JP6241804B1 - 水素生成装置 - Google Patents
水素生成装置 Download PDFInfo
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- JP6241804B1 JP6241804B1 JP2017089365A JP2017089365A JP6241804B1 JP 6241804 B1 JP6241804 B1 JP 6241804B1 JP 2017089365 A JP2017089365 A JP 2017089365A JP 2017089365 A JP2017089365 A JP 2017089365A JP 6241804 B1 JP6241804 B1 JP 6241804B1
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- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 250
- 239000001257 hydrogen Substances 0.000 title claims abstract description 250
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 181
- 239000007789 gas Substances 0.000 claims abstract description 106
- 239000003054 catalyst Substances 0.000 claims abstract description 94
- 150000002431 hydrogen Chemical class 0.000 claims abstract description 93
- 239000012528 membrane Substances 0.000 claims abstract description 91
- 238000000926 separation method Methods 0.000 claims abstract description 91
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 110
- 229910021529 ammonia Inorganic materials 0.000 claims description 53
- 238000006555 catalytic reaction Methods 0.000 claims description 5
- 238000011144 upstream manufacturing Methods 0.000 claims description 5
- 239000002994 raw material Substances 0.000 abstract description 49
- 238000000354 decomposition reaction Methods 0.000 abstract description 18
- 230000009471 action Effects 0.000 abstract description 4
- 238000004519 manufacturing process Methods 0.000 abstract description 4
- 229910052751 metal Inorganic materials 0.000 description 10
- 239000002184 metal Substances 0.000 description 10
- 238000000034 method Methods 0.000 description 10
- 239000010409 thin film Substances 0.000 description 10
- 238000010438 heat treatment Methods 0.000 description 9
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 9
- 230000004888 barrier function Effects 0.000 description 8
- 238000006243 chemical reaction Methods 0.000 description 8
- 239000000446 fuel Substances 0.000 description 8
- 239000000395 magnesium oxide Substances 0.000 description 7
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 7
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 7
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 5
- 229910001252 Pd alloy Inorganic materials 0.000 description 5
- 229910045601 alloy Inorganic materials 0.000 description 5
- 239000000956 alloy Substances 0.000 description 5
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 5
- 150000002739 metals Chemical class 0.000 description 5
- 229910052759 nickel Inorganic materials 0.000 description 5
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 4
- 229910052707 ruthenium Inorganic materials 0.000 description 4
- 125000006850 spacer group Chemical group 0.000 description 4
- 229910001873 dinitrogen Inorganic materials 0.000 description 3
- 229930195733 hydrocarbon Natural products 0.000 description 3
- 150000002430 hydrocarbons Chemical class 0.000 description 3
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 2
- 239000004215 Carbon black (E152) Substances 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 2
- 239000004202 carbamide Substances 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 239000010408 film Substances 0.000 description 2
- 239000011261 inert gas Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 239000010955 niobium Substances 0.000 description 2
- 238000000629 steam reforming Methods 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- 229910018487 Ni—Cr Inorganic materials 0.000 description 1
- 239000004642 Polyimide Substances 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-N acrylic acid group Chemical group C(C=C)(=O)O NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- -1 alumina Chemical compound 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 1
- 229910002113 barium titanate Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000001010 compromised effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 229910052735 hafnium Inorganic materials 0.000 description 1
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 description 1
