CN114984864A - 一种高能效低碳排放内部电加热固定床制氢反应器 - Google Patents
一种高能效低碳排放内部电加热固定床制氢反应器 Download PDFInfo
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- CN114984864A CN114984864A CN202210478485.XA CN202210478485A CN114984864A CN 114984864 A CN114984864 A CN 114984864A CN 202210478485 A CN202210478485 A CN 202210478485A CN 114984864 A CN114984864 A CN 114984864A
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- 238000005485 electric heating Methods 0.000 title claims abstract description 95
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 69
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 69
- 239000001257 hydrogen Substances 0.000 title claims abstract description 69
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 64
- 239000003054 catalyst Substances 0.000 claims abstract description 75
- 238000001035 drying Methods 0.000 claims abstract description 30
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 27
- 239000007789 gas Substances 0.000 claims abstract description 26
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- 239000012495 reaction gas Substances 0.000 claims abstract description 19
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- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical compound [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 claims abstract description 10
- 229910052751 metal Inorganic materials 0.000 claims abstract description 9
- 239000002184 metal Substances 0.000 claims abstract description 9
- VXAUWWUXCIMFIM-UHFFFAOYSA-M aluminum;oxygen(2-);hydroxide Chemical compound [OH-].[O-2].[Al+3] VXAUWWUXCIMFIM-UHFFFAOYSA-M 0.000 claims abstract description 6
- 238000010438 heat treatment Methods 0.000 claims description 20
- 229910052799 carbon Inorganic materials 0.000 claims description 19
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 15
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 14
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- 229910052878 cordierite Inorganic materials 0.000 claims description 6
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 6
- -1 polyoxyethylene Polymers 0.000 claims description 6
