Hydrogen storage materials and methods including hydrides and hydroxides
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
C01B-003/02
C01B-003/00
C01B-006/00
C01B-006/02
C01B-006/04
C01B-006/06
C01B-006/26
출원번호
UP-0787292
(2004-02-26)
등록번호
US-7521036
(2009-07-01)
발명자
/ 주소
Vajo, John J
Mertens, Florian O
Jorgensen, Scott W
출원인 / 주소
General Motors Corporation
인용정보
피인용 횟수 :
1인용 특허 :
15
초록▼
In one aspect, the invention provides a hydrogen storage composition having a hydrogenated state and a dehydrogenated state. In the hydrogenated state, such composition comprises a hydride and a hydroxide. In a dehydrogenated state, the composition comprises an oxide. The present invention also pro
In one aspect, the invention provides a hydrogen storage composition having a hydrogenated state and a dehydrogenated state. In the hydrogenated state, such composition comprises a hydride and a hydroxide. In a dehydrogenated state, the composition comprises an oxide. The present invention also provides methods of producing hydrogen, including for mobile fuel cell device applications.
대표청구항▼
What is claimed is: 1. A method of producing hydrogen comprising: conducting a reaction between a hydride composition and a dehydrated hydroxide composition to form hydrogen and an oxide composition, wherein said hydroxide composition is represented by the formula: MIIy(OH)y, where MII represents o
What is claimed is: 1. A method of producing hydrogen comprising: conducting a reaction between a hydride composition and a dehydrated hydroxide composition to form hydrogen and an oxide composition, wherein said hydroxide composition is represented by the formula: MIIy(OH)y, where MII represents one or more cationic species other than hydrogen and is selected from the group consisting of Al, As, Ba, Be, Ca, Cd, Ce, Cs, Cu, Eu, Fe, Ga, Gd, Ge, Hf, Hg, In, La, Li, Mg, Mn, Na, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Si, Sm, Sn, Sr, Th, Ti, Tl, V, W, Y, Yb, Zn, Zr, and mixtures thereof and y represents an average valence state of MII. 2. The method according to claim 1 wherein said hydride composition has one or more cationic species other than hydrogen. 3. The method according to claim 2 wherein said oxide composition comprises at least one of said one or more cations other than hydrogen derived from either of said hydride or said hydroxide compositions, respectively. 4. The method according to claim 1 wherein said hydride composition is represented by the formula: MIxHx, where MI represents said one or more cationic species other than hydrogen and x represents an average valence state of MI. 5. The method of claim 1 wherein said hydride composition is represented by MIxHx, where MI represents one or more cationic species other than hydrogen, and x represents an average valence state of MI. 6. The method of claim 5 wherein MI and MII are different cationic species. 7. The method claim 5 wherein MI and MII are the same cationic species. 8. The method of claim 5 wherein MI is a complex cationic species comprising two distinct cationic species. 9. The method of claim 5 wherein MII is a complex cationic species comprising two distinct cationic species. 10. of claim 5 wherein MI is selected from the group consisting of Al, As, B, Ba, Be, Ca, Cd, Ce, Cs, Cu, Eu, Fe, Ga, Gd, Ge, Hf, Hg, In, K, La, Li, Mg, Mn, Na, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Si, Sm, Sn, Sr, Th, Ti, Tl, V, W, Y, Yb, Zn, Zr, and mixtures thereof. 11. The method of claim 5 wherein MI and MII are each elements independently selected from the group consisting of Al, Ba, Be, Ca, Cs, Li, Mg, Na, Rb, Si, Sr, Ti, V and mixtures thereof. 12. The method of claim 11 wherein MI and MII are each elements independently selected from the group consisting of Al, Be, Ca, Li, Mg, Na, Sr, Ti, and mixtures thereof. 13. The method according to claim 1 wherein said hydride composition is selected from the group consisting of: lithium hydride (LiH), sodium hydride (NaH), potassium hydride (KH), beryllium hydride (BeH2), magnesium hydride (MgH2), calcium hydride (CaH2), strontium hydride (SrH2), titanium hydride (TiH2), aluminum hydride (AlH3), boron hydride (BH3), lithium borohydride (LiBH4), sodium borohydride (NaBH4), magnesium borohydride (Mg(BH4)2), calcium borohydride (Ca(BH4)2), lithium alanate (LiAlH4), sodium alanate (NaAlH4), magnesium alanate (Mg(AlH4)2), calcium alanate (Ca(AlH4)2), and mixtures thereof. 