxide, alumina, polystyrene, melamine, diatoms, diatomaceous frustules, diatomaceous fragments, diatomaceous remains, and mixtures thereof;   a first, ionic liquid electrolyte; and   a polymer or polymeric precursor.   
     
     
         27 . The composition of  claim 26 , wherein the ionic liquid electrolyte comprises one or more ionic liquid cations selected from the group consisting of: butyltrimethylammonium, 1-ethyl-3-methylimidazolium, 1-butyl-3-methylimidazolium, 1-methyl-3-propylimidazolium, 1-hexyl-3-methylimidazolium, choline, ethylammonium, tributylmethylphosphonium, tributyl(tetradecyl)phosphonium, trihexyl(tetradecyl)phosphonium, 1-ethyl-2,3-methylimidazolium, 1-butyl-1-methylpiperidinium, diethylmethylsulfonium, 1-methyl-3-propylimidazolium, 1-methyl-1-propylpiperidinium, 1-butyl-2-methylpyridinium, 1-butyl-4-methylpyridinium, 1-butyl-1-methylpyrrolidinium, and mixtures thereof. 
     
     
         28 . The composition of  claim 26 , wherein the ionic liquid electrolyte comprises one or more ionic liquid anions selected from the group consisting of: tris(pentafluoroethyl)trifluorophosphate, trifluoromethanesulfonate, hexafluorophosphate, tetrafluoroborate, ethyl sulfate, methyl sulfate, dimethyl phosphate, trifluoromethanesulfonate, methanesulfonate, triflate, tricyanomethanide, dibutylphosphate, bis(trifluoromethylsulfonyl)imide, bis-2,4,4-(trimethylpentyl)phosphinate, iodide, chloride, bromide, nitrate, thiocyanate, and mixtures thereof. 
     
     
         29 . The composition of  claim 26 , wherein the ionic liquid electrolyte comprises one or more ionic liquid electrolytes or salts selected from the group consisting of: butyltrimethylammonium bis(trifluoromethylsulfonyl)imide; 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide; 1-methyl-3-propylimidazolium bis(trifluoromethylsulfonyl)imide; 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide; choline bis(trifluoromethylsulfonyl)imide; ethylammonium nitrate; tributylmethylphosphonium methylsulfate; 1-ethyl-2,3-methylimidazolium tetrafluoroborate; 1-butyl-1-methylpiperidinium iodide; diethylmethylsulfonium bis(trifluoromethylsulfonyl)imide; 1-methyl-3-propylimidazolium iodide; 1-ethyl-3-methylimidazolium thiocyanate; 1-methyl-1-propylpiperidinium bis(trifluoromethylsulfonyl)imide; 1-butyl-2-methylpyridinium bis(trifluoromethylsulfonyl)imide; 1-butyl-4-methylpyridinium bis(trifluoromethylsulfonyl)imide; 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide; diethylmethylsulfonium bis(trifluoromethylsulfonyl)imide; including salts, such as metallic salts such as lithium, zinc, silver, cadmium and nickel of bis(trifluoromethylsulfonyl)imide, tris(pentafluoroethyl)trifluorophosphate, trifluoromethanesulfonate, hexafluorophosphate, tetrafluoroborate, ethyl sulfate, dimethyl phosphate, trifluoromethanesulfonate, triflate, tricyanomethanide, dibutylphosphate; and mixtures thereof. 
     