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 5
- 229920003171 Poly (ethylene oxide) Polymers 0.000 claims description 5
- 239000002202 Polyethylene glycol Substances 0.000 claims description 5
- 230000032683 aging Effects 0.000 claims description 5
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- 239000008367 deionised water Substances 0.000 claims description 5
- 229910021641 deionized water Inorganic materials 0.000 claims description 5
- 229910017604 nitric acid Inorganic materials 0.000 claims description 5
- 229920001223 polyethylene glycol Polymers 0.000 claims description 5
- 239000002994 raw material Substances 0.000 claims description 5
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 4
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- 229910000838 Al alloy Inorganic materials 0.000 claims description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 3
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- 238000005234 chemical deposition Methods 0.000 claims description 2
- 239000004927 clay Substances 0.000 claims description 2
- 229910017052 cobalt Inorganic materials 0.000 claims description 2
- 239000010941 cobalt Substances 0.000 claims description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 2
- 238000013461 design Methods 0.000 claims description 2
- 229910052742 iron Inorganic materials 0.000 claims description 2
- 239000002808 molecular sieve Substances 0.000 claims description 2
- 229910052763 palladium Inorganic materials 0.000 claims description 2
- 229910052697 platinum Inorganic materials 0.000 claims description 2
- 229910052761 rare earth metal Inorganic materials 0.000 claims description 2
- 150000002910 rare earth metals Chemical class 0.000 claims description 2
- 229910052703 rhodium Inorganic materials 0.000 claims description 2
- 239000010948 rhodium Substances 0.000 claims description 2
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 2
- 239000012266 salt solution Substances 0.000 claims description 2
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 2
- 239000000243 solution Substances 0.000 claims description 2
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- 229910001220 stainless steel Inorganic materials 0.000 claims description 2