14. The method according to claim 1 wherein said hydroxide composition is selected from the group consisting of: lithium hydroxide (LiOH), sodium hydroxide (NaOH), beryllium hydroxide (Be(OH)2), magnesium hydroxide (Mg(OH)2), calcium hydroxide (Ca(OH)2), strontium hydroxide (Sr(OH)2), titanium hydroxide (Ti(OH)2), aluminum hydroxide (Al(OH)3), and mixtures thereof. 15. The method according to claim 1 wherein said hydride composition comprises LiH and said hydroxide composition comprises LiOH. 16. The method according to claim 15 wherein said reaction proceeds according to a reaction mechanism of LiH+LiOH→Li2O+H2. 17. The method according to claim 1 wherein said hydride composition comprises NaH and said hydroxide composition comprises LiOH. 18. The method according to claim 17 wherein said reaction proceeds according to a reaction mechanism of NaH+LiOH→½ Li2O+½ Na2O+H2. 19. The method according to claim 1 wherein said hydride composition comprises MgH2 and said hydroxide composition comprises Mg(OH)2. 20. The method according to claim 19 wherein said reaction proceeds according to a reaction mechanism of MgH2+Mg(OH)2→MgO+2 H2. 21. The method according to claim 1 wherein said hydride composition comprises AlH3 and said hydroxide composition comprises Al(OH)3. 22. The method according to claim 21 wherein said reaction proceeds according to a reaction mechanism of AlH3+Al(OH)3→Al2O3+3H2 . 23. The method according to claim 1 wherein said hydride composition comprises CaH2 and said hydroxide composition comprises Ca(OH)2. 24. The method according to claim 23 wherein said reaction proceeds according to a reaction mechanism of CaH2+Ca(OH)2→CaO+2 H2. 25. The method according to claim 1 wherein said hydride composition comprises SrH2 and said hydroxide composition comprises Sr(OH)2. 26. The method according to claim 25 wherein said reaction proceeds according to a reaction mechanism of SrH2+Sr(OH)2→SrO+2 H2. 27. The method according to claim 1 wherein said hydride composition comprises BeH2 and said hydroxide composition comprises Be(OH)2. 28. The method according to claim 27 wherein said reaction proceeds according to a reaction mechanism of BeH2+Be(OH)2→BeO+2 H2. 29. The method according to claim 1 where said hydride composition comprises LiBH4 and said hydroxide composition comprises LiOH. 30. The method according to claim 29 where said reaction proceeds according to a reaction mechanism of LiBH4+4LiOH→LiBO2+2Li2O+4H2 . 31. The method according to claim 1 where said hydride composition comprises NaBH4 and said hydroxide composition comprises Mg(OH)2. 32. The method according to claim 31 where said reaction proceeds according to a reaction mechanism of NaBH4+2 Mg(OH)2→NaBO2+2MgO+4H2. 33. The method according to claim 1 where said hydride composition comprises NaBH4 and said hydroxide composition comprises NaOH. 34. The method according to claim 33 where said reaction proceeds according to a reaction mechanism of NaBH4+4NaOH→NaBO2+2Na2O+4H2 . 35. The method according to claim 1 wherein said reaction is reversible to form a species of said hydride composition or said hydroxide composition. 36. The method according to claim 35 wherein said reversible reaction is conducted by exposing said oxide composition to hydrogen to form said species. 37. The method according to claim 36 wherein said reversible reaction regenerates said hydride composition and said hydroxide composition. 38. The method according to claim 1 wherein said reaction is conducted at an elevated temperature relative to ambient conditions. 39. The method according to claim 38 wherein said reaction is conducted at a temperature 40° C. or greater. 40. The method according to claim 1 wherein said hydride composition and said hydroxide composition are in particle form and said reaction is a solid-state reaction. 41. The method according to claim 40 wherein said hydride composition and said hydroxide composition are reduced in particle size prior to said reaction. 42. The method according to claim 1 wherein before conducting said reaction, said hydride composition and said hydroxide composition are essentially homogeneously mixed together. 43. The method according to claim 1 wherein during said reaction, said oxide composition, said hydrogen, or both, are removed from said hydride composition and said hydroxide composition, as said reaction proceeds. 