     
         30 . The composition of  claim 26 , wherein the polymer or polymeric precursor comprises one or more polymers selected from the group consisting of: polymers (or equivalently, polymeric precursors or polymerizable precurors) such as polyvinyl pyrrolidone (“PVP”, also referred to or known as polyvinyl pyrrolidinone), polyvinyl alcohol (“PVA”), polyvinylidene fluoride (“PVFD”), polyvinylidene fluoride-trifluoroethylene, polytetrafluoroethylene (“PTFE”), polydimethylsiloxane, polyethelene, polypropylene, polyethylene oxide, polypropylene oxide, polyethylene glycolhexafluoropropylene, polyethylene terefphtalatpolyacrylonitryle, polyvinylalcogel, polyvinylpyrrolidone, polyvynilchloride, polyvinyl butyral; polyimide polymers and copolymers (including aliphatic, aromatic and semi-aromatic polyimides) such as polyamide, polyaramides, polyacrylamide; acrylate and (meth)acrylate polymers and copolymers such as polymethylmethacrylate, polyacrylonitrile, acrylonitrile butadiene styrene, allylmethacrylate, polyvinylcaprolactam, polystyrene, polybutadiene, polybutylene terephthalate, polycarbonate, polychloroprene, polyethersulfone, nylon, styrene-acrylonitrile resin; clays such as hectorite clays, garamite clays, organo-modified clays; saccharides and polysaccharides such as guar gum, xanthan gum, starch, butyl rubber, agarose, pectin; celluloses and modified celluloses such as hydroxy methylcellulose, methylcellulose, ethyl cellulose, propyl methylcellulose, methoxy cellulose, methoxy methylcellulose, methoxy propyl methylcellulose, hydroxy propyl methylcellulose, carboxy methylcellulose, hydroxy ethylcellulose, ethyl hydroxylethylcellulose, cellulose ether, cellulose ethyl ether, chitosan; fumed silica (such as Cabosil), silica powders and modified ureas such as BYK® 420 (available from BYK Chemie GmbH); and mixtures thereof. 
     
     
         31 . The composition of  claim 26 , further comprising a second electrolyte different from the first electrolyte. 
     
     
         32 . The composition of  claim 31 , wherein the second electrolyte comprises one or more electrolytes selected from the group consisting of: potassium hydroxide, sodium hydroxide, ammonium hydroxide, lithium hydroxide, nickel hydroxide, cadmium hydroxide, magnesium hydroxide, sulfuric acid, hydrochloric acid, fluoroboric acid, ammonium chloride, zinc chloride, zinc bis(trifluoromethanesulfonyl)imide, aluminium chloride, chromium chloride, magnesium perchloride, barium chromate, lithium chromate, lithium-thyonyl chloride, lithium perchlorate, lithium bromide, lithium triflate, lithium hexafluorophosphate, lithium tetrafluoroborate, lithium bis-oxalato borate, lithium bis(trifluoromethanesulfonyl)imide, lithium bisoxalatoborate, lithium iodide, lithium tetrachloroaluminate, potassium carbonate, potassium fluoride, potassium borate, silver nitride, silver tetrafluoroborate; and mixtures thereof. 
     
     
         33 . The composition of  claim 26 , wherein the plurality of particles are present in an amount between about 10%-90% by weight; the ionic liquid electrolyte is present in an amount between about 10%-90% by weight; and the polymer or polymeric precursor is present in an amount between about 0.5%-90% by weight. 
     
     
         34 . The composition of  claim 26 , wherein the plurality of particles are present in an amount between about 30%-80% by weight; the ionic liquid electrolyte is present in an amount between about 5%-50% by weight; and the polymer or polymeric precursor is present in an amount between about 1.0%-20% by weight. 
     
     
         35 . The composition of  claim 26 , wherein the plurality of particles are present in an amount between about 40%-60% by weight; the ionic liquid electrolyte is present in an amount between about 15%-30% by weight; and the polymer or polymeric precursor is present in an amount between about 1.0%-10% by weight. 
     
     
         36 . The composition of  claim 26 , further comprising a second electrolyte different from the first electrolyte and further comprising a solvent comprising N-methyl-2-pyrrolidinone; and wherein the plurality of particles are comprised of silicate glass; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid; and the polymer or polymeric precursor comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof. 
     
     
         37 . The composition of  claim 26 , further comprising a second electrolyte different from the first electrolyte and further comprising a solvent comprising N-methyl-2-pyrrolidinone present in an amount between about 15%-25% by weight; and wherein the plurality of particles are comprised of silicate glass, and are present in an amount between about 40%-75% by weight; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid and are present in an amount between about 15%-45% by weight; and the polymer or polymeric precursor comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof and present in an amount between about 0.5%-15% by weight. 
     
     
         38 . A composition comprising:
 a plurality of particles;   a first, ionic liquid electrolyte;   a second electrolyte different from the first electrolyte; and   a polymer or polymeric precursor.   
     
     
         39 . The composition of  claim 38 , wherein the plurality of particles have a size (in any dimension) between about 5.0 to about 15 microns. 
     