- 239000010935 stainless steel Substances 0.000 claims description 2
- 238000000629 steam reforming Methods 0.000 claims description 2
- 239000004215 Carbon black (E152) Substances 0.000 claims 3
- 229930195733 hydrocarbon Natural products 0.000 claims 3
- 150000002430 hydrocarbons Chemical class 0.000 claims 3
- 229910000604 Ferrochrome Inorganic materials 0.000 claims 1
- 239000002253 acid Substances 0.000 claims 1
- 150000007513 acids Chemical class 0.000 claims 1
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- 229910045601 alloy Inorganic materials 0.000 claims 1
- 239000000956 alloy Substances 0.000 claims 1
- 238000002453 autothermal reforming Methods 0.000 claims 1
- 235000019441 ethanol Nutrition 0.000 claims 1
- 150000002170 ethers Chemical class 0.000 claims 1
- 150000002632 lipids Chemical class 0.000 claims 1
- 229910001120 nichrome Inorganic materials 0.000 claims 1
- 239000003921 oil Substances 0.000 claims 1
- 238000002407 reforming Methods 0.000 claims 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 abstract description 16
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 abstract description 12
- 239000001569 carbon dioxide Substances 0.000 abstract description 6
- 229910002092 carbon dioxide Inorganic materials 0.000 abstract description 6
- 238000000034 method Methods 0.000 abstract description 6
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- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 description 4
- 238000011160 research Methods 0.000 description 4
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- 238000009826 distribution Methods 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- NWAHZABTSDUXMJ-UHFFFAOYSA-N platinum(2+);dinitrate Chemical compound [Pt+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O NWAHZABTSDUXMJ-UHFFFAOYSA-N 0.000 description 3
- 238000005034 decoration Methods 0.000 description 2
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- 239000002803 fossil fuel Substances 0.000 description 2