44. The method according to claim 1 wherein during said reaction said hydrogen is removed as said reaction proceeds. 45. The method according to claim 1 wherein said reaction is conducted in the presence of a catalyst in contact with said hydride composition and said hydroxide composition. 46. The method according to claim 45 wherein said catalyst comprises a compound comprising an element selected from the group consisting of Ti, V, Cr, C, Fe, Mn, Ni, Nb, Pd, Si, Al, and mixtures thereof. 47. A method for releasing hydrogen from hydrogen storage materials comprising: mixing a first hydrogen storage material with a second hydrogen storage material, where said first hydrogen storage material comprises a hydride composition represented by MIxHx and said second hydrogen storage material comprises a dehydrated hydroxide composition represented by MIIy(OH)y, where MI and MII each represent a cationic species or a mixture of cationic species other than hydrogen, where MII is selected from the group consisting of Al, As, Ba, Be, Ca, Cd, Ce, Cs, Cu, Eu, Fe, Ga, Gd, Ge, Hf, Hg, In, La, Li, Mg, Mn, Na, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Si, Sm, Sn, Sr, Th, Ti, Tl, V, W, Y, Yb, Zn, Zr, and mixtures thereof, and where x and y represent average valence states of respectively MI and MII; and conducting a reaction between said first storage material with said second storage material for a time and at a temperature sufficient to produce a reaction product comprising an oxide material and hydrogen. 48. The method of claim 47 wherein MI and MII are different cationic species. 49. The method of claim 47 wherein MI and MII are the same cationic species. 50. The method of claim 47 wherein MI is a complex cationic species comprising two distinct cationic species. 51. The method of claim 47 wherein MII is a complex cationic species comprising two distinct cationic species. 52. The method of claim 47 wherein MII is selected from the group consisting of OH3, C2H5, C3H7, Al, As, Ba, Be, Ca, Cd, Ce, Cs, Cu, Eu, Fe, Ga, Gd, Ge, Hf, Hg, In, La, Li, Mg, Mn, Na, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Si, Sm, Sn, Sr, Th, Ti, Tl, V, W, Y, Yb, Zn, Zr, and mixtures thereof. 53. The method of claim 52 wherein MI and MII are each elements independently selected from the group consisting of Al, Ba, Be, Ca, Cs, Li, Mg, Na, Rb, Si, Sr, Ti, V and mixtures thereof. 54. The method of claim 53 wherein MI and MII are each elements independently selected from the group consisting of Al, Be, Ca, Li, Mg, Na, Sr, Ti, and mixtures thereof. 55. The method according to claim 47 wherein said hydride composition is selected from the group consisting of: lithium hydride (LiH), sodium hydride (NaH), potassium hydride (KH), beryllium hydride (BeH2), magnesium hydride (MgH2), calcium hydride (CaH2), strontium hydride (SrH2), titanium hydride (TiH2), aluminum hydride (AlH3), boron hydride (BH3), lithium borohydride (LiBH4), sodium borohydride (NaBH4), magnesium borohydride (Mg(BH4)2), calcium borohydride (Ca(BH4)2), lithium alanate (LiAlH4), sodium alanate (NaAlH4), magnesium alanate (Mg(AlH4)2), calcium alanate (Ca(AlH4)2), and mixtures thereof. 56. The method according to claim 47 wherein said hydroxide composition is selected from the group consisting of: lithium hydroxide (LiOH), sodium hydroxide (NaOH), beryllium hydroxide (Be(OH)2), magnesium hydroxide (Mg(OH)2), calcium hydroxide (Ca(OH)2), strontium hydroxide (Sr(OH)2), titanium hydroxide (Ti(OH)2), aluminum hydroxide (Al(OH)3), and mixtures thereof. 57. The method according to claim 47 wherein said hydride composition comprises LiH and said hydroxide composition comprises LiOH. 58. The method according to claim 57 wherein said reaction proceeds according to a reaction mechanism of LiH+LiOH→Li2O+H2. 59. The method according to claim 47 wherein said hydride composition comprises NaH and said hydroxide composition comprises LiOH. 60. The method according to claim 59 wherein said reaction proceeds according to a reaction mechanism of NaH+LiOH→½ Li2O+½ Na2O+H2. 61. The method according to claim 47 wherein said reaction is reversed by exposing said oxide material to hydrogen to form a regenerated first storage material comprising a hydride and a regenerated second storage material comprising a hydroxide. 62. The method according to claim 61 wherein said hydride of said regenerated first storage material and said hydroxide of said regenerated second storage material are the same species as said first and said second starting materials, comprising said hydride and said hydroxide, respectively. 