- 238000009396 hybridization Methods 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- FEBJSGQWYJIENF-UHFFFAOYSA-N nickel niobium Chemical compound [Ni].[Nb] FEBJSGQWYJIENF-UHFFFAOYSA-N 0.000 description 1
- HBVFXTAPOLSOPB-UHFFFAOYSA-N nickel vanadium Chemical compound [V].[Ni] HBVFXTAPOLSOPB-UHFFFAOYSA-N 0.000 description 1
- ZSJFLDUTBDIFLJ-UHFFFAOYSA-N nickel zirconium Chemical compound [Ni].[Zr] ZSJFLDUTBDIFLJ-UHFFFAOYSA-N 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910052755 nonmetal Inorganic materials 0.000 description 1
- 150000002843 nonmetals Chemical class 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- 229920002492 poly(sulfone) Polymers 0.000 description 1
- 229920000515 polycarbonate Polymers 0.000 description 1
- 239000004417 polycarbonate Substances 0.000 description 1
- 229920001721 polyimide Polymers 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000003566 sealing material Substances 0.000 description 1
- VSZWPYCFIRKVQL-UHFFFAOYSA-N selanylidenegallium;selenium Chemical compound [Se].[Se]=[Ga].[Se]=[Ga] VSZWPYCFIRKVQL-UHFFFAOYSA-N 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 239000002918 waste heat Substances 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
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- C01B3/047—Decomposition of ammonia
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Abstract
Description
(1)水素生成装置で好適に用いられる原料ガスは、アンモニア、尿素、またはメタン等の炭化水素系ガス、アンモニア単体ではなくアンモニアと不活性ガスの混合ガスとすることができる。また、液化アンモニアや尿素から発生したアンモニア単体またはそのアンモニアと不活性ガスの混合ガスとすることができる。
(2)触媒は、Ni、またはRuといった触媒金属を、酸化マグネシウム(MgO)またはアルミナ(Al2O3)に担持させたアンモニア分解触媒が好適に用いられる。
(3)水素分離膜は、高電圧電源に接続された場合、高電圧電極として機能する。水素分離膜が高電圧電極となっているとき、誘電体を挟んで対向している電極は、アースされて接地電極として機能する。
(4)水素分離膜は、アースされている場合、接地電極として機能する。水素分離膜が接地電極となっているとき、誘電体を挟んで対向している電極は高電圧電源に接続されて高電圧電極として機能する。
(5)高電圧電極と接地電極とは誘電体を隔てて対向している形態となっており、誘電体バリア放電によって、原料ガス流路の中の原料ガスを大気圧非平衡プラズマとする。高電圧電源は、高電圧電極に対して、両極性パルス波形を印加する。
(6)誘電体は、石英ガラスなどのガラス、アルミナなどのセラミックス、チタン酸バリウム、ポリカーボネート、アクリルなどの絶縁性の高い樹脂で形成される。
(7)水素分離膜は、パラジウム合金薄膜を特に好適に使用することができる。
(8)水素流路は、水素流路板と水素分離膜によって区画された空間を用いることができる。
(9)水素流路は、水素分離膜と水素分離膜を支持する支持体の内部に形成される空間を用いることができる。
以下、本発明にかかる水素生成装置の好適な実施例について、図面を参照しつつ説明する。図1は、本発明の実施例に従った水素生成装置1を模式的に示す分解斜視図である。水素生成装置1は、誘電体2と、電極3と、水素流路板4と、水素分離膜5と、高電圧電源6と、絶縁スペーサ9と、触媒10とを備えている。尚、以下の記載においては、図1において右側に表示した各要素の側面を右側面と称し、左側に表示した各要素の側面を左側面と称する。
2NH3+e→N2+3H2+e (式1)
図2に、本実施例の水素生成装置21を示す。水素生成装置21は、誘電体である石英ガラス製のプラズマ反応器22の中に、触媒を収容した触媒管23と、パラジウム合金の薄膜を円筒形に成形した水素分離膜24が収容されている。本実施例の触媒管23と水素分離膜24は、ほぼ同一の径で形成されて直列に接続されており、プラズマ反応器22に対して同心円状に配置されている。プラズマ反応器22の内面と、触媒管23および水素分離膜24の外面との間に、原料ガス流路26が規定されている。水素分離膜24の内側の円筒状の空間が、水素流路27を形成する。
図3に、本実施例の水素生成装置31を示す。水素生成装置31は、プラズマ反応器32と、このプラズマ反応器32の中に収容された高電圧電極40と、プラズマ反応器32の外側を覆うように配置された接地電極42とを備えている。プラズマ反応器32は、石英ガラス製であり、円筒形に形成されて誘電体として機能する。高電圧電極40は、円筒形の水素分離膜34と、水素分離膜34の両端を支持する円盤状の支持体35とを備えている。水素分離膜34の好適な素材は、パラジウム合金の薄膜である。高電圧電極40は高電圧電源6に接続されており、高電圧が印加される。
実施例で説明した水素生成装置1、21、31の構成は、適宜変更が可能である。たとえば、実施例1の変形例として、誘電体上に形成する原料ガス流路13のパターンは、原料ガス流路13内で放電を発生させる範囲で、その位置および形状を変更することができる。実施例1から3の接地電極と高電圧電極は、いずれか一方が高電圧電極となって他方が接地電極となれば良く、電極の素材、高電圧電源や絶縁スペーサの配置等に会わせて適宜入れ替えが可能である。実施例3の円筒型のプラズマ反応器32を用いた水素生成装置31では、触媒41が水素分離膜34に対して上流に配置されれば良く、たとえば水素分離膜34の外側表面に触媒を担持または塗布することも可能である。また、プラズマ反応器32と水素分離膜34との間の原料ガス流路36に、実施例2で適用したペレット状の触媒30を充填することも可能である。
2 誘電体
3 電極
4 水素流路板
5 水素分離膜(接地電極)
6 高電圧電源
9 絶縁スペーサ
10、30、41 触媒
11 第一の面
13、26、36 原料ガス流路
14、38 原料ガス流路入口
15、43 原料ガス流路出口
16 原料ガス流路の往路部分
17 原料ガス流路の復路部分
18、27、37 水素流路
19、28、39 水素導出口
22、32 プラズマ反応器(誘電体)
23 触媒管
24、34 水素分離膜(高電圧電極)
25、42 接地電極
40 高電圧電極
Claims (4)
- 原料ガス流路を規定する誘電体と、
前記原料ガス流路を流れる原料ガスの少なくとも一部を分解して水素ガスを生成する触媒と、
前記誘電体に接して配置される電極と、
前記誘電体を隔てて前記電極に対向する水素分離膜と、
前記水素分離膜が分離した水素を導出する水素流路と、
電力を供給して前記水素分離膜と前記電極との間で放電を発生させる高電圧電源と、
を備えていることを特徴とする水素生成装置。 - 前記原料ガス流路が平板状の前記誘電体の表面に溝として形成されており、
前記溝の開口を薄板状の前記触媒が覆っており、
前記触媒に前記水素分離膜が積層されており、
前記水素分離膜は、放電または触媒反応によって原料ガスから生成した水素を分離して前記水素流路に導入することを特徴とする請求項1記載の水素生成装置。 - 前記誘電体が円筒形であり、
前記電極が前記誘電体の外側に配置されており、
前記誘電体の内側に前記水素分離膜が同心円状に配置されて、前記誘電体と前記水素分離膜との間に前記原料ガス流路が規定されており、
前記触媒が、前記原料ガス流路の中の前記水素分離膜よりも上流となる位置に配置されており、
前記水素分離膜は、放電または触媒反応によって原料ガスから生成した水素を分離して前記水素流路に導入することを特徴とする請求項1記載の水素生成装置。 - 前記原料ガスがアンモニアであることを特徴とする請求項1から3のいずれか1項記載の水素生成装置。
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