- 239000004570 mortar (masonry) Substances 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000006004 Quartz sand Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 230000003321 amplification Effects 0.000 description 1
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- 238000006386 neutralization reaction Methods 0.000 description 1
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Abstract
本发明涉及一种高能效低碳排放内部电加热固定床制氢反应器,主要包括如下步骤:(1)将电加热球进行表面预处理;(2)取拟薄水铝石,配制浆料,在电加热球表面制备涂层;(3)取硝酸镍溶液浸渍涂层,干燥后焙烧获得表面带催化剂的电加热金属球;(4)取活性氧化铝球浸渍硝酸镍溶液,制备制氢球状催化剂;(5)在管式反应器底部放置导电板,随后将电加热球和制氢催化剂逐层堆积间隔排布,随后上层加导电板;(6)反应器底部进反应气,上端出气,出气口设置泡沫氧化铝绝缘和气体分散;(7)将导线和导电板连接。本方法发明较传统固定床反应器具有催化剂利用率高、温度均匀且响应块、能源效率高、二氧化碳排放低等优势,为工业规模化甲烷制氢提供良好策略。
Description
技术领域
本发明属于反应器制备技术领域,尤其涉及一种高能效低碳排放内部电加热固定床制氢反应器。
背景技术
在碳达峰-碳中和背景下,交通、能源、建筑等工业部门都需要依靠氢能实现深度脱碳,给氢能发展带来前所未有的机遇。然而由于电解水等其他制氢方式存在生产成本高、设备投资大、技术限制等原因,使得我国目前氢能来源中化石燃料制氢占比高达99%,并且在很长一段时间内仍无法摆脱。
在化石燃料制氢中,天然气蒸汽重整制氢较为成熟,是国内外主流制氢方式。在目前在建和使用中的天然气制氢装置,均为传统颗粒催化剂固定床反应器,通过外部燃烧天然气等气源给反应器内催化剂供热,因此不可避免的存在二氧化碳排放高、温度分布不均等问题,因此,如何在工业规模上实现反应床层温度均匀且快速响应、提升催化剂利用率、提升能源效率、减少二氧化碳排放成为国内外的研究重点。
国际上,化工设备电气化成为主流趋势,巴斯夫、托普索和RWE等都开始在电加热化工装备投入大量研究力量,如能利用可再生能源产生的绿电应用于工业生产是研究热点。目前在甲烷制氢反应器如何实现电加热主要集中在三个方面。一、反应器优化,通过反应器改造直接给壁面直接通电,为内部颗粒催化剂供热,这种形式虽改变了传统的燃烧加热形式,但带来设备复杂、安全隐患等问题,同时仍未能解决催化剂床层温差大、积碳等问题;二、阵列毛细管反应器,内壁涂覆催化剂,通过管壁通电直接给内部催化剂供热。但存在涂覆量低、无法放大等问题;三、颗粒催化剂床层内部电加棒形式,此方式虽可以实现反应器体积的大幅缩小,但仍存在径向温差大、使用寿命低等问题。因此如何快速有效的提升工业天然气制氢催化剂和能源有效利用率,优化反应器内部温度分布,降低二氧化碳的排放,仍需要大量的研究工作继续开展。
基于以上天然气制氢困境,本发明直接采用在电加热球表面涂覆一层催化剂,在反应器内部通过电加热球和颗粒催化剂一起堆叠排放,创新性的在上下导电板作用下,实现内置电加热球通电产生热量迅速给内部颗粒催化剂供热,解决了传热限制和内部温差问题,在前后气体进出口设置泡沫氧化铝实现了气体混合,避免的气流不均匀问题,四周的陶瓷体起到了绝缘和安全保证,本发明反应器在工业制氢产业中具有非常重大的应用价值。
发明内容
本发明的目的在于解决了传统天然气制氢反应器存在的制氢催化剂有效利用率低、能源效用低、反应器内部温度冷热点和二氧化碳的排放高等问题,提供了一种高能效低碳排放内部电加热固定床制氢反应器的方案设计。
本发明一种高能效低碳排放内部电加热固定床制氢反应器是通过以下技术方案实现的:
一种高能效低碳排放内部电加热固定床制氢反应器,包括如下技术步骤:
(1)将电加热球浸没于无水乙醇中处理20~600分钟后,室温干燥;随后将电加热球浸没于质量分数为1~20%氢氧化钠中处理1~30分钟后,室温干燥;随后将电加热球浸没于质量分数为1~20%硝酸中处理1~30分钟后, 50~150℃干燥30~180分钟后,以1~10℃/min升温至650~1050℃焙烧30~ 800分钟;得到处理好的电加热球;
(2)配置浆料,其原料的组份质量分数为:
聚乙二醇为0.5~15%,
聚氧化乙烯为0.5~15%,
改性纤维素醚为0.1~5%,
去离子水为10~50%,
拟薄水铝石为0.5~15%,
纳米γ-氧化铝为余量;
混合搅拌10~200分钟后,老化12~36小时备用,得到老化后的料;随后采用喷涂方法在步骤(1)处理好的电加热球上制备0.1~500μm浆料,随后在50~150℃干燥30~180分钟后,以1~10℃/min升温至250~750℃焙烧 30~200分钟,得到涂覆浆料的电加热球;