63. The method according to claim 47 wherein said reaction is conducted at an elevated temperature relative to ambient conditions. 64. The method according to claim 63 wherein said reaction is conducted at a temperature of 40° C. or greater. 65. The method according to claim 47 wherein said first starting material and said second starting material are in particle form and said reaction is a solid state reaction. 66. The method according to claim 65 wherein said first starting material and said second starting material are reduced in particle size prior to said reaction. 67. The method according to claim 47 wherein before conducting said reaction, said first starting material and said second starting material are essentially homogeneously mixed together. 68. The method according to claim 47 wherein during said reaction, said oxide, said hydrogen, or both, are removed from said first starting material and said second starting material, as said reaction proceeds. 69. The method according to claim 47 wherein during said reaction said hydrogen is a removed from said first and said second starting materials as said reaction proceeds. 70. The method according to claim 47 wherein said reaction is conducted in the presence of a catalyst in contact with said first starting material and said second starting material. 71. The method according to claim 70 wherein said catalyst comprises a compound comprising an element selected from the group consisting of Ti, V, Cr, C, Fe, Mn, Ni, Nb, Pd, Si, Al, and mixtures thereof. 72. A method of producing a source of hydrogen gas comprising: liberating hydrogen from a solid hydrogenated starting material composition comprising a hydride and a dehydrated hydroxide selected from the group consisting of: lithium hydroxide (LiOH), sodium hydroxide (NaOH), beryllium hydroxide (Be(OH)2), magnesium hydroxide (Mg(OH)2), calcium hydroxide (Ca(OH)2), strontium hydroxide (Sr(OH)2), titanium hydroxide (Ti(OH)2), aluminum hydroxide (Al(OH)3 and mixtures thereof, by reacting said hydride and said dehydrated hydroxide in a solid state reaction to produce a dehydrogenated reaction product and hydrogen gas. 73. The method according to claim 72 wherein said hydride and said hydroxide each have one or more cationic species other than hydrogen. 74. The method according to claim 72 further comprising regenerating said hydrogenated starting material composition by exposing said dehydrogenated product to hydrogen gas. 75. The method of claim 72 wherein said dehydrogenated product comprises an oxide. 76. The method of claim 74 wherein said regenerating is conducted at an elevated temperature relative to ambient conditions. 77. The method of claim 76 wherein said liberating of hydrogen is conducted at an elevated temperature greater than about 40° C. 78. The method of claim 72 wherein said liberating is conducted by removing said hydrogen gas as said reacting proceeds. 79. The method of claim 72 wherein said liberating is conducted in the presence of a catalyst in contact with said starting material composition. 80. The method according to claim 79 wherein said catalyst comprises a compound comprising an element selected from the group consisting of Ti, V, Cr, C, Fe, Mn, Ni, Nb, Pd, Si, Al, and mixtures thereof. 81. A hydrogen storage composition having a hydrogenated state and a dehydrogenated state: (a) in said hydrogenated state, said composition comprises a hydride represented by MIxHx and a dehydrated hydroxide represented by MIIy(OH)y, where MI and MII respectively represent one or more cationic species other than hydrogen that are selected from the group consisting of Al, As, Ba, Be, Ca, Cd, Ce, Cs, Cu, Eu, Fe, Ga, Gd, Ge, Hf, Hg, In, La, Li, Mg, Mn, Na, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Si, Sm, Sn, Sr, Th, Ti, Tl, V, W, Y, Yb, Zn, Zr, and mixtures thereof, wherein at least one of MI or MII is a complex cationic species comprising two distinct cationic species and x and y represent average valence states of MI and MII, respectively; and (b) in said dehydrogenated state, said composition comprises an oxide. 82. The composition of claim 81 wherein MI is said complex cationic species. 83. The composition of claim 81 wherein MII is a said complex cationic species. 