     
         40 . The composition of  claim 38 , wherein the ionic liquid electrolyte comprises one or more ionic liquid cations selected from the group consisting of: butyltrimethylammonium, 1-ethyl-3-methylimidazolium, 1-butyl-3-methylimidazolium, 1-methyl-3-propylimidazolium, 1-hexyl-3-methylimidazolium, choline, ethylammonium, tributylmethylphosphonium, tributyl(tetradecyl)phosphonium, trihexyl(tetradecyl)phosphonium, 1-ethyl-2,3-methylimidazolium, 1-butyl-1-methylpiperidinium, diethylmethylsulfonium, 1-methyl-3-propylimidazolium, 1-methyl-1-propylpiperidinium, 1-butyl-2-methylpyridinium, 1-butyl-4-methylpyridinium, 1-butyl-1-methylpyrrolidinium, and mixtures thereof. 
     
     
         41 . The composition of  claim 38 , wherein the ionic liquid electrolyte comprises one or more ionic liquid anions selected from the group consisting of: tris(pentafluoroethyl)trifluorophosphate, trifluoromethanesulfonate, hexafluorophosphate, tetrafluoroborate, ethyl sulfate, methyl sulfate, dimethyl phosphate, trifluoromethanesulfonate, methanesulfonate, triflate, tricyanomethanide, dibutylphosphate, bis(trifluoromethylsulfonyl)imide, bis-2,4,4-(trimethylpentyl)phosphinate, iodide, chloride, bromide, nitrate, thiocyanate, and mixtures thereof. 
     
     
         42 . The composition of  claim 38 , wherein the ionic liquid electrolyte comprises one or more ionic liquid electrolytes or salts selected from the group consisting of: butyltrimethylammonium bis(trifluoromethylsulfonyl)imide; 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide; 1-methyl-3-propylimidazolium bis(trifluoromethylsulfonyl)imide; 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide; choline bis(trifluoromethylsulfonyl)imide; ethylammonium nitrate; tributylmethylphosphonium methylsulfate; 1-ethyl-2,3-methylimidazolium tetrafluoroborate; 1-butyl-1-methylpiperidinium iodide; diethylmethylsulfonium bis(trifluoromethylsulfonyl)imide; 1-methyl-3-propylimidazolium iodide; 1-ethyl-3-methylimidazolium thiocyanate; 1-methyl-1-propylpiperidinium bis(trifluoromethylsulfonyl)imide; 1-butyl-2-methylpyridinium bis(trifluoromethylsulfonyl)imide; 1-butyl-4-methylpyridinium bis(trifluoromethylsulfonyl)imide; 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide; diethylmethylsulfonium bis(trifluoromethylsulfonyl)imide; including salts, such as metallic salts such as lithium, zinc, silver, cadmium and nickel of bis(trifluoromethylsulfonyl)imide, tris(pentafluoroethyl)trifluorophosphate, trifluoromethanesulfonate, hexafluorophosphate, tetrafluoroborate, ethyl sulfate, dimethyl phosphate, trifluoromethanesulfonate, triflate, tricyanomethanide, dibutylphosphate; and mixtures thereof. 
     
     
         43 . The composition of  claim 38 , wherein the polymer or polymeric precursor comprises one or more polymers selected from the group consisting of: polymers (or equivalently, polymeric precursors or polymerizable precurors) such as polyvinyl pyrrolidone (“PVP”, also referred to or known as polyvinyl pyrrolidinone), polyvinyl alcohol (“PVA”), polyvinylidene fluoride (“PVFD”), polyvinylidene fluoride-trifluoroethylene, polytetrafluoroethylene (“PTFE”), polydimethylsiloxane, polyethelene, polypropylene, polyethylene oxide, polypropylene oxide, polyethylene glycolhexafluoropropylene, polyethylene terefphtalatpolyacrylonitryle, polyvinylalcogel, polyvinylpyrrolidone, polyvynilchloride, polyvinyl butyral; polyimide polymers and copolymers (including aliphatic, aromatic and semi-aromatic polyimides) such as polyamide, polyaramides, polyacrylamide; acrylate and (meth)acrylate polymers and copolymers such as polymethylmethacrylate, polyacrylonitrile, acrylonitrile butadiene styrene, allylmethacrylate, polyvinylcaprolactam, polystyrene, polybutadiene, polybutylene terephthalate, polycarbonate, polychloroprene, polyethersulfone, nylon, styrene-acrylonitrile resin; clays such as hectorite clays, garamite clays, organo-modified clays; saccharides and polysaccharides such as guar gum, xanthan gum, starch, butyl rubber, agarose, pectin; celluloses and modified celluloses such as hydroxy methylcellulose, methylcellulose, ethyl cellulose, propyl methylcellulose, methoxy cellulose, methoxy methylcellulose, methoxy propyl methylcellulose, hydroxy propyl methylcellulose, carboxy methylcellulose, hydroxy ethylcellulose, ethyl hydroxylethylcellulose, cellulose ether, cellulose ethyl ether, chitosan; fumed silica (such as Cabosil), silica powders and modified ureas such as BYK® 420 (available from BYK Chemie GmbH); and mixtures thereof. 
     