(3)将步骤(2)制备的涂覆浆料的电加热球放入配制的5~40%硝酸镍水溶液中浸没5~600分钟,随后在20~120℃干燥10~180分钟后,以1~ 10℃/min升温至250~550℃焙烧30~240分钟,获得带涂层的电加热球;
(4)取活性氧化铝球放入配制的5~40%硝酸镍水溶液中浸没5~600分钟,随后在20~120℃干燥10~180分钟后,以1~10℃/min升温至250~550℃焙烧30~240分钟,获得制氢球状催化剂;
(5)在管式反应器四周放置1~60mm厚绝缘陶瓷后,在底部放置1~ 60mm厚导电板,随后将步骤(3)制备的带涂层的电加热球和步骤(4)制备的制氢催化剂间隔放置,随后逐层堆积,期间保证上下电加热球必须接触,最后在催化剂上端放置1~60mm厚导电板;
(6)反应器底部开孔作为反应气进口,反应气进口和催化剂之间设置1~ 300mm厚泡沫氧化铝用于绝缘和气体分散,在反应器顶部开孔作为反应器出口,反应气出口和催化剂之间同样设置1~300mm厚泡沫氧化铝用于绝缘和气体分散;
(7)在反应器器壁开孔,将导线和上下导电板连接;完成内部电加热固定床制氢反应器制备。
进一步的电加热球的材料是镍铬合金,多孔碳材料,铁铬铝合金,不锈钢,镍合金,铜合金,铝合金等导电球中的一种或者几种。
进一步的电加热球也可以设计为正方形,长方形,椭圆,三角,柱状,螺旋,丝,带,折叠,片状,波纹等中的一种。
进一步的浆料制备的涂层主体可以为γ-氧化铝,也可以是分子筛,尖晶石,稀土材料等一种或者几种替换。其涂层制备方法也不限于喷涂方法,也可以为浸渍提拉,涂覆,化学沉积,溶胶凝胶等。其形状可以为球状,也可以是多孔,柱状,五角星等多种形式。
进一步的浸渍溶液为硝酸镍,也可以是铂,铑,钯,铜,铁,钴一种或者几种混合的盐溶液。
进一步的反应器绝缘材料为陶瓷,也可以为橡胶,耐火泥等其他绝缘体。
进一步的进出口和催化剂之间设置泡沫氧化铝用于绝缘和气体分散,也可以为多孔堇青石,多孔耐火泥,球状颗粒等;
进一步的金属球和催化剂顶端设置导电板,也可以是导电丝,电源线等用于电加热球连接。
进一步的金属球表面制备催化剂涂层,也可以为无涂层金属球单纯作为电加热器为颗粒催化剂供热。
进一步的电加热金属球可以为无序排列,也可以为有序有接触式排列。
与现有技术相比,本发明的积极效果是:
本发明选用带催化剂涂层的电加热球作为加热器和表面催化剂,利用焦耳热源与反应位点之间的密切接触,使反应接近热平衡,解决了涂敷量低下、停留时间不足、催化剂利用率低等问题。采用内部电加热形式可以大幅缩小反应器体积,提高能源热效率和催化剂性能,大幅降低二氧化碳排放量。电加热催化剂球和催化剂颗粒无序间隔排列大大提升了换热面积,实现催化剂床层内部的快速启停,解决了催化剂存在的温度梯度,降低了催化剂积碳的风险,同时避免了催化剂床层内部的径向和轴向温差。在反应器避免增加陶瓷隔离层和进出口增加泡沫材料气体分配,避免的气流不均匀问题和安全隐患。与传统重整器相比,这种导电粒子和催化剂颗粒的内部排列使重整器更紧凑,能源利用率更高,可以大幅降低供热燃烧产生的CO2,实现制氢过程从“灰”变“绿”,助力双碳目标早日实现。
附图说明:
图1:一种高能效低碳排放内部电加热固定床制氢反应器的示例图一;
图1-1:一种高能效低碳排放内部电加热固定床制氢反应器的示例图二;
图2:电加热球表面催化剂涂层SEM图;
图3:本发明反应器和传统外部加热固定床反应器内部温差对比图;
具体实施方式
以下提供本发明一种高能效低碳排放内部电加热固定床制氢反应器具体实施方式。
实施例1
本实施例提供了一种高能效低碳排放内部电加热固定床制氢反应器,包括以下步骤:
如图1所示,一种高能效低碳排放内部电加热固定床制氢反应器包含反应器壁(1)、电源连接接头(2)、导电板(3)、绝缘陶瓷(4)、制氢球状催化剂(5)、电加热球(6)和泡沫氧化铝(7)。
(1)将FeCrAl电加热球浸没于无水乙醇中处理30分钟后,室温干燥;随后将电加热球浸没于20%氢氧化钠中处理5分钟后,室温干燥;随后将电加热球浸没于10%硝酸中处理10分钟后,90℃干燥180分钟后,以10℃/min 升温至1050℃焙烧300分钟。
(2)配置浆料,其原料的组份质量分数为:
聚乙二醇为5%,
聚氧化乙烯为5%,
改性纤维素醚为2%,
去离子水为30%,
拟薄水铝石3%,
纳米γ-氧化铝为余量;
混合搅拌30分钟后,老化36小时备用,得到老化后的料;随后采用喷涂方法在(1)处理好的电加热球上制备20μm浆料,随后在120℃干燥30 分钟后,以10℃/min升温至550℃焙烧30分钟。
(3)将(2)中电加热球放入配制的5%硝酸镍水溶液中浸没30分钟,随后在80℃干燥180分钟后,以2℃/min升温至550℃焙烧240分钟。
(4)取活性氧化铝球放入配制的5%硝酸镍水溶液中浸没40分钟,随后在120℃干燥100分钟后,以5℃/min升温至350℃焙烧40分钟,获得制氢球状催化剂;
(5)在管式反应器四周放置绝缘陶瓷后,在底部放置铜导电板,随后将电加热球和制氢催化剂间隔放置,随后逐层堆积,期间保证上下电加热球必须接触,最后在催化剂上端放置导电板;