84. The composition of claim 81 wherein MII is selected from the group consisting of Al, As, Ba, Be, Ca, Cd, Ce, Cs, Cu, Eu, Fe, Ga, Gd, Ge, Hf, Hg, In, La, Li, Mg, Mn, Na, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Si, Sm, Sn, Sr, Th, Ti, Tl, V, W, Y, Yb, Zn, Zr, and mixtures thereof. 85. The composition of claim 84 wherein MI and MII is selected from the group consisting of Al, Ba, Be, Ca, Cs, Li, Mg, Na, Rb, Si, Sr, Ti, V and mixtures thereof. 86. The composition of claim 85 wherein MI or MII is selected from the group consisting of Al, Be, Ca, Li, Mg, Na, Sr, Ti, and mixtures thereof. 87. The composition of claim 81 wherein said hydride is selected from the group consisting of: lithium hydride (LiH), sodium hydride (NaH), potassium hydride (KH), beryllium hydride (BeH2), magnesium hydride (MgH2), calcium hydride (CaH2), strontium hydride (SrH2), titanium hydride (TiH2), aluminum hydride (AlH3), boron hydride (BH3), lithium borohydride (LiBH4), sodium borohydride (NaBH4), magnesium borohydride (Mg(BH4)2), calcium borohydride (Ca(BH4)2), lithium alanate (LiAlH4), sodium alanate (NaAlH4), magnesium alanate (Mg(AlH4)2), calcium alanate (Ca(AlH4)2), and mixtures thereof. 88. The composition of claim 81 wherein said hydroxide is selected from the group consisting of: lithium hydroxide (LiOH), sodium hydroxide (NaOH), beryllium hydroxide (Be(OH)2), magnesium hydroxide (Mg(OH)2), calcium hydroxide (Ca(OH)2), strontium hydroxide (Sr(OH)2), titanium hydroxide (Ti(OH)2), aluminum hydroxide (Al(OH)3), and mixtures thereof. 89. The composition of claim 81 wherein said hydride comprises LiH. 90. The composition of claim 81 wherein said hydroxide comprises LiOH. 91. The composition according to claim 81 where said hydride composition comprises LiBH4 and said hydroxide comprises LiOH. 92. The composition according to claim 91 where said reaction proceeds according to a reaction mechanism of LiBH44 LiOH →LiBO2+2 Li2O+4H2. 93. The composition according to claim 81 where said hydride composition comprises NaBH4 and said hydroxide comprises Mg(OH)2. 94. The composition according to claim 93 where said reaction proceeds according to a reaction mechanism of NaBH4+2 Mg(OH)2→NaBO2+2MgO +4H2. 95. The composition according to claim 81 where said hydride composition comprises NaBH4 and said hydroxide comprises NaOH. 96. The composition according to claim 95 where said reaction proceeds according to a reaction mechanism of NaBH4+4 NaOH→NaBO2+2 Na2O4 H2. 97. A hydrogen storage composition having a hydrogenated state and a dehydrogenated state: (a) in said hydrogenated state, said composition comprises a hydride represented by MIxHx and a dehydrated hydroxide represented by MIIy(OH)y, where MI and MII respectively represent one or more cationic species other than hydrogen that are selected from the group consisting of Al, Be, Ca, Mg, Sr, and mixtures thereof, wherein x and y represent average valence states of MI and MII, respectively; and (b) in said dehydrogenated state, said composition comprises an oxide. 98. The composition according to claim 97 wherein said hydride composition comprises MgH2 and said hydroxide composition comprises Mg(OH)2. 99. The composition according to claim 98 wherein said reaction proceeds according to a reaction mechanism of MgH2+Mg(OH)2→MgO+2 H2. 100. The composition according to claim 97 wherein said hydride composition comprises AlH3 and said hydroxide composition comprises Al(OH)3. 101. The composition according to claim 100 wherein said reaction proceeds according to a reaction mechanism of AlH3+Al(OH)3→Al2O3+3H2 . 102. The composition according to claim 97 wherein said hydride composition comprises CaH2 and said hydroxide composition comprises Ca(OH)2. 103. The composition according to claim 102 wherein said reaction proceeds according to a reaction mechanism of CaH2+Ca(OH)2→CaO+2 H2. 104. The composition according to claim 97 wherein said hydride composition comprises SrH2 and said hydroxide composition comprises Sr(OH)2. 105. The composition according to claim 104 wherein said reaction proceeds according to a reaction mechanism of SrH2+Sr(OH)2→SrO+2 H2. 106. The composition according to claim 97 wherein said hydride composition comprises BeH2 and said hydroxide composition comprises Be(OH)2. 107. The composition according to claim 106 wherein said reaction proceeds according to a reaction mechanism of BeH2+Be(OH)2→BeO+2 H2.
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