     
         44 . The composition of  claim 38 , wherein the second electrolyte comprises one or more electrolytes selected from the group consisting of: potassium hydroxide, sodium hydroxide, ammonium hydroxide, lithium hydroxide, nickel hydroxide, cadmium hydroxide, magnesium hydroxide, sulfuric acid, hydrochloric acid, fluoroboric acid, ammonium chloride, zinc chloride, zinc bis(trifluoromethanesulfonyl)imide, aluminium chloride, chromium chloride, magnesium perchloride, barium chromate, lithium chromate, lithium-thyonyl chloride, lithium perchlorate, lithium bromide, lithium triflate, lithium hexafluorophosphate, lithium tetrafluoroborate, lithium bis-oxalato borate, lithium bis(trifluoromethanesulfonyl)imide, lithium bisoxalatoborate, lithium iodide, lithium tetrachloroaluminate, potassium carbonate, potassium fluoride, potassium borate, silver nitride, silver tetrafluoroborate; and mixtures thereof. 
     
     
         45 . The composition of  claim 38 , wherein the plurality of particles comprise one or more particles selected from the group consisting of: silicate glass, silicon dioxide glass, alumina, polystyrene, melamine, diatoms, diatomaceous frustules, and/or diatomaceous fragments or remains; and mixtures thereof. 
     
     
         46 . The composition of  claim 38 , wherein the plurality of particles have a size (in any dimension) between about 0.5 to about 30 microns and are present in an amount between about 30%-80% by weight; the first and second electrolytes are present in an amount between about 5%-50% by weight; and the polymer or polymeric precursor is present in an amount between about 1.0%-20% by weight. 
     
     
         47 . The composition of  claim 38 , wherein the plurality of particles have a size (in any dimension) between about 0.5 to about 30 microns and are present in an amount between about 40%-60% by weight; the first and second electrolytes are present in an amount between about 15%-30% by weight; and the polymer or polymeric precursor is present in an amount between about 1.0%-10% by weight. 
     
     
         48 . The composition of  claim 38 , further comprising a solvent comprising N-methyl-2-pyrrolidinone; and wherein the plurality of particles have a size (in any dimension) between about 5.0 to about 15 microns and are comprised of silicate glass; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid; and the polymer or polymeric precursor comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof. 
     
     
         49 . The composition of  claim 38 , further comprising a solvent comprising N-methyl-2-pyrrolidinone present in an amount between about 15%-25% by weight; and wherein the plurality of particles have a size (in any dimension) between about 5.0 to about 15 microns, are comprised of silicate glass, and are present in an amount between about 40%-75% by weight; the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid and are present in an amount between about 15%-45% by weight; and the polymer or polymeric precursor comprises polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof and present in an amount between about 0.5%-15% by weight. 
     
     
         50 . A composition comprising:
 a plurality of particles having a size (in any dimension) between about 3.0 to about 15 microns and present in an amount between about 40%-75% by weight, wherein the plurality of particles comprise one or more particles selected from the group consisting of: silicate glass, silicon dioxide, alumina, polystyrene, melamine, diatoms, diatomaceous frustules, diatomaceous fragments; and mixtures thereof;   a first, ionic liquid electrolyte;   a second electrolyte different from the first electrolyte, wherein the first and second electrolytes comprise zinc tetrafluoroborate salt in 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid and are present in an amount between about 15%-45% by weight;   a polymer or polymeric precursor comprising polyvinyl alcohol (“PVA”) or polyvinylidene fluoride (“PVFD”) or mixtures thereof and present in an amount between about 0.5%-15% by weight;   and a solvent comprising N-methyl-2-pyrrolidinone present in an amount between about 15%-25% by weight.