(6)反应器底部开孔作为反应气进口,反应气进口和催化剂之间设置泡沫氧化铝用于绝缘和气体分散,在反应器顶部开孔作为反应器出口,反应气出口和催化剂之间同样设置泡沫氧化铝用于绝缘和气体分散;
(7)在反应器器壁开孔,将导线和上下导电板连接。完成内部电加热固定床制氢反应器制备。
将导线接入电源,控制反应温度和空速,当一定水碳比的CH4和水混合气进入反应器内,快速发生反应,产生氢气。
对比例:采用传统固定床反应器,催化剂和实施例1一样的颗粒催化剂,催化剂填充量和实施例1一致,保证催化剂填充高度一致,体积不足部分用石英砂替代。采用传统电加热炉在管式反应器外部加热,保证温度内部电加热一致。所有实验参数和实施例1一致。其内部温差对比图如图3所示。
实施例2
本实施例提供了一种高能效低碳排放内部电加热固定床制氢反应器,包括以下步骤:
(1)将Ni电加热球浸没于无水乙醇中处理100分钟后,室温干燥;随后将电加热球浸没于2%氢氧化钠中处理30分钟后,室温干燥;随后将电加热球浸没于5%硝酸中处理30分钟后,50℃干燥80分钟后,以10℃/min升温至650℃焙烧200分钟。
(2)配置浆料,其原料的组份质量分数为:
聚乙二醇为0.5%,
聚氧化乙烯为0.5%,
改性纤维素醚为0.1%,
去离子水为50%,
拟薄水铝石5%,
纳米γ-氧化铝为余量;
混合搅拌10分钟后,老化12小时备用,得到老化后的料;随后浸渍提拉法在(1)处理好的电加热球上制备80μm浆料,随后在50℃干燥90分钟后,以2℃/min升温至350℃焙烧200分钟。
(3)将(2)中电加热球放入配制的20%硝酸铂水溶液中浸没5分钟,随后在50℃干燥10分钟后,以2℃/min升温至550℃焙烧240分钟。
(4)取活性氧化铝球放入配制的10%硝酸铂水溶液中浸没20分钟,随后在120℃干燥180分钟后,以2℃/min升温至550℃焙烧240分钟,获得制氢球状催化剂;
(5)在管式反应器四周放置绝缘陶瓷后,在底部放置导电线,随后将电加热球和制氢催化剂间隔放置,无序摆放,随后逐层堆积,期间保证上下电加热球必须接触,最后在催化剂上端放导电线;
(6)反应器底部开孔作为反应气进口,反应气进口和催化剂之间设置堇青石陶瓷用于绝缘和气体分散,在反应器顶部开孔作为反应器出口,反应气出口和催化剂之间同样设置堇青石陶瓷用于绝缘和气体分散;
(7)在反应器器壁开孔,将导线和导电线连接。完成内部电加热固定床制氢反应器制备。
将导线接入电源,控制反应温度和空速,当一定水碳比的CH4和水混合气进入反应器内,快速发生反应,产生氢气。
实施例3
一种高能效低碳排放内部电加热固定床制氢反应器,包括如下技术步骤:
(1)将Cu正方体块浸没于无水乙醇中处理600分钟后,室温干燥;随后将Cu正方体块浸没于2%氢氧化钠中处理2分钟后,室温干燥;随后将Cu 正方体块浸没于6%硝酸中处理30分钟后,50℃干燥180分钟后,以2℃/min 升温至650℃焙烧30分钟。
(2)配置浆料,其原料的组份质量分数为:
聚乙二醇为6%,
聚氧化乙烯为6%,
改性纤维素醚为2%,
去离子水为30%,
拟薄水铝石8%,
纳米γ-氧化铝为余量;
混合搅拌200分钟后,老化18小时备用,得到老化后的料;随后采用涂覆方法在(1)处理好的电加热体上制备0.1浆料,随后在60℃干燥30分钟后,以3℃/min升温至750℃焙烧100分钟。
(3)将(2)中Cu正方体块放入配制的5%硝酸铁水溶液中浸没20分钟,随后在120℃干燥180分钟后,以10℃/min升温至550℃焙烧240分钟,获得 Cu正方体块催化剂。
(4)取活性氧化铝球放入配制的20%硝酸铁水溶液中浸没100分钟,随后在120℃干燥180分钟后,以5℃/min升温至550℃焙烧30~240分钟,获得制氢球状催化剂;
(5)在管式反应器四周放置耐火泥后,在底部放置导电板,随后将(3) 所得的Cu正方体块和(4)所得制氢催化剂间隔放置,随后逐层堆积,期间保证上下电加热体必须接触,最后在催化剂上端放置导电板;
(6)反应器底部开孔作为反应气进口,反应气进口和催化剂之间设置泡沫氧化铝用于绝缘和气体分散,在反应器顶部开孔作为反应器出口,反应气出口和催化剂之间同样设置泡沫氧化铝用于绝缘和气体分散;
(7)在反应器器壁开孔,将导线和上下导电板连接。完成内部电加热固定床制氢反应器制备。
实施例4
本实施例提供了一种高能效低碳排放内部电加热固定床制氢反应器,包括以下步骤:
(1)将Ni电加热球浸没于无水乙醇中处理100分钟后,室温干燥
(2)取活性氧化铝球放入配制的10%硝酸铂水溶液中浸没20分钟,随后在120℃干燥180分钟后,以2℃/min升温至550℃焙烧240分钟,获得制氢球状催化剂;
(3)在管式反应器四周放置绝缘陶瓷后,在底部放置导电线,随后将电加热球和制氢催化剂间隔放置,无序摆放,随后逐层堆积,期间保证上下电加热球必须接触,最后在催化剂上端放导电线;
(4)反应器底部开孔作为反应气进口,反应气进口和催化剂之间设置堇青石陶瓷用于绝缘和气体分散,在反应器顶部开孔作为反应器出口,反应气出口和催化剂之间同样设置堇青石陶瓷用于绝缘和气体分散;
(5)在反应器器壁开孔,将导线和导电线连接。完成内部电加热固定床制氢反应器制备。
将导线接入电源,控制反应温度和空速,当一定水碳比的CH4和水混合气进入反应器内,快速发生反应,产生氢气。
以上所述仅是本发明的优选实施方式,应当指出,对于本技术领域的普通技术人员,在不脱离本发明构思的前提下,还可以做出若干改进和润饰,这些改进和润饰也应视为本发明的保护范围内。
Claims (10)
1.一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,包括如下技术步骤:
(1)将电加热球浸没于无水乙醇中处理20~600分钟后,室温干燥;随后将电加热球浸没于质量分数为1~20%氢氧化钠中处理1~30分钟后,室温干燥;随后将电加热球浸没于质量分数为1~20%硝酸中处理1~30分钟后,50~150℃干燥30~180分钟后,以1~10℃/min升温至650~1050℃焙烧30~800分钟;得到处理好的电加热球;
(2)配置浆料,其原料的组份质量分数为:
聚乙二醇为0.5~15%,
聚氧化乙烯为0.5~15%,
改性纤维素醚为0.1~5%,
去离子水为10~50%,
拟薄水铝石为0.5~15%,
纳米γ-氧化铝为余量;
混合搅拌10~200分钟后,老化12~36小时备用,得到老化后的料;随后采用喷涂方法在步骤(1)处理好的电加热球上制备0.1~500μm浆料,随后在50~150℃干燥30~180分钟后,以1~10℃/min升温至250~750℃焙烧30~200分钟,得到涂覆浆料的电加热球;
(3)将步骤(2)制备的涂覆浆料的电加热球放入配制的5~40%硝酸镍水溶液中浸没5~600分钟,随后在20~120℃干燥10~180分钟后,以1~10℃/min升温至250~550℃焙烧30~240分钟,获得带涂层的电加热球;
(4)取活性氧化铝球放入配制的5~40%硝酸镍水溶液中浸没5~600分钟,随后在20~120℃干燥10~180分钟后,以1~10℃/min升温至250~550℃焙烧30~240分钟,获得制氢球状催化剂;
(5)在管式反应器四周放置1~60mm厚绝缘陶瓷后,在底部放置1~60毫米厚导电板,随后将步骤(3)制备的带涂层的电加热球和步骤(4)制备的制氢催化剂间隔放置,随后逐层堆积,期间保证上下电加热球必须接触,最后在催化剂上端放置1~60毫米厚导电板;
(6)反应器底部开孔作为反应气进口,反应气进口和催化剂之间设置1~300毫米厚泡沫氧化铝用于绝缘和气体分散,在反应器顶部开孔作为反应器出口,反应气出口和催化剂之间同样设置1~300毫米厚泡沫氧化铝用于绝缘和气体分散;
(7)在反应器器壁开孔,将导线和上下导电板连接;完成内部电加热固定床制氢反应器制备。
2.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,电加热球的材料是镍铬合金,多孔碳材料,铁铬铝合金,不锈钢,镍合金,铜合金,铝合金导电球中的一种或者几种。
3.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,电加热球设计为正方形,长方形,椭圆,三角,柱状,螺旋,丝,带,折叠,片状,波纹中的一种。
4.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,所述的浆料制备的涂层主体为γ-氧化铝,分子筛,尖晶石,稀土材料一种或者几种替换;
其涂层制备方法也不限于喷涂方法,或者为浸渍提拉,涂覆,化学沉积,溶胶凝胶;
其形状为球状,或者是多孔,柱状,五角星。
5.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,所述的浸渍溶液为硝酸镍,或者是铂,铑,钯,铜,铁,钴一种或者几种混合的盐溶液。
6.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,所述的制氢反应可以为常规烃类蒸汽重整、常规烃类干重整、常规烃类自热重整,常规醇类、醚类、酸类、脂类、油类中的一种或者几种。
7.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,所述的进出口和催化剂之间设置泡沫氧化铝用于绝缘和气体分散,或者为多孔堇青石,多孔耐火泥,球状颗粒。
8.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,所述的金属球和催化剂顶端设置导电板,为导电丝,电源线用于电加热球连接。
9.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,所述的金属球表面制备催化剂涂层,或者为无涂层金属球单纯作为电加热器为颗粒催化剂供热。
10.如权利要求1所述的一种高能效低碳排放内部电加热固定床制氢反应器,其特征在于,所述的电加热金属球为无序排列,或者为有序有接触式排列。
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